High-throughput printing of functionally gradient material from self-propagation

High-throughput printing of functionally gradient material from self-propagation | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article High-throughput printing of functionally gradient material from self-propagation yan zhang, yuqiang liu, jianping zhou, daqian sun This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6071151/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 03 Nov, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract The development of new materials is of great significance for scientific and technological innovation and is essential in addressing significant societal challenges (1). Combinatorial material deposition techniques facilitate the understanding of composition-structure-property relationships and permit the rapid screening of materials across diverse compositional ranges (2). However, there are considerable challenges associated with the universal integration of multiple materials and the creation of gradient material libraries due to the lack of efficient mixing mechanisms and the difficulty in achieving precise and rapid dispensing (3-5). In this study, we introduce a novel printing approach for multicomponent gradient materials, which amalgamates various constituent materials for the three-dimensional printing of multiscale and high-throughput multigradient materials. This innovation overcomes the limitations of prolonged cycle times, high experimental costs, and low efficiency inherent in traditional manufacturing methods. First, we developed 3D-printed precursor materials that can be shaped arbitrarily. By meticulously proportioning the components of these precursor materials through high-throughput techniques and material libraries, we enable multi-degree-of-freedom adjustments in ratios and on-demand combinations, resulting in the fabrication of complex materials not achievable through conventional manufacturing processes. Subsequently, we established a highly adaptable self-propagating energy deposition technology based on the precursor materials, which reduces the conventional reliance on specific equipment and processes. Finally, we demonstrated the application of this technology through a printing strategy for various copper-based composites and multicomponent gradient materials, which allows for the simultaneous incorporation of an array of metallic and non-metallic compounds with graded properties across multiple compositions and structures. This advancement significantly enhances the scope of additive manufacturing applications in composition optimization, functional grading, and structural tuning, surpassing the capabilities of traditional printing methods. Our ability to synchronize the printing of multilayer gradient materials during the process, while mitigating thermal accumulation and structural defects such as cracks through thermal stacking between gradients, represents a marked improvement over traditional hot-cold stacking methods. Furthermore, we transitioned from the conventional outside-in model of additive manufacturing—where methods and equipment dictate the consumables—to a novel inside-out model, whereby consumables inform the methodology and equipment. Such a paradigm shift will facilitate the development of new functionally graded materials with unique compositions and structural arrangements unattainable through established manufacturing techniques. Physical sciences/Materials science/Techniques and instrumentation/Design, synthesis and processing Physical sciences/Materials science/Structural materials/Metals and alloys Figures Figure 1 Figure 2 Figure 3 Figure 4 Introduction Materials are fundamental to numerous scientific and technological innovations, and advancements in the development of new materials are crucial for addressing significant societal challenges. Three-dimensional (3D) printing, as a leading-edge and widely adopted technology in additive manufacturing (AM), primarily relies on digitally designed models to construct targeted objects. This technology builds items through sequential layering of materials, employing a layer-by-layer stacking and superimposition technique to achieve complex 3D structures, thus providing a practical alternative for the fabrication of intricate and hollow components (6-9). Currently, the most advanced 3D printing technologies are predominantly based on thermoplastic processes, including melting and particle sintering (10,11). During the AM process, raw materials are transformed into filaments, which are subsequently melted via heating within a nozzle and deposited onto a substrate (12,13). This additional step not only elevates manufacturing costs but also presents challenges, as certain thermoplastic polymers cannot be entirely converted into filaments (14). Although the filament-based extrusion process offers simplicity and flexibility for metal 3D printing, it is constrained by its layer-by-layer stacking methodology (15). For instance, the inherent layer-by-layer structure often results in adhesion issues and voids between layers, adversely affecting the mechanical properties of the printed objects (16). Furthermore, residual powder generated during the sintering process may undergo melting, rendering it unsuitable for reuse and escalating material reprocessing costs (17, 18). The recycling of polymer materials poses further complications, as the identification and separation of different polymers are inherently challenging due to variations in their chemical properties (19). This complexity not only amplifies printing costs but may also lead to material degradation or environmental pollution. Consequently, even after recycling, the presence of polymers with disparate thermal properties can generate undesirable by-products in the final printed products (20-22). Moreover, the sintering process in metal 3D printing is accompanied by oxidation, necessitating the establishment of an inert environment. The oxide layer that forms inhibits the wettability of liquid metal with the powder, leading to porosity in the final product (23). While metal oxides provide several benefits over traditional metal powders—including lower costs, availability in submicron sizes, and reduced reactivity—their high melting points hinder the effective application of high-energy beams required for sintering (24,25). Consequently, the interplay of heat source limitations and print material constraints, coupled with the absence of a flexible handling mechanism for the printing materials, results in restricted material options and challenges in the universal integration of diverse materials and the development of gradient material libraries. In order to address the challenges associated with beam heat source sintering and the recycling of metallic materials, a new paradigm is required to facilitate high-quality manufacturing and economic integration of 3D printing in the metalworking sector. We propose a Self-Propagating Energy Deposition Technology (SPEDT) that leverages the spontaneous behavior of the Oxidation-Reduction Reaction (ORR). This innovative method eliminates the need for an external heat source, requiring only the energization and ignition of bulk metal during the printing process to produce molten metal directly. Consequently, SPEDT enables multimaterial 3D printing while avoiding the inherent limitations of conventional thermoplastic 3D printing techniques for metals, significantly simplifying the manufacturing process. In our study, we designed a granular plate structure that is capable of spontaneous progression utilizing a bottom-up fabrication strategy. This approach allows for the use of the liquid metal generated through the continuous ORR to facilitate a multimaterial 3D printing process. As a result, this method enables on-demand design capabilities and the formation of patterned macrostructures. The new materials produced through this heat-free sintering method have demonstrated exceptional mechanical properties, heat resistance, high electrical conductivity, corrosion resistance, and other characteristics typically associated with superalloys. SPEDT effectively overcomes the limitations imposed by traditional metal 3D printing methods, which often rely on external heat sources, suffer from oxidized layer formation, exhibit limited recyclability of waste metal powders, and incur high operational costs. This novel approach presents significant potential for mass production in the development of new materials. By circumventing irregularities found in layer-by-layer assembly, SPEDT enhances final product performance through precise control over the composition ratios of the materials used, resulting in superior material properties once the printed structure has cooled and solidified. SPEDT represents a highly efficient, non-contact AM technology that confines the dispersion of liquid metal through a nozzle, enabling the formation of specific jet amplitudes for on-demand geometric pattern manufacturing. Compared to traditional material printing techniques, SPEDT offers precise control over heterogeneous interfaces, thereby facilitating the creation of more complex structures. It has broad applicability in areas that require intricate model designs, such as human skeletal reconstructions, engine blocks, and customized architectural projects, thus providing a novel solution for the design and fabrication of advanced materials. Such an innovative AM technique paves the way for new strategies in material design and synthesis. 1. Preparation and properties of 3DPS Copper (Cu) plays a vital role in high-temperature applications due to its exceptional thermal and electrical conductivity ( 26 ). However, the increasing demand for complex structural components has rendered traditional methods of fabricating pure Cu insufficient to meet these needs. Currently, three-dimensional (3D) metallic structures of Cu are predominantly produced through AM techniques, including Selective Laser Melting, Electron Beam Melting, and Directed Energy Deposition ( 27 ). These methods require an external heat source (e.g., laser or electron beam) as well as metal powder or wire. The high reflectivity of Cu significantly diminishes the efficiency of energy utilization, presenting challenges for beam-based AM of metallic materials ( 28 , 29 ). To address these challenges, we developed a precursor material aimed at the preparation of novel materials. We formulated a composite system of aluminum (Al) and copper(II) oxide (CuO) in paste form, accompanied by plasticization, to exploit the spontaneous ORR ( 30 ). This approach leverages the inherent capacity of reducing CuO to pure Cu and facilitates metal deposition (MD) (Fig. 1 a), leading to the successful precipitation of pure metal. The Al/CuO nanoparticle composite demonstrated a high reaction rate owing to the abundance of reaction sites created by the large surface area of the composite, thereby enhancing its overall reactivity ( 31 ). The simplicity of the excitation conditions required for spontaneous and continuous reaction progression stimulated further development of Al/CuO-based systems. Building on the favorable combustion characteristics and reaction products of the Al/CuO composite system (Fig. 1 b), we designed consumables capable of 3D printing metallic materials using a bottom-up material synthesis strategy (Supplementary Data 1) and high-throughput experiments (Supplementary Data 2). The preparation process for specific 3D printed materials was delineated into three stages, designated A, B, and C (Fig. 1 c). In stage A, to enhance the binding properties between Al and CuO, their surface viscosities were modified with Polyvinyl Butyral (PVB) in an ethanol solution. This modification promoted cohesive binding and facilitated surface assembly, resulting in the formation of Metal Precursor Materials (MPM). Through high-throughput experimentation, over 300 experimental configurations were evaluated to optimize the particle plate structure for MPM, ultimately leading to the identification of a configuration that facilitated the formation of metal-based alloys with a stable combustion process and superior performance. However, further modification of the deposited Cu was required due to issues related to inferior mechanical properties, porosity, difficulties in slag separation, and limited controllability of the reaction rate. To mitigate these challenges, we incorporated calcium fluoride (CaF 2 ) in stage B to enhance the strength of the MD within the MPM. The reaction between Al and CuO is critical in CuO development, as is the self-reaction of CuO. Given that the Al-CuO reaction is exothermic, and recognizing that CaF 2 can absorb oxygen and hydrogen from the environment, the oxidation and hydrogen cracking of the MD are inhibited at elevated temperatures ( 32 , 33 ). Furthermore, the rapid reaction of Al with CuO, combined with the addition of calcium carbonate (CaCO 3 ), not only moderates the reaction rate but also results in the formation of calcium oxide (CaO) and carbon dioxide (CO 2 ), allowing the by-product aluminum oxide (Al 2 O 3 ) to float on the surface of the Cu. The CO 2 acts as a protective gas, preventing excessive oxidation of Al. Additionally, the inclusion of boron (B) powder can react with excess CuO, modulating the reaction rate between Al and CuO while producing B 2 O 3 , thereby promoting effective separation of slag from molten metal droplets. Utilizing these advantageous material properties, precise proportions of the reactive components were determined to yield Pre-Mixed Metal Powder Materials (PMMPM). This stage aimed to establish control over the reaction between Al and CuO during heat source formation and movement, thereby facilitating further separation of by-products from the deposited liquid metal. This strategic manipulation sought to improve the quality of the metal internals, minimize the physical distance between Al and CuO, enhance ORR ignition and combustion characteristics, and optimize the diffusion process of CuO, ultimately creating a continuously moving self-generated heat source ( 34 , 35 ). To achieve dense metal powders, low-viscosity printing inks were utilized to enhance the continuous printing of metal precursor powders within a polymer matrix. This modification yielded a high solids loading content of the metal precursor powder, thereby increasing the material's viscosity while diminishing light penetration depth and photosensitivity, elements that are incompatible with layerless AM processes ( 36 ). In contrast, the compact interaction between solid mixtures did not exhibit these performance deficiencies. Consequently, a comprehensive set of auxiliary structures was essential for achieving macroscopic control of the MD process, thereby facilitating the continuous progression of the entirety of the reaction. Accordingly, a curing agent was introduced during stage B to convert the powdered PMMPM into block C, resulting in the production of 3D Printing Supplies (3DPS). Details of the material preparation processes for stages A, B, and C are provided in Supplementary Data 3. The microscopic morphology of the MPM was examined using scanning electron microscopy (SEM) (Fig. 1 d), which indicated that Al effectively coated the surface of CuO flakes, thereby achieving robust inter-component bonding (Supplementary Data 4). The 3D printed materials produced through high-throughput experimentation and a bottom-up design strategy released substantial heat during combustion, with heat of combustion values for MPM, PMMPM, and 3DPS measuring 91,263.04 J, 65,516.27 J, and 75,864.45 J, respectively (Fig. 1 e). The notably lower heat of combustion for PMMPM compared to MPM is likely due to the incorporation of additional substances that participate in the Al/CuO reaction, which absorb a portion of the heat. The transition from PMMPM to 3DPS alters the temporary status of the material without fundamentally changing its internal structure and characteristics, resulting in only a slight difference in heat of combustion between 3DPS and PMMPM. To investigate the efficacy of our pre-fabricated materials in 3D printing applications, we filled 3DPS into a graphite groove and applied energy to ignite it. Observation and studies (Fig. 1 f) revealed that upon ignition, 3DPS initiated the ORR between Al and CuO (Supplementary Movie S1). The resulting molten liquid metal subsequently cooled and solidified, depositing within the graphite trough and forming a metallic luster. A layer of black, discontinuous impurities adhered to the surface, which X-ray photoelectron spectroscopy (XPS) analysis identified as pure Cu, while the black impurity was determined to be an Al 2 O 3 by-product, which could be dislodged through mechanical agitation (Supplementary Data 5). In the ORR, pure Cu was fully derived from CuO, with the reaction process releasing considerable heat and producing an Al 2 O 3 slag (Supplementary Data 6). Conventional metal 3D printing requires an external heat source to sinter and melt metal powder or wire material, which requires metal powder with high purity, high sphericity, fine particle size, and narrow particle size distribution. However, our pre-fabricated 3DPS has a strong molding ability, which not only does not require metal powder or wire material, but also does not require an external heat source for sintering and melting to obtain the desired molten liquid metal, which develops a more convenient material to use for the design of new methods of 3D printing. In use, only a very small current needs to be applied to 3DPS to excite the ORR and obtain molten liquid metal Cu, which can be cooled and solidified to obtain a metal structure with a geometrical shape. Therefore, 3DPS is expected to deposit liquid metal onto the substrate through the nozzle according to a predetermined path during the 3D printing process and obtain metal 3D spatial structures with certain geometrical patterns by layer-by-layer stacking. In addition, our pre-fabricated 3DPS does not have any limitations in terms of external shape and internal structure, and not only can it be molded arbitrarily, but also the metal oxides in the A-step can be replaced according to the actual needs. For example, by replacing CuO in step A with FeO, and then repeating the following steps, we can obtain metal products made of Fe, which greatly improves the flexibility of metal 3D printing technology in terms of the shape and type of the required materials, and fundamentally solves the high dependence of traditional 3D printing technology on the materials and the external heat source. 3DPS preparation avoids the need for AM for metal powders or wires and the defective structure of poor contact between the components. Components are not in close contact with each other as a structural defect, which provides strong material support for realizing high flexibility, high efficiency, and high precision AM. 2. SPEDT Printed Pure Cu The previous study utilized a bottom-up material synthesis strategy in conjunction with high-throughput experimentation to develop a novel consumable for metal 3D printing (Fig. 2 ). Initially, the specially formulated 3DPS was loaded into the crucible of the 3D printer. During the printing process, a resistive filament ignited the consumable, initiating an ORR process that generated liquid metal in a continuous manner. This liquid metal was subsequently injected and shaped through a fixed ceramic nozzle. To construct the desired part, a three-dimensional CAD model was layered and sliced using computer software to obtain the corresponding two-dimensional contour data. This contour data was then converted into the motion trajectory for the numerical control workbench ( Fig. 2 a). By meticulously regulating parameters such as the height, diameter, travel path, and speed of the nozzle, the injection and deposition of the liquid metal could be precisely controlled, facilitating the layer-by-layer construction of the part ( Fig. 2 b). To further investigate the combustion mechanism of 3DPS within the crucible, a comprehensive analysis was performed using physical model diagrams. The primer ignited through the application of an electric current (Fig. 2 c), which subsequently triggered the combustion of 3DPS, thereby stimulating the ORR and generating the initial heat source (Fig. 2 d). As the ORR progressed, the heat source expanded, leading to the consumption of 3DPS and the resultant formation of molten liquid metal. This molten metal exited the ceramic nozzle once formed. From the analysis, it is evident that the primary product of the reaction is liquid copper, while Al 2 O 3 slag, a by-product, rises toward the crucible's sidewalls due to gas flow (such as CO 2 ) and liquid buoyancy, thereby facilitating the effective separation of the metal from its by-products (Fig. 2 e). The tightly bound components of 3DPS maintain a continuous upward motion of the heat source, promoting the sustained execution of the ORR, which is a significant advantage of 3DPS. As sufficient liquid metal accumulates within the crucible, it is dispensed through the ceramic nozzle, imprinting a predefined pattern onto the substrate in accordance with the movement of the CNC table (Fig. 2 f). After a thorough analysis of the combustion mode and mechanism, experimental sample preparation for the 3D printing process was conducted. During the movement of the CNC table, the crucible is guided along a pre-defined trajectory corresponding to the pattern specifications. The 3D printing process in the post-ignition phase of 3DPS involves three primary steps: the formation of molten droplets, their ejection, and subsequent plasticization. Upon ignition, 3DPS transitions from a solid to a liquid state, resulting in the formation of molten droplets that are expelled from the ceramic nozzle. During the droplet ejection process, the liquid metal flows downward due to the combined effects of tension and gravity exerted by the walls of the ceramic orifice, which facilitates a smooth outflow of the droplets. The temperature of these molten droplets exhibits a declining trend. Specifically, the temperature in the vicinity of the nozzle falls within the range of 1083°C to 1283°C, nearing the melting point of Cu. As the droplets approach a right angle, their temperature decreases from 860°C to 1083°C, leading to a transition from a liquid state to a semi-solid state, which aids in their plasticization upon contact with the substrate. Upon reaching the substrate, the molten droplets gradually solidify at room temperature, below 860°C. I In the context of utilizing this 3D printing system, the distance between the nozzle and the substrate plays a critical role in determining the geometry of the printed object (Figs. 2 g and 2 j). Specifically, the height at which the nozzle is positioned above the substrate significantly influences the printed geometry. If the nozzle is situated too high, the molten droplets may solidify completely before being able to flow out, resulting in geometric patterns that are challenging to plasticize, as the droplets enter a supercooled state upon contact with the substrate. Conversely, if the nozzle is positioned too low, the droplets that land on the substrate remain in liquid form, and their high fluidity can lead to an improper stacking of layers, which may either be semi-solidified or fully solidified, thereby deviating from the intended geometric pattern ( Fig. 2 h and Fig. 2 k). Moreover, the rate at which the CNC table moves exerts a significant influence on the results of 3D printing. Excessively high speeds can lead to intermittent droplet ejection (Supplementary Movie S2), while slower speeds encourage droplet accumulation (Fig. 2 i and Fig. 2 l). This analysis underscores the importance of optimizing both the height of the nozzle and the movement speed to achieve the desired 3D printing patterns. Consequently, the optimal nozzle diameter, height, and movement speed were determined to be in the ranges of 2–9 mm, 10–15 mm, and 20–40 mm/s, respectively. The experiments successfully yielded 3D geometric patterns that corresponded with those designed in 3D CAD (Fig. 2 m). To ascertain the composition of the resultant geometric patterns, morphological and scanning analyses were conducted ( Fig. 2 n, Figs. 2 o and 2 p). The energy spectrum analysis revealed pronounced peak signals indicative of Cu, supporting the conclusion that high-purity metallic Cu can be successfully synthesized using the ORR method through the precise formulation of the components in the 3DPS. This technology eliminates the need for traditional heating and melting processes typically associated with metal materials, relying instead on the self-propagating reaction of 3DPS to produce liquid metal Cu. This approach significantly simplifies the fabrication process and reduces equipment complexity. Moreover, the fast propagation of the self-reaction facilitates a high printing speed and enhances the technology's adaptability for diverse substrate applications, including the repair of micro-cracks and AM on existing components. We propose utilizing this innovative method, referred to as SPEDT, which allows for the rapid production of three-dimensional metal structures characterized by uniform material distribution, elimination of heat source-induced sintering, and layer-free stacking. SPEDT bears similarities to traditional manufacturing techniques such as stereolithography (SLA), selective laser sintering (SLS), fused deposition modeling (FDM), powder bed fusion (PBF), and directed energy deposition (DED). In contrast to the intricacies inherent in multi-laser or multi-mode 3D printing technologies—such as electric arc methods and other advanced modalities ( 37 – 41 )—SPEDT offers several advantages: a streamlined powder preparation process, the absence of high-energy beam sintering and melting, and the elimination of conveyor systems. This improvement circumvents the adverse effects associated with the high reflectivity, electrical conductivity, and thermal conductivity of Cu powder when subjected to external heat sources for sintering. Additionally, SPEDT alleviates the complexities related to layer thickness resolution derived from 2D computer-aided design (CAD) images, a significant contributor to process flow complexity ( 42 ). Consequently, SPEDT not only enhances production efficiency but also reduces manufacturing costs, minimizes energy consumption, and lowers environmental pollution, thereby paving the way for large-scale production and engineering applications of copper-based superalloys. Furthermore, the technique entirely eliminates the detrimental impacts of external heat sources on the sintering and melting processes of metallic wires or powders, marking a revolutionary advancement in the field of additive manufacturing. 3. SPEDT Printed Cu Matrix Composites The SPEDT method effectively eliminates the reliance on external heat sources, enabling the production of liquid metals that facilitate AM through a layer-free stacking approach. This advancement significantly enhances the flexibility and efficiency of the deposition process, thereby offering considerable potential for large-scale engineering applications. To this end, we have established a comprehensive library of materials characterized by exceptional properties, including high thermal conductivity, high corrosion resistance, superconductivity, and high strength, through high-throughput experimentation (Fig. 3 a). This library enables precise and flexible formulation of material components, in situ alloying, and the development of copper-based composites, including variable-component gradient materials and nanoparticle-reinforced materials. This methodology contributes to both the high flexibility and efficiency of material preparation and provides robust technical support for the rapid research and development of new materials. Initially, various functional powders—comprising metals, non-metals, and composites—were mixed in single or composite combinations to achieve precise and flexible proportions of material components. These were subsequently incorporated into the B-step to generate the three-dimensional printing structure in the C-step. Subsequently, copper-based composites that meet the criteria for new materials were produced via the SPEDT technique (Supplementary Data 7). The functional powders were blended with molten liquid metal, leading to the formation of unique composite structures upon cooling and solidification, thus facilitating in situ alloying. The metallurgical reactions involving these functional powders were based on ORR, resulting in products that functioned as reinforcing phases dispersed uniformly within the liquid metal (Supplementary Data 8). This uniform distribution enhances both the microstructural and macroscopic properties of the copper-based composites. The 3D printing of copper-based composites eliminates the need for traditional sintering and melting processes that utilize external heat sources, demonstrating significant advantages in the development of new materials. To achieve rapid 3D printing of these composites, extensive experimentation with varying ratios of different functional powders was conducted, leading to the identification of optimal powder compositions that align with the desired material properties. Multiple sets of material morphologies with varying component ratios were synthesized (Supplementary Data 9). The resulting 3D-printed copper-based composites exhibited minimal structural defects, including cracks and voids; however, increased surface roughness was identified as an area for future enhancement. Microstructural analysis indicated a uniform distribution of tissue throughout the samples, with no observable cracks or pores (Supplementary Data 10). Among the evaluated samples, the Cu-based composites incorporating an 11% Ni60Cr40 alloy powder demonstrated superior mechanical properties (Supplementary Data 11). Observations via optical microscopy revealed the presence of deposited NiCr matrix grains, characterized by a regular dendritic structure in the horizontal plane (Fig. 3 b). The highest hardness values were recorded for composites utilizing a 5% WC88CO12 alloy powder ratio (Supplementary Data 11), which exhibited a lack of fine grains in the microstructural matrix (Fig. 3 c). This absence of fine grains inhibited both the formation and growth of dendrites, thereby facilitating a transition from elongated to shorter, rod-like dendrites. Consequently, this process resulted in the generation of fine grains and a significant quantity of equiaxial crystals, which impeded dislocation formation associated with cross-slip and pitting. Notably, the effects observed were comparable to those of intermetallic compounds, such as TiN and VC ( 43 ) or intercalation compounds with equivalent efficacy ( 38 ). In contrast, the Cu-based composites enhanced with ZrO 2 ceramic powder exhibited smooth interfaces free from cracks, mechanical interlocking, or porosity-related defects. The grayish-white ZrO 2 contributed to improvements in hardness, wear resistance, and corrosion resistance of the materials (Fig. 3 d). This finding suggests that SPEDT not only facilitates 3D printing of homogeneous materials but also demonstrates compatibility and efficacy between heterogeneous materials. The microhardness of various powder compositions, formulated in different ratios, was evaluated through high-throughput experiments. The maximum recorded hardness reached 543.75 HV, attributed to the NiCr-CrC metal powder (Fig. 3 e). Additionally, we employed an 11% Ag@Cu powder as the conductive medium, yielding Cu-based composites with a resistivity of 1.6 × 10 − 7 Ω·cm, indicative of their excellent conductive properties (Fig. 3 f). Furthermore, we assessed the corrosion resistance of the Cu-based composites. Utilizing a filler material comprising 14% NiCr-Cr3C2, the samples underwent salt spray corrosion testing, resulting in a minimal mass loss rate of 0.0088% (Fig. 3 g). This negligible change in quality demonstrates robust corrosion resistance, particularly in marine environments. Moreover, we integrated 7% NiCr-CrC functional powder to investigate the specific heat capacity through SPEDT printing of Cu-based composites. The results revealed a continuous increase in specific heat capacity with rising temperature; however, the slope of the corresponding curve decreased, indicating a reduction in the rate of change of specific heat capacity with temperature (Fig. 3 h). This observation is suggestive of excellent thermal conductivity. The incorporation of heterogeneous materials such as oxides, carbides, and ceramics—characterized by significant disparities in their intrinsic properties—has also facilitated the development of composites with outstanding functional compatibility via SPEDT. This advancement represents a significant contribution to the field of new material research. The near-zero loss associated with 3DPS during the fabrication of copper-based composites via SPEDT presents significant opportunities for the development of new materials with tailored properties. This is achieved through the precise control of material ratios and high throughput techniques, which facilitate accurate proportioning of compositional components. The adaptability of 3DPS to a diverse range of metal and ceramic powder materials, including refractory metals and carbides, further enhances the potential for constructing structures with varying physical and chemical characteristics. To harness these advantages, we have swiftly developed a material library through high-throughput experiments, enabling the efficient screening and development of new materials suitable for rapid printing of heterogeneous compositions. This approach significantly broadens the scope of reference for the efficient fabrication of innovative materials. Furthermore, SPEDT transcends the limitations associated with conventional manufacturing techniques pertaining to precision design and offers refined control over both the composition and microstructure of composite materials. Consequently, it holds considerable promise for widespread application in the printing of metals and other composite materials. 4. SPEDT printing of multicomponent gradient materials SPEDT enables the high-precision printing of periodic materials by alternately stacking multiple heterogeneous substances to create gradient materials that can perform multiple functions simultaneously. The ultra-flexibility of 3DPS allows for arbitrary adjustments in both the ratio and structure of each layer. As the crucible moves along a predetermined trajectory, it forms multi-component gradient materials with various combinations. The stacking mode employed in 3DPS significantly influences the characteristics of the final product. Under the longitudinal stacking mode (designated as Mode C), the 3DPS operates by igniting layers sequentially, resulting in the liquid metal ejected from the nozzle flowing in a single stream. Consequently, the printed multifunctional gradient material is constructed layer by layer (Fig. 4 a). In contrast, when the lateral stacking mode (also referred to as Mode C) is utilized, combustion occurs synchronously across different gradients after ignition. In this scenario, the liquid metal exiting the nozzle comprises several distinct layers, allowing for synchronized layering of the multifunctional gradient material (Fig. 4 b). By modifying the stacking pattern of the 3DPS, it is possible to minimize the contact gap between different gradients significantly. The aforementioned capability enhances design flexibility and facilitates the coordinated printing of both the composition and structure of multicomponent gradient materials. To mitigate the stepwise variation in elemental and thermophysical parameters, as well as the species and content of phases during the transition of gradient materials, it is essential to consider the properties of the final product obtained from the materials library ( 44 , 45 ). This necessitates the precise adjustment of both the compositional and structural gradients of 3DPS, enabling the development of novel materials characterized by innovative characteristics and high performance. In our research, we successfully synthesized multicomponent gradient materials comprising two or three layers facilitated by the materials library. The combination of Fe and Cu exhibited seamless bonding with minimal crack formation at the gradient interfaces. The high strength of Fe, when paired with the exceptional plastic toughness of Cu, resulted in a gradient structure featuring a smooth transition interface between the two metals (Fig. 4 c). This transition interface significantly enhances the bonding strength between Fe and Cu compared to conventional simple bonding methods. It effectively reduces stress concentration and the occurrence of defects, such as microcracks, at the interface, thereby improving the overall performance of the material. Additionally, we explored the printing of three-layer multicomponent gradient materials composed of Ni60WC45, Ni60WC35, and Ni70Cr3 (Fig. 4 d). In this configuration, key elements such as nickel (Ni), chromium (Cr), and tungsten (W) participated in diffusion and metallurgical bonding at the interfaces (Supplementary Data 12), resulting in a multicomponent gradient material that boasts diverse compositions and functionalities. SPEDT effectively achieves the desired compositional and structural gradients without excessive dependence on equipment or printing parameters. This method enables the simultaneous printing of multiple materials, thereby accommodating the compatibility of varied materials and significantly enhancing the likelihood of stable bonding to form a heterogeneous structure. Ultimately, this approach minimizes the potential for mismatches at the ends of the gradient. Conventional gradient materials are typically fabricated using a hot-cold stacking method between layers, a process that is highly susceptible to thermal accumulation and the development of crack defects. This presents significant challenges in the preparation of multicomponent gradient materials ( 46 , 47 ). In contrast, SPEDT offers distinct advantages for materials exhibiting both compositional and structural gradients. The inter-gradient bonding facilitated by the uniquely structured consumables in SPEDT utilizes a hot-hot stacking technique, which alleviates the need for meticulous management of printing parameters—such as temperature, flow rate, and deposition rate—required in traditional printing methods. This characteristic represents a significant advantage over conventional techniques. During the printing process, the upper layer of liquid metal is formed prior to the solidification of the lower layer, ensuring that the formation of adjacent gradients is consistently maintained throughout the thermal stacking process. This approach markedly reduces the temperature differentials between each layer of liquid metal (Fig. 4 e). Additionally, during thermal stacking, the two layers of liquid metal do not fuse with one another due to the surface fluid tension, allowing for a seamless transition between gradients without the interference of liquid flow infiltration characteristics. Consequently, SPEDT enables precise control over gradient transitions and promotes grain refinement within the metal and enhancing the microstructure of the material, which results in improved mechanical properties, including strength and toughness, and mitigates the risk of thermal accumulation and defect formation, such as cracks, within the material's structure. Simultaneously, the phase composition of the gradient material can be tailored by manipulating the composition and quantity of 3DPS, thereby achieving an optimal phase structure that enhances the performance of multi-component gradient materials. For intricate metal structures, such as aero-engine blades, the application of SPEDT facilitates the fabrication of complex geometries in a single step, circumventing the extensive cutting and assembly processes associated with traditional manufacturing methods. By fine-tuning the type and ratio of powders within the 3DPS, precise control over both the structure and composition of the printed material is attained. This approach not only enables the creation of new materials with functional gradients—ranging from homogeneous to heterogeneous structures—but also significantly simplifies the material preparation process. To address the varying material property requirements for specific application scenarios, we have successfully produced multi-component gradient materials via SPEDT that possess multiple functions and facilitate continuous gradient changes in a single direction. The continuous alteration in composition and structure allows different sections of the material to exhibit distinct functionalities. This innovative layered structure integrates the advantageous properties of multiple materials, thereby offering greater design flexibility for applications involving new material printing. The multi-component gradient materials fabricated through SPEDT demonstrate exceptional attributes, including high hardness (Figs. 4 f and 4 g), enhanced electrical conductivity (Fig. 4 h), and superior corrosion resistance (Fig. 4 i). These properties render them suitable for manufacturing high-voltage switches, power transformers, power capacitors, cores, and other electrical equipment, significantly improving the efficiency and stability of such systems. Moreover, SPEDT enables the deliberate placement of material components tailored to specific conditions, optimizing the composition ratio for desired alterations in structural properties. This results in the regional enhancement of mechanical properties, electrical and thermal conductivity, corrosion resistance, and metallurgical compatibility, while achieving a gradient distribution of properties and the selective integration of functionalities. SPEDT employs a self-developed technique known as 3DPS to accurately regulate the composition and structure of printing materials, which can obtain the powder with a precise ratio between each component. The process utilizes an innovative technique called ORR, whereby the powder is uniformly mixed through stirring and intermixing, leading to the formation of a continuously movable, self-generated heat source. Upon cooling and solidification, this results in a multi-component liquid metal that forms a gradient material, embodying the distinct characteristics of each constituent material. However, other metal AM technologies rely on external heat sources to melt metal powders, which can result in poor inter-powder contact, necessitating additional powder transfer devices. Such requirements not only increase manufacturing costs but also complicate the overall process. The SPEDT approach, in contrast, is independent of external heat sources and metal powders. It utilizes dispersed metal powders, which are processed into a tightly bonded block structure. The 3DPS generated through resistive filament excitation in conjunction with ORR facilitates the creation of liquid metal, enabling the manufacturing of geometric patterns as per on-demand designs. Traditional 3D printing methods are hindered by various limitations, including the necessity for pre-made powders, supplementary powder delivery devices, and considerations related to powder melting. The SPEDT method circumvents these challenges, allowing for the simultaneous printing of dozens to hundreds of multi-component gradient materials with varying compositions. This capability significantly reduces the research and development cycle and associated costs, thereby offering valuable insights for the design of alloy compositions prepared through additive manufacturing. Our research fundamentally redefines the design principles associated with traditional materials. First and foremost, the on-demand design of metal particles is achieved through 3DPS that facilitate high throughput and material library prefabrication. This approach offers several advantages, including a streamlined process, a high degree of design freedom, and the ability to create materials with gradient continuity. Consequently, it reshapes conventional design thinking and manufacturing methodologies. This innovation signifies not only disruptive advancements in processes and equipment but also a systematic overhaul of the entire workflow—from design and production to service. Moreover, SPEDT developed in conjunction with 3DPS leverages the benefits of self-propagating synthesis, enabling the synchronous or sequential printing of multi-component gradient materials. SPEDT is characterized by its high adaptability in front-end consumables design and new materials development, allowing for better control over the composition and structural regulation of novel materials. In this way, the preparation processes are significantly enhanced and material costs are reduced, thereby providing a groundbreaking solution for the design and development of new materials. SPEDT also addresses the limitations and complexities associated with traditional AM by enabling the precise proportioning of high-density metals, metal oxides, and multi-metal alloys. This capability compensates for the constraints of traditional single-material printing and offers unique advantages, particularly in the fabrication of gradient functional structures. Looking ahead, our research will concentrate on the systematic design of 3DPS through the application of material genetic engineering technology. We aim to develop micrometer-scale gradient materials with high efficacy, establish reliable databases through high-throughput experimental methods, and utilize first principles alongside artificial intelligence to guide the design and synthesis strategies for new materials. These efforts are expected to significantly shorten the development cycles of new materials while reducing associated research costs, ultimately accelerating the emergence of innovative materials needed for societal advancement. These materials are poised to find widespread application across various fields. Materials and Methods PVB ethanol solution preparation: 1.0 g of PVB was placed in a beaker, 200 mL of anhydrous ethanol was added, and a homogeneous ethanol solution of PVB was obtained after sealing and resting for 24 hours. Modified lamellar CuO: Transfer 15g of flaky CuO with a particle size of 1mm to a beaker, add 0.015g of citric acid, and mix well, then add 100mL of deionized water, place in an ultrasonic apparatus, and ultrasonic dispersed for 30 min, rest for 1 hour when the supernatant was poured off, rinsed with deionized water for 2 times to remove excess citric acid, and placed in a vacuum drying oven and dried at 80 °C. Trimming Spherical Al: 4g of spherical Al with a particle size of 10~100μm was placed in a beaker, 0.04g of CTAB (cetyltrimethylammonium bromide) powder was added and stirred homogeneously, 50mL of anhydrous ethanol was added and ultrasonically dispersed for 30 minutes, and then the supernatant was poured off after 1 hour of rest, and the excess CTAB was removed by rinsing with anhydrous ethanol for 2 times, and was dried in a vacuum oven at 80°C. The sample was then dried in a vacuum drying oven. Preparation of 3D Printing SuppliesPreparation of A: Weigh 15g of modified flake CuO and 4g of modified alumina in a beaker, mix well and add 80mL of isopropanol, ultrasonic dispersion for 10 minutes and then add PVB ethanol solution 0.5mL drop by drop, continue to ultrasonic for 20 minutes, and then pour off the supernatant after resting for 1 hour and then put it in a vacuum drying oven to vacuum-dry at 80°C to get the bonded aluminum thermite. Preparation of B: The prepared A was weighed 19.0 g, and 0.3 g of 100 μm B powder, 0.2 g of CaCO3, 0.2 g of CaO, and 1.0 g of Ni-Cr alloy were added, and placed in a mixing tube for 5 min to obtain B after mechanical mixing. Preparation of C: The ceramic abrasive was placed on a 304 stainless steel tape fitted with a temperature-controlled Cu mesh with wires, and B was transferred to the homemade ceramic abrasive, which was molded by adding 5 mL of PVB ethanol solution and then left to stand for 1 minute, and then the block C was obtained by standing and drying at room temperature. Test Analysis of A, B and C: The surface microstructure and elemental distribution of A, B and C were characterized by scanning electron microscopy (SEM) and energy spectrometry (EDS). The physical phase and crystal surface of A were characterized by an X-ray diffractometer (XRD). The valence changes of the elements in A were qualitatively analyzed by X-ray photoelectron spectroscopy (XPS) and surface charge correction was performed with 284.8 eV. The molecular functional group composition and structure in A were analyzed using Fourier transform infrared spectroscopy (FT-IR). The composition and crystal structure of A were qualitatively analyzed using Raman spectroscopy (Raman). Thermogravimetry (TG) and differential scanning calorimetry (DSC) were used to characterize the thermal stability of A, B and C. Based on this, the specific heat capacity calculation was carried out, which was used to study the combustion performance of A. The preparation process of 3D Printed Super Alloys 1. Modeling Modeling is the process of creating a digital model of an object. This process can be accomplished through computer-aided design (CAD) software. In CAD software, users can create a digital model of an object and edit and modify it. The digital model can be of any shape and size, from simple geometric shapes to complex organic shapes. 2 、 Slicing Slicing is the process of breaking down a digital model into a series of thin layers. This process can be accomplished through slicing software. In slicing software, the user can set the thickness of each layer and other parameters. The slicing software breaks down the digital model into a series of thin layers and transforms each layer into a set of instructions that will be used to control the printing process of the 3D printer. 3. Printing Printing is the process of transforming a digital model into a solid object. This process can be accomplished with a 3D printer. In a 3D printer, the print material is heated to the melting point and sprayed through a nozzle. The nozzle moves along the path of each layer and builds up the print material layer by layer until the entire object is created. Analytical Test Methods for Super Alloys Metallographic test solution was used to etch the ground and polished samples to show the morphology of the heat-affected zone, which facilitates the analysis of the cross-sectional morphology and microstructure of the metal deposited. A super depth-of-field three-dimensional microscope (VHX-5000) was used to observe the changes in the overall macroscopic morphology of the MD; the types and compositions of the interfacial elements were analyzed using a scanning electron microscope (SEM, Zeiss Supra55 VP) and an energy spectrometer (EDS, Bruker X-Flash SDD 5010), and the quantitative analysis of the elements was performed at the interfacial bonding, which facilitated the analysis of the temperature effect on element diffusion; and the composition of the physical phase on the fracture surface of the joints was analyzed by x-ray diffractometer (XRD). Declarations Data availability The datasets generated and/or analysed during the current study are available from the corresponding author on reasonable request. Author Contribution Yan Zhang contributed to the conception of the study; GuangZhen Ren performed the experiment; YuQiang Liu contributed significantly to analysis and manuscript preparation; Chen Yu helped perform the analysis with constructive discussions. Acknowledgements This research was mainly supported by Project funded by China Postdoctoral Science Foundation(2019M663861). This project is supported by the National Natural Science Foundation of China (Grant No.5210040951). Additional information Competing interests The authors declare no competing interests. References Zeng M, Du Y, Jiang Q et al (2023) High-throughput printing of combinatorial materials from aerosols[J]. Nature. 10.1038/s41586-023-05898-9 Green ML, Takeuchi I, Hattrick-Simpers JR (2013) Applications of high throughput (combinatorial) methodologies to electronic, magnetic, optical, and energy-related materials[J]. J Appl Phys, 113(23) Chen X, Liu X, Ouyang M et al Multi-metal 4D printing with a desktop electrochemical 3D printer.[J].Scientific Reports, 2019(1) Reiser A,Lindén, Rohner M (2019) P, Multi-metal electrohydrodynamic redox 3D printing at the submicron scale[J]. Nat Commun, 10(1) Queraltó A et al (2021) Combinatorial screening of cuprate superconductors by drop-on-demand inkjet printing. ACS Appl Mater Interfaces 13(7):9101–9112 Alqutaibi AY, Alghauli MA, Aljohani MHA et al (2024) Advanced additive manufacturing in implant dentistry: 3D printing technologies, printable materials, current applications and future requirements[J]. Bioprinting, : e00356 Wang Y, Wu T, Huang G (2024) State-of-the-art research progress and challenge of the printing techniques, potential applications for advanced ceramic materials 3D printing[J]. Mater Today Commun, : 110001 Jin H, Yang Z, Zhong J et al (2019) Mechanical and dielectric properties of 3D printed highly porous ceramics fabricated via stable and durable gel ink[J]. J Eur Ceram Soc 39(15):4680–4687 Kernan BD, Sachs EM, Oliveira MA et al (2007) Three-dimensional printing of tungsten carbide–10 wt% cobalt using a cobalt oxide precursor[J]. Int J Refract Met Hard Mater 25(1):82–94 Bauer J, Crook C, Baldacchini T (2023) A sinterless, low-temperature route to 3D print nanoscale optical-grade glass[J]. Science 380(6648):960–966 Zhang D, Liu X, Qiu J (2021) 3D printing of glass by additive manufacturing techniques: a review[J]. Front Optoelectron 14:263–277 Pal AK, Mohanty AK, Misra M (2021) Additive manufacturing technology of polymeric materials for customized products: recent developments and future prospective[J]. RSC Adv 11(58):36398–36438 Dul S, Fambri L, Pegoretti A (2016) Fused deposition modelling with ABS–graphene nanocomposites [J]. Compos Part A: Appl Sci Manufac 85:181–191 Akhoundi B, Sousani F (2024) An experimental investigation of screw-based material extrusion 3D printing of metallic parts[J]. J Eng Res 12(2):226–232 Dul S, Perret E, Hufenus R (2024) Bicomponent melt-spinning of filaments for material extrusion 3D printing[J]. Additive Manuf 85:104165 Dul S, Fambri L, Pegoretti A (2021) High-performance polyamide/carbon fiber composites for fused filament fabrication: mechanical and functional performances[J]. J Mater Eng Perform 30:5066–5085 Grossin DA, Montón, Navarrete-Segado P et al (2021) A review of additive manufacturing of ceramics by powder bed selective laser processing (sintering/melting): Calcium Phosphate, Silicon Carbide, Zirconia, Alumina, and their composites[J]. Open Ceramics Ang X, Tey JY, Yeo WH et al (2023) A review on metallic and ceramic material extrusion method: Materials, rheology, and printing parameters[J]. J Manuf Process 90:28–42 Ignatyev IA, Thielemans W, Vander Beke B (2014) Recycling of polymers: a review[J]. Chemsuschem 7(6):1579–1593 Singh N, Hui D, Singh R et al (2017) Recycling of plastic solid waste: A state of art review and future applications[J]. Compos Part B: Eng 115:409–422 Yang Y, Boom R, Irion B et al (2012) Recycling of composite materials[J]. Chem Eng Process 51:53–68 Taneepanichskul N, Purkiss D, Miodownik M (2022) A review of sorting and separating technologies suitable for compostable and biodegradable plastic packaging[J]. Front Sustain 3:901885 Olakanmi EO, Cochrane RF, Dalgarno KW (2015) A review on selective laser sintering/melting (SLS/SLM) of aluminium alloy powders: Processing, microstructure, and properties[J]. Prog Mater Sci 74:401–477 Jakus AE, Taylor SL, Geisendorfer NR et al (2015) Metallic architectures from 3D-printed powder‐based liquid inks[J]. Adv Funct Mater 25(45):6985–6995 Williams CB, Cochran JK, Rosen DW (2011) Additive manufacturing of metallic cellular materials via three-dimensional printing[J]. Int J Adv Manuf Technol 53:231–239 Sakib-Uz-Zaman C, Khondoker MAH (2023) A Review on Extrusion Additive Manufacturing of Pure Copper[J]. Metals 13(5):859 Li J, Huang Z, He B et al (2024) Experimental investigation of material extrusion additive manufacturing of copper with high powder loading rate[J]. J Mater Res Technol 33:2568–2579 Guschlbauer R, Burkhardt AK, Fu Z et al (2020) Effect of the oxygen content of pure copper powder on selective electron beam melting[J]. Mater Sci Engineering: A 779:139106 Santos C, Gatões D, Cerejo F et al (2021) Influence of metallic powder characteristics on extruded feedstock performance for indirect additive manufacturing[J]. Materials 14(23):7136 Lee K, Kim D, Shim J et al (2015) Formation of Cu layer on Al nanoparticles during thermite reaction in Al/CuO nanoparticle composites: Investigation of off-stoichiometry ratio of Al and CuO nanoparticles for maximum pressure change[J]. Combust Flame 162(10):3823–3828 Song P, Wen D, Guo ZX et al (2008) Oxidation investigation of nickel nanoparticles[J]. Phys Chem Chem Phys 10(33):5057–5065 Zhang X, Guo N, Xu C et al (2019) Influence of CaF2 on microstructural characteristics and mechanical properties of 304 stainless steel underwater wet welding using flux-cored wire[J]. J Manuf Process 45:138–146 Suga Y, Hasui A (1986) on The Formation of Porosity in Underwater Weld Metal (The 1st Report), Effect of Water Pressure on Formation of Porosity: IIW Doc[R]. IX-1388-86, American Council, AWS, Miami, FI Deng S, Jiang Y, Huang S et al (2018) Tuning the morphological, ignition and combustion properties of micron-Al/CuO thermites through different synthesis approaches[J]. Combust Flame 195:303–310 Wan C, Xiong Y, Qin H et al (2024) Precisely regulating combustion and ectrostatic discharge safety properties of Al/CuO nanothermite by inserting g-C3N4 nanosheet[J]. Appl Surf Sci 661:160044 Li C, Du J, Gao Y et al (2022) Stereolithography of 3D sustainable metal electrodes towards high-performance nickel iron battery[J]. Adv Funct Mater 32(40):2205317 Shahzadi L, Maya F, Breadmore MC et al (2022) Functional materials for DLP-SLA 3D printing using thiol–acrylate chemistry: Resin design and postprint applications[J]. ACS Appl Polym Mater 4(5):3896–3907 Xu X, Goyanes A, Trenfield SJ et al (2021) Stereolithography (SLA) 3D printing of a bladder device for intravesical drug delivery[J]. Mater Sci Engineering: C 120:111773 Sun X, Chen S, Qu B et al (2023) Light-oriented 3D printing of liquid crystal/photocurable resins and in-situ enhancement of mechanical performance[J]. Nat Commun 14(1):6586 Awad A, Fina F, Goyanes A et al (2021) Advances in powder bed fusion 3D printing in drug delivery and healthcare[J]. Adv Drug Deliv Rev 174:406–424 Svetlizky D, Das M, Zheng B et al (2021) Directed energy deposition (DED) additive manufacturing: Physical characteristics, defects, challenges and applications[J]. Mater Today 49:271–295 Joralmon D, Tang T, Prakash SR et al (2024) Continuous 3D printing of metal structures using ultrafast mask video projection initiated vat photopolymerization[J]. Additive Manuf 89:104314 Li N, Huang S, Zhang G et al (2019) Progress in additive manufacturing on new materials: A review[J]. J Mater Sci Technol 35(2):242–269 Liu L et al (2024) Additive manufacturing of multi-materials with interfacial component gradient by in-situ powder mixing and laser powder bed fusion. J Alloys Compd 978:173508 Liu C et al (2022) Dynamic recrystallization behavior under steady and transient mutation deformation state. Mater Sci Engineering: A Zhu C et al (2024) Toward Multiscale, Multimaterial 3D Printing. Adv Mater : 2314204 Zhou Y, Saitou K (2018) Gradient-based multi-component topology optimization for manufacturability [J].Structural and Multidisciplinary Optimization. Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryMovieS1.mp4 Supplementary Movie S1 SupplementaryMovieS2.mp4 Supplementary Movie S2 SupplementaryData.docx Supplementary Data SupplementaryText.docx Cite Share Download PDF Status: Published Journal Publication published 03 Nov, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6071151","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":425170033,"identity":"6b3e5ffb-c14f-45f9-ae51-f76be167fb12","order_by":0,"name":"yan zhang","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA8ElEQVRIiWNgGAWjYJACZhDB2N58/McHAxs74rUw9xxLkJxRkJZMvBb2GTkK0jwfDjE2EFJucPzs4c8FNXfsemfkMBjbGBxgZmA/fHQDXi1n8hKMZxx7ljyz5+2B5ByDO3wMPGlpN/BqOZBjkMzDdjjZsD0v4XCOwTNmBgkeM/xazr8xOMzz73Cy/YEcw2YLg8OMDQS13ACq5G07bMfYkWPMzECMFskbb4yZefsOJzD2HEtj7DFIS2Yj5Be+8znGn3m+HbYHRuUxhh9/bOz42Q8fw6tF4QCETmyAibDhUw4C8lCl9oQUjoJRMApGwQgGAINJUabCOLH/AAAAAElFTkSuQmCC","orcid":"https://orcid.org/0000-0002-1132-1147","institution":"Xinjiang University","correspondingAuthor":true,"prefix":"","firstName":"yan","middleName":"","lastName":"zhang","suffix":""},{"id":425170034,"identity":"83ecab40-95b9-4bfd-93ab-d9e869483e9b","order_by":1,"name":"yuqiang liu","email":"","orcid":"","institution":"xinjiang","correspondingAuthor":false,"prefix":"","firstName":"yuqiang","middleName":"","lastName":"liu","suffix":""},{"id":425170035,"identity":"496a46a8-bd2c-419e-85cd-177237ccb11b","order_by":2,"name":"jianping zhou","email":"","orcid":"","institution":"xinjiang","correspondingAuthor":false,"prefix":"","firstName":"jianping","middleName":"","lastName":"zhou","suffix":""},{"id":425170036,"identity":"ecc197af-a354-4b03-bd43-7bdc50b3d596","order_by":3,"name":"daqian sun","email":"","orcid":"","institution":"jilin","correspondingAuthor":false,"prefix":"","firstName":"daqian","middleName":"","lastName":"sun","suffix":""}],"badges":[],"createdAt":"2025-02-20 10:45:35","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6071151/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6071151/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41467-025-65189-x","type":"published","date":"2025-11-03T05:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":77964050,"identity":"9a3a87e2-66b6-4728-8dcb-175c8643bf71","added_by":"auto","created_at":"2025-03-07 09:35:11","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":1138201,"visible":true,"origin":"","legend":"\u003cp\u003ePreparation of 3D printing consumables: (a) ORR, (b) high-throughput experimental design scheme, (c) top-down material synthesis strategy, (d) SEM of Al/CuO, (e) combustion properties at different synthesis stages, and (f) MD process.\u003c/p\u003e","description":"","filename":"image1.png","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/1d8fd29fbcaa55d491d5e8ad.png"},{"id":77963744,"identity":"837ed611-f8f3-47a8-8fb5-a9a9d1131b43","added_by":"auto","created_at":"2025-03-07 09:27:11","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":1535838,"visible":true,"origin":"","legend":"\u003cp\u003eSPEDT printing structure design and mechanism analysis: (a) 3D printing equipment model diagram, (b) printer mechanism, (c) the primer inside the crucible starts to burn, (d) the heat source starts to form, (e) slag is formed, (f) the heat source moves and the molten droplets flow out, (g) the process of the molten droplets' change and the printer mechanism, (h) the influence of the nozzle's position on the shape of the deposition, (i) the influence of the movement speed of the control console on the deposition effect, (j) 3D printing experiments of H and V in the appropriate range, (k) discontinuous deposition shape formed when the nozzle position is too high or too low, (l) stacked deposition shape formed when the console moves too fast or too slow, (m) geometric patterns drawn by SPEDT, (n) SEM of Cu alloy, (o) full spectrum of maping region, (p) distribution of Cu elements,(q) energy spectrum.\u003c/p\u003e","description":"","filename":"image2.png","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/57839a2f74f37b57d36b3839.png"},{"id":77963741,"identity":"b5c360f8-4116-47c9-b910-bae6fba47e9e","added_by":"auto","created_at":"2025-03-07 09:27:11","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":1094984,"visible":true,"origin":"","legend":"\u003cp\u003ePreparation of superalloys by SPEDT. (a) Design concept of superalloys, (b) free-form proportioning and microstructure of functional powder Ni60Cr40, (c) free-form proportioning and microstructure of functional powder WC88CO12, (d) free-form proportioning and microstructure of functional powder ZrO\u003csub\u003e2\u003c/sub\u003e , (e) microhardness of superalloys prepared by high-throughput experiments, (f) electrical conductivity of superalloys, (g) corrosion resistance properties, (h) specific heat capacity.\u003c/p\u003e","description":"","filename":"image3.png","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/759621a960ae774d7ab494ba.png"},{"id":77963742,"identity":"24cf08b4-c8e3-4c71-8462-9c3c806463ac","added_by":"auto","created_at":"2025-03-07 09:27:11","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":1584505,"visible":true,"origin":"","legend":"\u003cp\u003eSPEDT printing of multifunctional gradient materials. (a) longitudinal burning of consumables, (b) Transverse burning of consumables, (c) Scanning of Fe/Cu multifunctional gradient material, (d) Scanning of Ni60WC45/Ni60WC35/Ni70Cr30 multifunctional gradient material, (e) Physical modeling diagrams of the combustion mode of consumable C and the printing process, (f) Microhardness of Cu/NiCr-CrC multifunctional gradient material, (g) microhardness of Ni60WC45/Ni60WC35/Ni70Cr30, (h) volume resistivity of Cu/Ag@Cu multifunctional gradient material, (i) corrosion properties of Cu/NiCr-Cr\u003csub\u003e3\u003c/sub\u003eC\u003csub\u003e2\u003c/sub\u003e multifunctional gradient material.\u003c/p\u003e","description":"","filename":"image4.png","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/fa0396a1939cabb6b1d357a8.png"},{"id":95089674,"identity":"92525154-264c-4f85-91df-fe9d64bb31aa","added_by":"auto","created_at":"2025-11-04 08:07:39","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":5662850,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/16cb304f-780e-4d0e-8a89-3b17278408dc.pdf"},{"id":77963739,"identity":"04cad8f4-ae03-4b54-a551-68427b44028e","added_by":"auto","created_at":"2025-03-07 09:27:11","extension":"mp4","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":791809,"visible":true,"origin":"","legend":"Supplementary Movie S1","description":"","filename":"SupplementaryMovieS1.mp4","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/129225c1a7dd76ba0a0fb84f.mp4"},{"id":77964051,"identity":"d9bbf03f-23c0-48f6-a125-ea908521e6fb","added_by":"auto","created_at":"2025-03-07 09:35:11","extension":"mp4","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":140042,"visible":true,"origin":"","legend":"\u003cp\u003eSupplementary Movie S2\u003c/p\u003e","description":"","filename":"SupplementaryMovieS2.mp4","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/1f1e5636e872f90d57411f9c.mp4"},{"id":77963748,"identity":"7d7cd5bb-877e-4b56-a3d6-0d069a40c0ab","added_by":"auto","created_at":"2025-03-07 09:27:11","extension":"docx","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":10931152,"visible":true,"origin":"","legend":"\u003cp\u003eSupplementary Data\u003c/p\u003e","description":"","filename":"SupplementaryData.docx","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/84df1ada65155be63964a83a.docx"},{"id":77963737,"identity":"c0b71849-23eb-4443-9a33-36eb3eabd686","added_by":"auto","created_at":"2025-03-07 09:27:11","extension":"docx","order_by":4,"title":"","display":"","copyAsset":false,"role":"supplement","size":14324,"visible":true,"origin":"","legend":"","description":"","filename":"SupplementaryText.docx","url":"https://assets-eu.researchsquare.com/files/rs-6071151/v1/bc8bf8ba39bd482fd08ba39f.docx"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"High-throughput printing of functionally gradient material from self-propagation","fulltext":[{"header":"Introduction","content":"\u003cp\u003eMaterials are fundamental to numerous scientific and technological innovations, and advancements in the development of new materials are crucial for addressing significant societal challenges. Three-dimensional (3D) printing, as a leading-edge and widely adopted technology in additive manufacturing (AM), primarily relies on digitally designed models to construct targeted objects. This technology builds items through sequential layering of materials, employing a layer-by-layer stacking and superimposition technique to achieve complex 3D structures, thus providing a practical alternative for the fabrication of intricate and hollow components (6-9). Currently, the most advanced 3D printing technologies are predominantly based on thermoplastic processes, including melting and particle sintering (10,11). During the AM process, raw materials are transformed into filaments, which are subsequently melted via heating within a nozzle and deposited onto a substrate (12,13). This additional step not only elevates manufacturing costs but also presents challenges, as certain thermoplastic polymers cannot be entirely converted into filaments (14). Although the filament-based extrusion process offers simplicity and flexibility for metal 3D printing, it is constrained by its layer-by-layer stacking methodology (15). For instance, the inherent layer-by-layer structure often results in adhesion issues and voids between layers, adversely affecting the mechanical properties of the printed objects (16). Furthermore, residual powder generated during the sintering process may undergo melting, rendering it unsuitable for reuse and escalating material reprocessing costs (17, 18). The recycling of polymer materials poses further complications, as the identification and separation of different polymers are inherently challenging due to variations in their chemical properties (19). This complexity not only amplifies printing costs but may also lead to material degradation or environmental pollution. Consequently, even after recycling, the presence of polymers with disparate thermal properties can generate undesirable by-products in the final printed products (20-22). Moreover, the sintering process in metal 3D printing is accompanied by oxidation, necessitating the establishment of an inert environment. The oxide layer that forms inhibits the wettability of liquid metal with the powder, leading to porosity in the final product (23). While metal oxides provide several benefits over traditional metal powders\u0026mdash;including lower costs, availability in submicron sizes, and reduced reactivity\u0026mdash;their high melting points hinder the effective application of high-energy beams required for sintering (24,25). Consequently, the interplay of heat source limitations and print material constraints, coupled with the absence of a flexible handling mechanism for the printing materials, results in restricted material options and challenges in the universal integration of diverse materials and the development of gradient material libraries.\u003c/p\u003e\n\u003cp\u003eIn order to address the challenges associated with beam heat source sintering and the recycling of metallic materials, a new paradigm is required to facilitate high-quality manufacturing and economic integration of 3D printing in the metalworking sector. We propose a Self-Propagating Energy Deposition Technology (SPEDT) that leverages the spontaneous behavior of the Oxidation-Reduction Reaction (ORR). This innovative method eliminates the need for an external heat source, requiring only the energization and ignition of bulk metal during the printing process to produce molten metal directly. Consequently, SPEDT enables multimaterial 3D printing while avoiding the inherent limitations of conventional thermoplastic 3D printing techniques for metals, significantly simplifying the manufacturing process. In our study, we designed a granular plate structure that is capable of spontaneous progression utilizing a bottom-up fabrication strategy. This approach allows for the use of the liquid metal generated through the continuous ORR to facilitate a multimaterial 3D printing process. As a result, this method enables on-demand design capabilities and the formation of patterned macrostructures. The new materials produced through this heat-free sintering method have demonstrated exceptional mechanical properties, heat resistance, high electrical conductivity, corrosion resistance, and other characteristics typically associated with superalloys. SPEDT effectively overcomes the limitations imposed by traditional metal 3D printing methods, which often rely on external heat sources, suffer from oxidized layer formation, exhibit limited recyclability of waste metal powders, and incur high operational costs. This novel approach presents significant potential for mass production in the development of new materials. By circumventing irregularities found in layer-by-layer assembly, SPEDT enhances final product performance through precise control over the composition ratios of the materials used, resulting in superior material properties once the printed structure has cooled and solidified. SPEDT represents a highly efficient, non-contact AM technology that confines the dispersion of liquid metal through a nozzle, enabling the formation of specific jet amplitudes for on-demand geometric pattern manufacturing. Compared to traditional material printing techniques, SPEDT offers precise control over heterogeneous interfaces, thereby facilitating the creation of more complex structures. It has broad applicability in areas that require intricate model designs, such as human skeletal reconstructions, engine blocks, and customized architectural projects, thus providing a novel solution for the design and fabrication of advanced materials. Such an innovative AM technique paves the way for new strategies in material design and synthesis.\u003c/p\u003e\n\u003ch3\u003e1. Preparation and properties of 3DPS\u003c/h3\u003e\n\u003cp\u003eCopper (Cu) plays a vital role in high-temperature applications due to its exceptional thermal and electrical conductivity (\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e). However, the increasing demand for complex structural components has rendered traditional methods of fabricating pure Cu insufficient to meet these needs. Currently, three-dimensional (3D) metallic structures of Cu are predominantly produced through AM techniques, including Selective Laser Melting, Electron Beam Melting, and Directed Energy Deposition (\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e). These methods require an external heat source (e.g., laser or electron beam) as well as metal powder or wire. The high reflectivity of Cu significantly diminishes the efficiency of energy utilization, presenting challenges for beam-based AM of metallic materials (\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e, \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e). To address these challenges, we developed a precursor material aimed at the preparation of novel materials. We formulated a composite system of aluminum (Al) and copper(II) oxide (CuO) in paste form, accompanied by plasticization, to exploit the spontaneous ORR (\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e). This approach leverages the inherent capacity of reducing CuO to pure Cu and facilitates metal deposition (MD) (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea), leading to the successful precipitation of pure metal. The Al/CuO nanoparticle composite demonstrated a high reaction rate owing to the abundance of reaction sites created by the large surface area of the composite, thereby enhancing its overall reactivity (\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e). The simplicity of the excitation conditions required for spontaneous and continuous reaction progression stimulated further development of Al/CuO-based systems.\u003c/p\u003e \u003cp\u003eBuilding on the favorable combustion characteristics and reaction products of the Al/CuO composite system (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb), we designed consumables capable of 3D printing metallic materials using a bottom-up material synthesis strategy (Supplementary Data 1) and high-throughput experiments (Supplementary Data 2). The preparation process for specific 3D printed materials was delineated into three stages, designated A, B, and C (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec). In stage A, to enhance the binding properties between Al and CuO, their surface viscosities were modified with Polyvinyl Butyral (PVB) in an ethanol solution. This modification promoted cohesive binding and facilitated surface assembly, resulting in the formation of Metal Precursor Materials (MPM). Through high-throughput experimentation, over 300 experimental configurations were evaluated to optimize the particle plate structure for MPM, ultimately leading to the identification of a configuration that facilitated the formation of metal-based alloys with a stable combustion process and superior performance. However, further modification of the deposited Cu was required due to issues related to inferior mechanical properties, porosity, difficulties in slag separation, and limited controllability of the reaction rate. To mitigate these challenges, we incorporated calcium fluoride (CaF\u003csub\u003e2\u003c/sub\u003e) in stage B to enhance the strength of the MD within the MPM. The reaction between Al and CuO is critical in CuO development, as is the self-reaction of CuO. Given that the Al-CuO reaction is exothermic, and recognizing that CaF\u003csub\u003e2\u003c/sub\u003e can absorb oxygen and hydrogen from the environment, the oxidation and hydrogen cracking of the MD are inhibited at elevated temperatures (\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e, \u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e). Furthermore, the rapid reaction of Al with CuO, combined with the addition of calcium carbonate (CaCO\u003csub\u003e3\u003c/sub\u003e), not only moderates the reaction rate but also results in the formation of calcium oxide (CaO) and carbon dioxide (CO\u003csub\u003e2\u003c/sub\u003e), allowing the by-product aluminum oxide (Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e) to float on the surface of the Cu. The CO\u003csub\u003e2\u003c/sub\u003e acts as a protective gas, preventing excessive oxidation of Al. Additionally, the inclusion of boron (B) powder can react with excess CuO, modulating the reaction rate between Al and CuO while producing B\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, thereby promoting effective separation of slag from molten metal droplets. Utilizing these advantageous material properties, precise proportions of the reactive components were determined to yield Pre-Mixed Metal Powder Materials (PMMPM). This stage aimed to establish control over the reaction between Al and CuO during heat source formation and movement, thereby facilitating further separation of by-products from the deposited liquid metal. This strategic manipulation sought to improve the quality of the metal internals, minimize the physical distance between Al and CuO, enhance ORR ignition and combustion characteristics, and optimize the diffusion process of CuO, ultimately creating a continuously moving self-generated heat source (\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e, \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eTo achieve dense metal powders, low-viscosity printing inks were utilized to enhance the continuous printing of metal precursor powders within a polymer matrix. This modification yielded a high solids loading content of the metal precursor powder, thereby increasing the material's viscosity while diminishing light penetration depth and photosensitivity, elements that are incompatible with layerless AM processes (\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e). In contrast, the compact interaction between solid mixtures did not exhibit these performance deficiencies. Consequently, a comprehensive set of auxiliary structures was essential for achieving macroscopic control of the MD process, thereby facilitating the continuous progression of the entirety of the reaction. Accordingly, a curing agent was introduced during stage B to convert the powdered PMMPM into block C, resulting in the production of 3D Printing Supplies (3DPS). Details of the material preparation processes for stages A, B, and C are provided in Supplementary Data 3. The microscopic morphology of the MPM was examined using scanning electron microscopy (SEM) (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed), which indicated that Al effectively coated the surface of CuO flakes, thereby achieving robust inter-component bonding (Supplementary Data 4). The 3D printed materials produced through high-throughput experimentation and a bottom-up design strategy released substantial heat during combustion, with heat of combustion values for MPM, PMMPM, and 3DPS measuring 91,263.04 J, 65,516.27 J, and 75,864.45 J, respectively (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ee). The notably lower heat of combustion for PMMPM compared to MPM is likely due to the incorporation of additional substances that participate in the Al/CuO reaction, which absorb a portion of the heat. The transition from PMMPM to 3DPS alters the temporary status of the material without fundamentally changing its internal structure and characteristics, resulting in only a slight difference in heat of combustion between 3DPS and PMMPM. To investigate the efficacy of our pre-fabricated materials in 3D printing applications, we filled 3DPS into a graphite groove and applied energy to ignite it. Observation and studies (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ef) revealed that upon ignition, 3DPS initiated the ORR between Al and CuO (Supplementary Movie S1). The resulting molten liquid metal subsequently cooled and solidified, depositing within the graphite trough and forming a metallic luster. A layer of black, discontinuous impurities adhered to the surface, which X-ray photoelectron spectroscopy (XPS) analysis identified as pure Cu, while the black impurity was determined to be an Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e by-product, which could be dislodged through mechanical agitation (Supplementary Data 5). In the ORR, pure Cu was fully derived from CuO, with the reaction process releasing considerable heat and producing an Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e slag (Supplementary Data 6).\u003c/p\u003e \u003cp\u003eConventional metal 3D printing requires an external heat source to sinter and melt metal powder or wire material, which requires metal powder with high purity, high sphericity, fine particle size, and narrow particle size distribution. However, our pre-fabricated 3DPS has a strong molding ability, which not only does not require metal powder or wire material, but also does not require an external heat source for sintering and melting to obtain the desired molten liquid metal, which develops a more convenient material to use for the design of new methods of 3D printing. In use, only a very small current needs to be applied to 3DPS to excite the ORR and obtain molten liquid metal Cu, which can be cooled and solidified to obtain a metal structure with a geometrical shape. Therefore, 3DPS is expected to deposit liquid metal onto the substrate through the nozzle according to a predetermined path during the 3D printing process and obtain metal 3D spatial structures with certain geometrical patterns by layer-by-layer stacking. In addition, our pre-fabricated 3DPS does not have any limitations in terms of external shape and internal structure, and not only can it be molded arbitrarily, but also the metal oxides in the A-step can be replaced according to the actual needs. For example, by replacing CuO in step A with FeO, and then repeating the following steps, we can obtain metal products made of Fe, which greatly improves the flexibility of metal 3D printing technology in terms of the shape and type of the required materials, and fundamentally solves the high dependence of traditional 3D printing technology on the materials and the external heat source. 3DPS preparation avoids the need for AM for metal powders or wires and the defective structure of poor contact between the components. Components are not in close contact with each other as a structural defect, which provides strong material support for realizing high flexibility, high efficiency, and high precision AM.\u003c/p\u003e\n\u003ch3\u003e2. SPEDT Printed Pure Cu\u003c/h3\u003e\n\u003cp\u003eThe previous study utilized a bottom-up material synthesis strategy in conjunction with high-throughput experimentation to develop a novel consumable for metal 3D printing (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e). Initially, the specially formulated 3DPS was loaded into the crucible of the 3D printer. During the printing process, a resistive filament ignited the consumable, initiating an ORR process that generated liquid metal in a continuous manner. This liquid metal was subsequently injected and shaped through a fixed ceramic nozzle. To construct the desired part, a three-dimensional CAD model was layered and sliced using computer software to obtain the corresponding two-dimensional contour data. This contour data was then converted into the motion trajectory for the numerical control workbench ( Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea). By meticulously regulating parameters such as the height, diameter, travel path, and speed of the nozzle, the injection and deposition of the liquid metal could be precisely controlled, facilitating the layer-by-layer construction of the part ( Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb). To further investigate the combustion mechanism of 3DPS within the crucible, a comprehensive analysis was performed using physical model diagrams. The primer ignited through the application of an electric current (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec), which subsequently triggered the combustion of 3DPS, thereby stimulating the ORR and generating the initial heat source (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed). As the ORR progressed, the heat source expanded, leading to the consumption of 3DPS and the resultant formation of molten liquid metal. This molten metal exited the ceramic nozzle once formed. From the analysis, it is evident that the primary product of the reaction is liquid copper, while Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e slag, a by-product, rises toward the crucible's sidewalls due to gas flow (such as CO\u003csub\u003e2\u003c/sub\u003e) and liquid buoyancy, thereby facilitating the effective separation of the metal from its by-products (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee). The tightly bound components of 3DPS maintain a continuous upward motion of the heat source, promoting the sustained execution of the ORR, which is a significant advantage of 3DPS. As sufficient liquid metal accumulates within the crucible, it is dispensed through the ceramic nozzle, imprinting a predefined pattern onto the substrate in accordance with the movement of the CNC table (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef).\u003c/p\u003e \u003cp\u003eAfter a thorough analysis of the combustion mode and mechanism, experimental sample preparation for the 3D printing process was conducted. During the movement of the CNC table, the crucible is guided along a pre-defined trajectory corresponding to the pattern specifications. The 3D printing process in the post-ignition phase of 3DPS involves three primary steps: the formation of molten droplets, their ejection, and subsequent plasticization. Upon ignition, 3DPS transitions from a solid to a liquid state, resulting in the formation of molten droplets that are expelled from the ceramic nozzle. During the droplet ejection process, the liquid metal flows downward due to the combined effects of tension and gravity exerted by the walls of the ceramic orifice, which facilitates a smooth outflow of the droplets. The temperature of these molten droplets exhibits a declining trend. Specifically, the temperature in the vicinity of the nozzle falls within the range of 1083\u0026deg;C to 1283\u0026deg;C, nearing the melting point of Cu. As the droplets approach a right angle, their temperature decreases from 860\u0026deg;C to 1083\u0026deg;C, leading to a transition from a liquid state to a semi-solid state, which aids in their plasticization upon contact with the substrate. Upon reaching the substrate, the molten droplets gradually solidify at room temperature, below 860\u0026deg;C. I In the context of utilizing this 3D printing system, the distance between the nozzle and the substrate plays a critical role in determining the geometry of the printed object (Figs.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg and \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ej). Specifically, the height at which the nozzle is positioned above the substrate significantly influences the printed geometry. If the nozzle is situated too high, the molten droplets may solidify completely before being able to flow out, resulting in geometric patterns that are challenging to plasticize, as the droplets enter a supercooled state upon contact with the substrate. Conversely, if the nozzle is positioned too low, the droplets that land on the substrate remain in liquid form, and their high fluidity can lead to an improper stacking of layers, which may either be semi-solidified or fully solidified, thereby deviating from the intended geometric pattern ( Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eh and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ek). Moreover, the rate at which the CNC table moves exerts a significant influence on the results of 3D printing. Excessively high speeds can lead to intermittent droplet ejection (Supplementary Movie S2), while slower speeds encourage droplet accumulation (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003el). This analysis underscores the importance of optimizing both the height of the nozzle and the movement speed to achieve the desired 3D printing patterns. Consequently, the optimal nozzle diameter, height, and movement speed were determined to be in the ranges of 2\u0026ndash;9 mm, 10\u0026ndash;15 mm, and 20\u0026ndash;40 mm/s, respectively. The experiments successfully yielded 3D geometric patterns that corresponded with those designed in 3D CAD (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003em). To ascertain the composition of the resultant geometric patterns, morphological and scanning analyses were conducted ( Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003en, Figs.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eo and \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ep). The energy spectrum analysis revealed pronounced peak signals indicative of Cu, supporting the conclusion that high-purity metallic Cu can be successfully synthesized using the ORR method through the precise formulation of the components in the 3DPS.\u003c/p\u003e \u003cp\u003eThis technology eliminates the need for traditional heating and melting processes typically associated with metal materials, relying instead on the self-propagating reaction of 3DPS to produce liquid metal Cu. This approach significantly simplifies the fabrication process and reduces equipment complexity. Moreover, the fast propagation of the self-reaction facilitates a high printing speed and enhances the technology's adaptability for diverse substrate applications, including the repair of micro-cracks and AM on existing components. We propose utilizing this innovative method, referred to as SPEDT, which allows for the rapid production of three-dimensional metal structures characterized by uniform material distribution, elimination of heat source-induced sintering, and layer-free stacking. SPEDT bears similarities to traditional manufacturing techniques such as stereolithography (SLA), selective laser sintering (SLS), fused deposition modeling (FDM), powder bed fusion (PBF), and directed energy deposition (DED). In contrast to the intricacies inherent in multi-laser or multi-mode 3D printing technologies\u0026mdash;such as electric arc methods and other advanced modalities (\u003cspan additionalcitationids=\"CR38 CR39 CR40\" citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e)\u0026mdash;SPEDT offers several advantages: a streamlined powder preparation process, the absence of high-energy beam sintering and melting, and the elimination of conveyor systems. This improvement circumvents the adverse effects associated with the high reflectivity, electrical conductivity, and thermal conductivity of Cu powder when subjected to external heat sources for sintering. Additionally, SPEDT alleviates the complexities related to layer thickness resolution derived from 2D computer-aided design (CAD) images, a significant contributor to process flow complexity (\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e). Consequently, SPEDT not only enhances production efficiency but also reduces manufacturing costs, minimizes energy consumption, and lowers environmental pollution, thereby paving the way for large-scale production and engineering applications of copper-based superalloys. Furthermore, the technique entirely eliminates the detrimental impacts of external heat sources on the sintering and melting processes of metallic wires or powders, marking a revolutionary advancement in the field of additive manufacturing.\u003c/p\u003e\n\u003ch3\u003e3. SPEDT Printed Cu Matrix Composites\u003c/h3\u003e\n\u003cp\u003eThe SPEDT method effectively eliminates the reliance on external heat sources, enabling the production of liquid metals that facilitate AM through a layer-free stacking approach. This advancement significantly enhances the flexibility and efficiency of the deposition process, thereby offering considerable potential for large-scale engineering applications. To this end, we have established a comprehensive library of materials characterized by exceptional properties, including high thermal conductivity, high corrosion resistance, superconductivity, and high strength, through high-throughput experimentation (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea). This library enables precise and flexible formulation of material components, in situ alloying, and the development of copper-based composites, including variable-component gradient materials and nanoparticle-reinforced materials. This methodology contributes to both the high flexibility and efficiency of material preparation and provides robust technical support for the rapid research and development of new materials.\u003c/p\u003e \u003cp\u003eInitially, various functional powders\u0026mdash;comprising metals, non-metals, and composites\u0026mdash;were mixed in single or composite combinations to achieve precise and flexible proportions of material components. These were subsequently incorporated into the B-step to generate the three-dimensional printing structure in the C-step. Subsequently, copper-based composites that meet the criteria for new materials were produced via the SPEDT technique (Supplementary Data 7). The functional powders were blended with molten liquid metal, leading to the formation of unique composite structures upon cooling and solidification, thus facilitating in situ alloying. The metallurgical reactions involving these functional powders were based on ORR, resulting in products that functioned as reinforcing phases dispersed uniformly within the liquid metal (Supplementary Data 8). This uniform distribution enhances both the microstructural and macroscopic properties of the copper-based composites. The 3D printing of copper-based composites eliminates the need for traditional sintering and melting processes that utilize external heat sources, demonstrating significant advantages in the development of new materials. To achieve rapid 3D printing of these composites, extensive experimentation with varying ratios of different functional powders was conducted, leading to the identification of optimal powder compositions that align with the desired material properties.\u003c/p\u003e \u003cp\u003eMultiple sets of material morphologies with varying component ratios were synthesized (Supplementary Data 9). The resulting 3D-printed copper-based composites exhibited minimal structural defects, including cracks and voids; however, increased surface roughness was identified as an area for future enhancement. Microstructural analysis indicated a uniform distribution of tissue throughout the samples, with no observable cracks or pores (Supplementary Data 10). Among the evaluated samples, the Cu-based composites incorporating an 11% Ni60Cr40 alloy powder demonstrated superior mechanical properties (Supplementary Data 11). Observations via optical microscopy revealed the presence of deposited NiCr matrix grains, characterized by a regular dendritic structure in the horizontal plane (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb). The highest hardness values were recorded for composites utilizing a 5% WC88CO12 alloy powder ratio (Supplementary Data 11), which exhibited a lack of fine grains in the microstructural matrix (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec). This absence of fine grains inhibited both the formation and growth of dendrites, thereby facilitating a transition from elongated to shorter, rod-like dendrites. Consequently, this process resulted in the generation of fine grains and a significant quantity of equiaxial crystals, which impeded dislocation formation associated with cross-slip and pitting. Notably, the effects observed were comparable to those of intermetallic compounds, such as TiN and VC (\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e) or intercalation compounds with equivalent efficacy (\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e). In contrast, the Cu-based composites enhanced with ZrO\u003csub\u003e2\u003c/sub\u003e ceramic powder exhibited smooth interfaces free from cracks, mechanical interlocking, or porosity-related defects. The grayish-white ZrO\u003csub\u003e2\u003c/sub\u003e contributed to improvements in hardness, wear resistance, and corrosion resistance of the materials (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed). This finding suggests that SPEDT not only facilitates 3D printing of homogeneous materials but also demonstrates compatibility and efficacy between heterogeneous materials.\u003c/p\u003e \u003cp\u003eThe microhardness of various powder compositions, formulated in different ratios, was evaluated through high-throughput experiments. The maximum recorded hardness reached 543.75 HV, attributed to the NiCr-CrC metal powder (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee). Additionally, we employed an 11% Ag@Cu powder as the conductive medium, yielding Cu-based composites with a resistivity of 1.6 \u0026times; 10\u003csup\u003e\u0026minus;\u0026thinsp;7\u003c/sup\u003e Ω\u0026middot;cm, indicative of their excellent conductive properties (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef). Furthermore, we assessed the corrosion resistance of the Cu-based composites. Utilizing a filler material comprising 14% NiCr-Cr3C2, the samples underwent salt spray corrosion testing, resulting in a minimal mass loss rate of 0.0088% (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eg). This negligible change in quality demonstrates robust corrosion resistance, particularly in marine environments. Moreover, we integrated 7% NiCr-CrC functional powder to investigate the specific heat capacity through SPEDT printing of Cu-based composites. The results revealed a continuous increase in specific heat capacity with rising temperature; however, the slope of the corresponding curve decreased, indicating a reduction in the rate of change of specific heat capacity with temperature (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eh). This observation is suggestive of excellent thermal conductivity. The incorporation of heterogeneous materials such as oxides, carbides, and ceramics\u0026mdash;characterized by significant disparities in their intrinsic properties\u0026mdash;has also facilitated the development of composites with outstanding functional compatibility via SPEDT. This advancement represents a significant contribution to the field of new material research.\u003c/p\u003e \u003cp\u003eThe near-zero loss associated with 3DPS during the fabrication of copper-based composites via SPEDT presents significant opportunities for the development of new materials with tailored properties. This is achieved through the precise control of material ratios and high throughput techniques, which facilitate accurate proportioning of compositional components. The adaptability of 3DPS to a diverse range of metal and ceramic powder materials, including refractory metals and carbides, further enhances the potential for constructing structures with varying physical and chemical characteristics. To harness these advantages, we have swiftly developed a material library through high-throughput experiments, enabling the efficient screening and development of new materials suitable for rapid printing of heterogeneous compositions. This approach significantly broadens the scope of reference for the efficient fabrication of innovative materials. Furthermore, SPEDT transcends the limitations associated with conventional manufacturing techniques pertaining to precision design and offers refined control over both the composition and microstructure of composite materials. Consequently, it holds considerable promise for widespread application in the printing of metals and other composite materials.\u003c/p\u003e\n\u003ch3\u003e4. SPEDT printing of multicomponent gradient materials\u003c/h3\u003e\n\u003cp\u003eSPEDT enables the high-precision printing of periodic materials by alternately stacking multiple heterogeneous substances to create gradient materials that can perform multiple functions simultaneously. The ultra-flexibility of 3DPS allows for arbitrary adjustments in both the ratio and structure of each layer. As the crucible moves along a predetermined trajectory, it forms multi-component gradient materials with various combinations. The stacking mode employed in 3DPS significantly influences the characteristics of the final product. Under the longitudinal stacking mode (designated as Mode C), the 3DPS operates by igniting layers sequentially, resulting in the liquid metal ejected from the nozzle flowing in a single stream. Consequently, the printed multifunctional gradient material is constructed layer by layer (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea). In contrast, when the lateral stacking mode (also referred to as Mode C) is utilized, combustion occurs synchronously across different gradients after ignition. In this scenario, the liquid metal exiting the nozzle comprises several distinct layers, allowing for synchronized layering of the multifunctional gradient material (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb). By modifying the stacking pattern of the 3DPS, it is possible to minimize the contact gap between different gradients significantly. The aforementioned capability enhances design flexibility and facilitates the coordinated printing of both the composition and structure of multicomponent gradient materials.\u003c/p\u003e \u003cp\u003eTo mitigate the stepwise variation in elemental and thermophysical parameters, as well as the species and content of phases during the transition of gradient materials, it is essential to consider the properties of the final product obtained from the materials library (\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e, \u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e). This necessitates the precise adjustment of both the compositional and structural gradients of 3DPS, enabling the development of novel materials characterized by innovative characteristics and high performance. In our research, we successfully synthesized multicomponent gradient materials comprising two or three layers facilitated by the materials library. The combination of Fe and Cu exhibited seamless bonding with minimal crack formation at the gradient interfaces. The high strength of Fe, when paired with the exceptional plastic toughness of Cu, resulted in a gradient structure featuring a smooth transition interface between the two metals (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec). This transition interface significantly enhances the bonding strength between Fe and Cu compared to conventional simple bonding methods. It effectively reduces stress concentration and the occurrence of defects, such as microcracks, at the interface, thereby improving the overall performance of the material. Additionally, we explored the printing of three-layer multicomponent gradient materials composed of Ni60WC45, Ni60WC35, and Ni70Cr3 (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed). In this configuration, key elements such as nickel (Ni), chromium (Cr), and tungsten (W) participated in diffusion and metallurgical bonding at the interfaces (Supplementary Data 12), resulting in a multicomponent gradient material that boasts diverse compositions and functionalities. SPEDT effectively achieves the desired compositional and structural gradients without excessive dependence on equipment or printing parameters. This method enables the simultaneous printing of multiple materials, thereby accommodating the compatibility of varied materials and significantly enhancing the likelihood of stable bonding to form a heterogeneous structure. Ultimately, this approach minimizes the potential for mismatches at the ends of the gradient.\u003c/p\u003e \u003cp\u003eConventional gradient materials are typically fabricated using a hot-cold stacking method between layers, a process that is highly susceptible to thermal accumulation and the development of crack defects. This presents significant challenges in the preparation of multicomponent gradient materials (\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e, \u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e). In contrast, SPEDT offers distinct advantages for materials exhibiting both compositional and structural gradients. The inter-gradient bonding facilitated by the uniquely structured consumables in SPEDT utilizes a hot-hot stacking technique, which alleviates the need for meticulous management of printing parameters\u0026mdash;such as temperature, flow rate, and deposition rate\u0026mdash;required in traditional printing methods. This characteristic represents a significant advantage over conventional techniques. During the printing process, the upper layer of liquid metal is formed prior to the solidification of the lower layer, ensuring that the formation of adjacent gradients is consistently maintained throughout the thermal stacking process. This approach markedly reduces the temperature differentials between each layer of liquid metal (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee). Additionally, during thermal stacking, the two layers of liquid metal do not fuse with one another due to the surface fluid tension, allowing for a seamless transition between gradients without the interference of liquid flow infiltration characteristics. Consequently, SPEDT enables precise control over gradient transitions and promotes grain refinement within the metal and enhancing the microstructure of the material, which results in improved mechanical properties, including strength and toughness, and mitigates the risk of thermal accumulation and defect formation, such as cracks, within the material's structure.\u003c/p\u003e \u003cp\u003eSimultaneously, the phase composition of the gradient material can be tailored by manipulating the composition and quantity of 3DPS, thereby achieving an optimal phase structure that enhances the performance of multi-component gradient materials. For intricate metal structures, such as aero-engine blades, the application of SPEDT facilitates the fabrication of complex geometries in a single step, circumventing the extensive cutting and assembly processes associated with traditional manufacturing methods. By fine-tuning the type and ratio of powders within the 3DPS, precise control over both the structure and composition of the printed material is attained. This approach not only enables the creation of new materials with functional gradients\u0026mdash;ranging from homogeneous to heterogeneous structures\u0026mdash;but also significantly simplifies the material preparation process. To address the varying material property requirements for specific application scenarios, we have successfully produced multi-component gradient materials via SPEDT that possess multiple functions and facilitate continuous gradient changes in a single direction. The continuous alteration in composition and structure allows different sections of the material to exhibit distinct functionalities. This innovative layered structure integrates the advantageous properties of multiple materials, thereby offering greater design flexibility for applications involving new material printing. The multi-component gradient materials fabricated through SPEDT demonstrate exceptional attributes, including high hardness (Figs.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef and \u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eg), enhanced electrical conductivity (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eh), and superior corrosion resistance (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ei). These properties render them suitable for manufacturing high-voltage switches, power transformers, power capacitors, cores, and other electrical equipment, significantly improving the efficiency and stability of such systems. Moreover, SPEDT enables the deliberate placement of material components tailored to specific conditions, optimizing the composition ratio for desired alterations in structural properties. This results in the regional enhancement of mechanical properties, electrical and thermal conductivity, corrosion resistance, and metallurgical compatibility, while achieving a gradient distribution of properties and the selective integration of functionalities.\u003c/p\u003e \u003cp\u003eSPEDT employs a self-developed technique known as 3DPS to accurately regulate the composition and structure of printing materials, which can obtain the powder with a precise ratio between each component. The process utilizes an innovative technique called ORR, whereby the powder is uniformly mixed through stirring and intermixing, leading to the formation of a continuously movable, self-generated heat source. Upon cooling and solidification, this results in a multi-component liquid metal that forms a gradient material, embodying the distinct characteristics of each constituent material. However, other metal AM technologies rely on external heat sources to melt metal powders, which can result in poor inter-powder contact, necessitating additional powder transfer devices. Such requirements not only increase manufacturing costs but also complicate the overall process. The SPEDT approach, in contrast, is independent of external heat sources and metal powders. It utilizes dispersed metal powders, which are processed into a tightly bonded block structure. The 3DPS generated through resistive filament excitation in conjunction with ORR facilitates the creation of liquid metal, enabling the manufacturing of geometric patterns as per on-demand designs. Traditional 3D printing methods are hindered by various limitations, including the necessity for pre-made powders, supplementary powder delivery devices, and considerations related to powder melting. The SPEDT method circumvents these challenges, allowing for the simultaneous printing of dozens to hundreds of multi-component gradient materials with varying compositions. This capability significantly reduces the research and development cycle and associated costs, thereby offering valuable insights for the design of alloy compositions prepared through additive manufacturing.\u003c/p\u003e \u003cp\u003eOur research fundamentally redefines the design principles associated with traditional materials. First and foremost, the on-demand design of metal particles is achieved through 3DPS that facilitate high throughput and material library prefabrication. This approach offers several advantages, including a streamlined process, a high degree of design freedom, and the ability to create materials with gradient continuity. Consequently, it reshapes conventional design thinking and manufacturing methodologies. This innovation signifies not only disruptive advancements in processes and equipment but also a systematic overhaul of the entire workflow\u0026mdash;from design and production to service. Moreover, SPEDT developed in conjunction with 3DPS leverages the benefits of self-propagating synthesis, enabling the synchronous or sequential printing of multi-component gradient materials. SPEDT is characterized by its high adaptability in front-end consumables design and new materials development, allowing for better control over the composition and structural regulation of novel materials. In this way, the preparation processes are significantly enhanced and material costs are reduced, thereby providing a groundbreaking solution for the design and development of new materials. SPEDT also addresses the limitations and complexities associated with traditional AM by enabling the precise proportioning of high-density metals, metal oxides, and multi-metal alloys. This capability compensates for the constraints of traditional single-material printing and offers unique advantages, particularly in the fabrication of gradient functional structures.\u003c/p\u003e \u003cp\u003eLooking ahead, our research will concentrate on the systematic design of 3DPS through the application of material genetic engineering technology. We aim to develop micrometer-scale gradient materials with high efficacy, establish reliable databases through high-throughput experimental methods, and utilize first principles alongside artificial intelligence to guide the design and synthesis strategies for new materials. These efforts are expected to significantly shorten the development cycles of new materials while reducing associated research costs, ultimately accelerating the emergence of innovative materials needed for societal advancement. These materials are poised to find widespread application across various fields.\u003c/p\u003e"},{"header":"Materials and Methods","content":"\u003cp\u003e\u003cstrong\u003ePVB ethanol solution preparation:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e1.0 g of PVB was placed in a beaker, 200 mL of anhydrous ethanol was added, and a homogeneous ethanol solution of PVB was obtained after sealing and resting for 24 hours.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eModified lamellar CuO:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eTransfer 15g of flaky CuO with a particle size of 1mm to a beaker, add 0.015g of citric acid, and mix well, then add 100mL of deionized water, place in an ultrasonic apparatus, and ultrasonic dispersed for 30 min, rest for 1 hour when the supernatant was poured off, rinsed with deionized water for 2 times to remove excess citric acid, and placed in a vacuum drying oven and dried at 80 \u0026deg;C.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTrimming Spherical Al:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e4g of spherical Al with a particle size of 10~100\u0026mu;m was placed in a beaker, 0.04g of CTAB (cetyltrimethylammonium bromide) powder was added and stirred homogeneously, 50mL of anhydrous ethanol was added and ultrasonically dispersed for 30 minutes, and then the supernatant was poured off after 1 hour of rest, and the excess CTAB was removed by rinsing with anhydrous ethanol for 2 times, and was dried in a vacuum oven at 80\u0026deg;C. The sample was then dried in a vacuum drying oven.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePreparation of 3D Printing SuppliesPreparation of A:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eWeigh 15g of modified flake CuO and 4g of modified alumina in a beaker, mix well and add 80mL of isopropanol, ultrasonic dispersion for 10 minutes and then add PVB ethanol solution 0.5mL drop by drop, continue to ultrasonic for 20 minutes, and then pour off the supernatant after resting for 1 hour and then put it in a vacuum drying oven to vacuum-dry at 80\u0026deg;C to get the bonded aluminum thermite.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePreparation of B:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe prepared A was weighed 19.0 g, and 0.3 g of 100 \u0026mu;m B powder, 0.2 g of CaCO3, 0.2 g of CaO, and 1.0 g of Ni-Cr alloy were added, and placed in a mixing tube for 5 min to obtain B after mechanical mixing.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePreparation of C:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe ceramic abrasive was placed on a 304 stainless steel tape fitted with a temperature-controlled Cu mesh with wires, and B was transferred to the homemade ceramic abrasive, which was molded by adding 5 mL of PVB ethanol solution and then left to stand for 1 minute, and then the block C was obtained by standing and drying at room temperature.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTest Analysis of A, B and C:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe surface microstructure and elemental distribution of A, B and C were characterized by scanning electron microscopy (SEM) and energy spectrometry (EDS). The physical phase and crystal surface of A were characterized by an X-ray diffractometer (XRD). The valence changes of the elements in A were qualitatively analyzed by X-ray photoelectron spectroscopy (XPS) and surface charge correction was performed with 284.8 eV. The molecular functional group composition and structure in A were analyzed using Fourier transform infrared spectroscopy (FT-IR). The composition and crystal structure of A were qualitatively analyzed using Raman spectroscopy (Raman). Thermogravimetry (TG) and differential scanning calorimetry (DSC) were used to characterize the thermal stability of A, B and C. Based on this, the specific heat capacity calculation was carried out, which was used to study the combustion performance of A.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eThe preparation process of 3D Printed Super Alloys\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e1. Modeling\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eModeling is the process of creating a digital model of an object. This process can be accomplished through computer-aided design (CAD) software. In CAD software, users can create a digital model of an object and edit and modify it. The digital model can be of any shape and size, from simple geometric shapes to complex organic shapes.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003cstrong\u003e、\u003c/strong\u003e\u003cstrong\u003eSlicing\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eSlicing is the process of breaking down a digital model into a series of thin layers. This process can be accomplished through slicing software. In slicing software, the user can set the thickness of each layer and other parameters. The slicing software breaks down the digital model into a series of thin layers and transforms each layer into a set of instructions that will be used to control the printing process of the 3D printer.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3. Printing\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003ePrinting is the process of transforming a digital model into a solid object. This process can be accomplished with a 3D printer. In a 3D printer, the print material is heated to the melting point and sprayed through a nozzle. The nozzle moves along the path of each layer and builds up the print material layer by layer until the entire object is created.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAnalytical Test Methods for Super Alloys\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eMetallographic test solution was used to etch the ground and polished samples to show the morphology of the heat-affected zone, which facilitates the analysis of the cross-sectional morphology and microstructure of the metal deposited. A super depth-of-field three-dimensional microscope (VHX-5000) was used to observe the changes in the overall macroscopic morphology of the MD; the types and compositions of the interfacial elements were analyzed using a scanning electron microscope (SEM, Zeiss Supra55 VP) and an energy spectrometer (EDS, Bruker X-Flash SDD 5010), and the quantitative analysis of the elements was performed at the interfacial bonding, which facilitated the analysis of the temperature effect on element diffusion; and the composition of the physical phase on the fracture surface of the joints was analyzed by x-ray diffractometer (XRD).\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eData availability\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe datasets generated and/or analysed during the current study are available from the corresponding author on reasonable request.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor Contribution\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eYan Zhang contributed to the conception of the study; GuangZhen Ren performed the experiment; YuQiang Liu contributed significantly to analysis and manuscript preparation; Chen Yu helped perform the analysis with constructive discussions.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis research was mainly supported by Project funded by China Postdoctoral Science Foundation(2019M663861). This project is supported by the National Natural Science Foundation of China (Grant No.5210040951).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAdditional information\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting interests\u003c/strong\u003e The authors declare no competing interests.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n \u003cli\u003e\u003cspan\u003eZeng M, Du Y, Jiang Q et al (2023) High-throughput printing of combinatorial materials from aerosols[J]. Nature. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003e10.1038/s41586-023-05898-9\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eGreen ML, Takeuchi I, Hattrick-Simpers JR (2013) Applications of high throughput (combinatorial) methodologies to electronic, magnetic, optical, and energy-related materials[J]. J Appl Phys, 113(23)\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eChen X, Liu X, Ouyang M et al Multi-metal 4D printing with a desktop electrochemical 3D printer.[J].Scientific Reports, 2019(1)\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eReiser A,Lind\u0026eacute;n, Rohner M (2019) P, Multi-metal electrohydrodynamic redox 3D printing at the submicron scale[J]. Nat Commun, 10(1)\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eQueralt\u0026oacute; A et al (2021) Combinatorial screening of cuprate superconductors by drop-on-demand inkjet printing. ACS Appl Mater Interfaces 13(7):9101\u0026ndash;9112\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eAlqutaibi AY, Alghauli MA, Aljohani MHA et al (2024) Advanced additive manufacturing in implant dentistry: 3D printing technologies, printable materials, current applications and future requirements[J]. Bioprinting, : e00356\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eWang Y, Wu T, Huang G (2024) State-of-the-art research progress and challenge of the printing techniques, potential applications for advanced ceramic materials 3D printing[J]. Mater Today Commun, : 110001\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eJin H, Yang Z, Zhong J et al (2019) Mechanical and dielectric properties of 3D printed highly porous ceramics fabricated via stable and durable gel ink[J]. J Eur Ceram Soc 39(15):4680\u0026ndash;4687\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eKernan BD, Sachs EM, Oliveira MA et al (2007) Three-dimensional printing of tungsten carbide\u0026ndash;10 wt% cobalt using a cobalt oxide precursor[J]. Int J Refract Met Hard Mater 25(1):82\u0026ndash;94\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eBauer J, Crook C, Baldacchini T (2023) A sinterless, low-temperature route to 3D print nanoscale optical-grade glass[J]. Science 380(6648):960\u0026ndash;966\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eZhang D, Liu X, Qiu J (2021) 3D printing of glass by additive manufacturing techniques: a review[J]. Front Optoelectron 14:263\u0026ndash;277\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003ePal AK, Mohanty AK, Misra M (2021) Additive manufacturing technology of polymeric materials for customized products: recent developments and future prospective[J]. RSC Adv 11(58):36398\u0026ndash;36438\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eDul S, Fambri L, Pegoretti A (2016) Fused deposition modelling with ABS\u0026ndash;graphene nanocomposites [J]. Compos Part A: Appl Sci Manufac 85:181\u0026ndash;191\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eAkhoundi B, Sousani F (2024) An experimental investigation of screw-based material extrusion 3D printing of metallic parts[J]. J Eng Res 12(2):226\u0026ndash;232\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eDul S, Perret E, Hufenus R (2024) Bicomponent melt-spinning of filaments for material extrusion 3D printing[J]. Additive Manuf 85:104165\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eDul S, Fambri L, Pegoretti A (2021) High-performance polyamide/carbon fiber composites for fused filament fabrication: mechanical and functional performances[J]. J Mater Eng Perform 30:5066\u0026ndash;5085\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eGrossin DA, Mont\u0026oacute;n, Navarrete-Segado P et al (2021) A review of additive manufacturing of ceramics by powder bed selective laser processing (sintering/melting): Calcium Phosphate, Silicon Carbide, Zirconia, Alumina, and their composites[J]. Open Ceramics\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eAng X, Tey JY, Yeo WH et al (2023) A review on metallic and ceramic material extrusion method: Materials, rheology, and printing parameters[J]. J Manuf Process 90:28\u0026ndash;42\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eIgnatyev IA, Thielemans W, Vander Beke B (2014) Recycling of polymers: a review[J]. Chemsuschem 7(6):1579\u0026ndash;1593\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSingh N, Hui D, Singh R et al (2017) Recycling of plastic solid waste: A state of art review and future applications[J]. Compos Part B: Eng 115:409\u0026ndash;422\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eYang Y, Boom R, Irion B et al (2012) Recycling of composite materials[J]. Chem Eng Process 51:53\u0026ndash;68\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eTaneepanichskul N, Purkiss D, Miodownik M (2022) A review of sorting and separating technologies suitable for compostable and biodegradable plastic packaging[J]. Front Sustain 3:901885\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eOlakanmi EO, Cochrane RF, Dalgarno KW (2015) A review on selective laser sintering/melting (SLS/SLM) of aluminium alloy powders: Processing, microstructure, and properties[J]. Prog Mater Sci 74:401\u0026ndash;477\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eJakus AE, Taylor SL, Geisendorfer NR et al (2015) Metallic architectures from 3D-printed powder‐based liquid inks[J]. Adv Funct Mater 25(45):6985\u0026ndash;6995\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eWilliams CB, Cochran JK, Rosen DW (2011) Additive manufacturing of metallic cellular materials via three-dimensional printing[J]. Int J Adv Manuf Technol 53:231\u0026ndash;239\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSakib-Uz-Zaman C, Khondoker MAH (2023) A Review on Extrusion Additive Manufacturing of Pure Copper[J]. Metals 13(5):859\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eLi J, Huang Z, He B et al (2024) Experimental investigation of material extrusion additive manufacturing of copper with high powder loading rate[J]. J Mater Res Technol 33:2568\u0026ndash;2579\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eGuschlbauer R, Burkhardt AK, Fu Z et al (2020) Effect of the oxygen content of pure copper powder on selective electron beam melting[J]. Mater Sci Engineering: A 779:139106\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSantos C, Gat\u0026otilde;es D, Cerejo F et al (2021) Influence of metallic powder characteristics on extruded feedstock performance for indirect additive manufacturing[J]. Materials 14(23):7136\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eLee K, Kim D, Shim J et al (2015) Formation of Cu layer on Al nanoparticles during thermite reaction in Al/CuO nanoparticle composites: Investigation of off-stoichiometry ratio of Al and CuO nanoparticles for maximum pressure change[J]. Combust Flame 162(10):3823\u0026ndash;3828\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSong P, Wen D, Guo ZX et al (2008) Oxidation investigation of nickel nanoparticles[J]. Phys Chem Chem Phys 10(33):5057\u0026ndash;5065\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eZhang X, Guo N, Xu C et al (2019) Influence of CaF2 on microstructural characteristics and mechanical properties of 304 stainless steel underwater wet welding using flux-cored wire[J]. J Manuf Process 45:138\u0026ndash;146\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSuga Y, Hasui A (1986) on The Formation of Porosity in Underwater Weld Metal (The 1st Report), Effect of Water Pressure on Formation of Porosity: IIW Doc[R]. IX-1388-86, American Council, AWS, Miami, FI\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eDeng S, Jiang Y, Huang S et al (2018) Tuning the morphological, ignition and combustion properties of micron-Al/CuO thermites through different synthesis approaches[J]. Combust Flame 195:303\u0026ndash;310\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eWan C, Xiong Y, Qin H et al (2024) Precisely regulating combustion and ectrostatic discharge safety properties of Al/CuO nanothermite by inserting g-C3N4 nanosheet[J]. Appl Surf Sci 661:160044\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eLi C, Du J, Gao Y et al (2022) Stereolithography of 3D sustainable metal electrodes towards high-performance nickel iron battery[J]. Adv Funct Mater 32(40):2205317\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eShahzadi L, Maya F, Breadmore MC et al (2022) Functional materials for DLP-SLA 3D printing using thiol\u0026ndash;acrylate chemistry: Resin design and postprint applications[J]. ACS Appl Polym Mater 4(5):3896\u0026ndash;3907\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eXu X, Goyanes A, Trenfield SJ et al (2021) Stereolithography (SLA) 3D printing of a bladder device for intravesical drug delivery[J]. Mater Sci Engineering: C 120:111773\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSun X, Chen S, Qu B et al (2023) Light-oriented 3D printing of liquid crystal/photocurable resins and in-situ enhancement of mechanical performance[J]. Nat Commun 14(1):6586\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eAwad A, Fina F, Goyanes A et al (2021) Advances in powder bed fusion 3D printing in drug delivery and healthcare[J]. Adv Drug Deliv Rev 174:406\u0026ndash;424\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eSvetlizky D, Das M, Zheng B et al (2021) Directed energy deposition (DED) additive manufacturing: Physical characteristics, defects, challenges and applications[J]. Mater Today 49:271\u0026ndash;295\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eJoralmon D, Tang T, Prakash SR et al (2024) Continuous 3D printing of metal structures using ultrafast mask video projection initiated vat photopolymerization[J]. Additive Manuf 89:104314\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eLi N, Huang S, Zhang G et al (2019) Progress in additive manufacturing on new materials: A review[J]. J Mater Sci Technol 35(2):242\u0026ndash;269\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eLiu L et al (2024) Additive manufacturing of multi-materials with interfacial component gradient by in-situ powder mixing and laser powder bed fusion. J Alloys Compd 978:173508\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eLiu C et al (2022) Dynamic recrystallization behavior under steady and transient mutation deformation state. Mater Sci Engineering: A\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eZhu C et al (2024) Toward Multiscale, Multimaterial 3D Printing. Adv Mater : 2314204\u003c/span\u003e\u003c/li\u003e\n \u003cli\u003e\u003cspan\u003eZhou Y, Saitou K (2018) Gradient-based multi-component topology optimization for manufacturability [J].Structural and Multidisciplinary Optimization.\u003c/span\u003e\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-6071151/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6071151/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe development of new materials is of great significance for scientific and technological innovation and is essential in addressing significant societal challenges (1). Combinatorial material deposition techniques facilitate the understanding of composition-structure-property relationships and permit the rapid screening of materials across diverse compositional ranges (2). However, there are considerable challenges associated with the universal integration of multiple materials and the creation of gradient material libraries due to the lack of efficient mixing mechanisms and the difficulty in achieving precise and rapid dispensing (3-5). In this study, we introduce a novel printing approach for multicomponent gradient materials, which amalgamates various constituent materials for the three-dimensional printing of multiscale and high-throughput multigradient materials. This innovation overcomes the limitations of prolonged cycle times, high experimental costs, and low efficiency inherent in traditional manufacturing methods. First, we developed 3D-printed precursor materials that can be shaped arbitrarily. By meticulously proportioning the components of these precursor materials through high-throughput techniques and material libraries, we enable multi-degree-of-freedom adjustments in ratios and on-demand combinations, resulting in the fabrication of complex materials not achievable through conventional manufacturing processes. Subsequently, we established a highly adaptable self-propagating energy deposition technology based on the precursor materials, which reduces the conventional reliance on specific equipment and processes. Finally, we demonstrated the application of this technology through a printing strategy for various copper-based composites and multicomponent gradient materials, which allows for the simultaneous incorporation of an array of metallic and non-metallic compounds with graded properties across multiple compositions and structures. This advancement significantly enhances the scope of additive manufacturing applications in composition optimization, functional grading, and structural tuning, surpassing the capabilities of traditional printing methods. Our ability to synchronize the printing of multilayer gradient materials during the process, while mitigating thermal accumulation and structural defects such as cracks through thermal stacking between gradients, represents a marked improvement over traditional hot-cold stacking methods. Furthermore, we transitioned from the conventional outside-in model of additive manufacturing—where methods and equipment dictate the consumables—to a novel inside-out model, whereby consumables inform the methodology and equipment. Such a paradigm shift will facilitate the development of new functionally graded materials with unique compositions and structural arrangements unattainable through established manufacturing techniques.\u003c/p\u003e","manuscriptTitle":"High-throughput printing of functionally gradient material from self-propagation","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-03-07 09:27:06","doi":"10.21203/rs.3.rs-6071151/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"91292724-43c8-465e-bf07-ab89ceadf811","owner":[],"postedDate":"March 7th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":45315296,"name":"Physical sciences/Materials science/Techniques and instrumentation/Design, synthesis and processing"},{"id":45315297,"name":"Physical sciences/Materials science/Structural materials/Metals and alloys"}],"tags":[],"updatedAt":"2025-11-04T08:07:32+00:00","versionOfRecord":{"articleIdentity":"rs-6071151","link":"https://doi.org/10.1038/s41467-025-65189-x","journal":{"identity":"nature-communications","isVorOnly":false,"title":"Nature Communications"},"publishedOn":"2025-11-03 05:00:00","publishedOnDateReadable":"November 3rd, 2025"},"versionCreatedAt":"2025-03-07 09:27:06","video":"","vorDoi":"10.1038/s41467-025-65189-x","vorDoiUrl":"https://doi.org/10.1038/s41467-025-65189-x","workflowStages":[]},"version":"v1","identity":"rs-6071151","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6071151","identity":"rs-6071151","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}