Nano‑Ni-Based Multi-Channel Recyclable Thermal Interface Material with Dual-Mode Interface Adaptability

Nano‑Ni-Based Multi-Channel Recyclable Thermal Interface Material with Dual-Mode Interface Adaptability | 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 Research Article Nano‑Ni-Based Multi-Channel Recyclable Thermal Interface Material with Dual-Mode Interface Adaptability Xinbei Zhu, Yuan Liu, Jingkai Liu, Xiaoqin Feng, Ziyu Liu, Xiaoqing Liu This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9241480/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 7 You are reading this latest preprint version Abstract The rapid miniaturization and integration of electronic devices demand highly efficient thermal management while concurrently exacerbating the global electronic waste (e-waste) crisis. Although thermal interface materials (TIMs) are important for heat dissipation, their end-of-life recycling remains a formidable challenge due to stable polymers usually serve as an essential component. Herein, we develop a polymer-grafted Nickel nanoparticles as thermal interface paste (DAMF-Ni) that features dual-mode interface conformability and multi-pathway recyclability. By integrating phase-change polymer segments onto the surface of nickel nanoparticles via reversible covalent bonds, DAMF-Ni achieves enhanced interfacial adaptability through melt infiltration and magnetic-induced attachment, while enabling both chemical and physical recycling via dynamic reactions and magnetic force. Consequently, the material exhibits a remarkably low thermal contact resistance of 0.61 cm² K W⁻¹, enabling a maximum temperature reduction of 27.3°C at the device interface. Also, its core-shell polymer brush structure allows for upcycling into nanofluids and phase-change composites after end-of-life, demonstrating attractive potential in liquid cooling and thermal storage applications. This work not only broadens the design paradigm of TIMs with interface adaptability but also establishes a sustainable paradigm for mitigating e-waste in thermal management systems. Nanocomposite Thermal interface material Recycling and upcycling Phase change materials Interface conformability Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Introduction Driven by the rapid miniaturization and integration of electronic devices, soaring power densities lead to substantial internal heat accumulation, which severely compromises device performance, reliability, and service lifespan [ 1 – 3 ]. The principal bottleneck in heat dissipation is the ubiquitous solid-solid interface, where microscale air gaps act as thermal insulators. Thermal interface materials (TIMs) are therefore indispensable, serving as “thermal bridges” that fill these gaps to establish an efficient heat flow path between heat-generating components and heat sinks [ 4 ]. However, the surge in electronic device usage has also exacerbated the global electronic waste (e-waste) crisis. Conventional TIMs, typically involving the use of polymer matrix/adhesive filled with thermally conductive particles, are designed for stability, not for disposal. This phenomenon makes them difficult to be recycled at end-of-life and creating a pressing need for sustainable TIM solutions. According to market outlook, the global market for TIMs has exceeded US $ 3 billion and is growing at an annual growth rate of more than 10%[ 5 ]. Meanwhile, the increasing e-waste with an estimated growth rate of 3–5% annually is generated and discarded globally [ 6 , 7 ], highlighting the urgent demand for recyclable TIMs at the same time [ 8 ]. Most recycling strategies for polymeric materials focus on constructing dynamic covalent networks [ 9 – 11 ] or reversible supramolecular interactions (e.g., hydrogen or ionic bonds) [ 12 , 13 ] to enable thermal reshaping or chemical depolymerization. While these approaches have been successfully applied to create self-healing or reprocessable TIMs [ 12 , 14 ], they are inherently limited. They primarily aim to extend the service life of the material in situ or recover its raw chemical components. However, polymer-containing TIMs often suffer from performance degradation during reuse, which constitutes downcycling, and the destructive disassembly caused by cohesive failure tends to incur additional losses [ 15 ]. Critically, reports on the upcycling of spent TIMs into higher-value applications are scarce. This suggests that the recycling efficiency of TIMs is far from optimal and holds great potential for further enhancement. Alongside the end-of-life issue, optimal interface adaptability of a TIM to alleviate mismatch and scattering at the interface presents another formidable challenge [ 16 ]. In this context, extensive research has focused on improving the intrinsic thermal conductivity of the materials. The combination of different nanomaterials, such as “1D + 2D”, can construct heterostructured structures with unexpected enhancement [ 17 ]. Moreover, external field-induced orientation enables increased directional thermal conductivity, including vertically aligned boron nitride[ 18 ], magnetically oriented graphite[ 19 ], and directionally arranged two-dimensional nanosheets[ 20 ]. However, high filler loading and high orientation often contradict low modulus, posing an additional challenge to the critical function of TIMs in achieving flawless interfacial contact[ 21 ]. The common forms of TIMs also have their own limitations in this regard, including thermally conductive pads[ 22 ], grease[ 23 ], adhesives[ 24 ], and phase change materials (PCMs)[ 25 , 26 ]. For examples, thermally conductive pads suffer from high contact resistance due to their rigidity [ 27 ]; thermal greases, despite high conductivity, are prone to pump-out and dry-out, leading to long-term reliability issues [ 28 ]. and while phase change materials (PCMs) offer improved conformability, their low intrinsic thermal conductivity often necessitates a compromise [ 29 ]. Although multilevel structures represented by using liquid metals can effectively fill gaps, they simultaneously introduce more interfaces or increase the risk of pump-out [ 30 ]. A more elegant solution lies in chemically modifying inorganic nanoparticles with phase-change materials, a strategy that synergistically combines the high thermal conductivity of the former with the superior surface-wetting capability of the latter during melting [ 31 ]. This wetting contact is expected to be further enhanced when the inner nanoparticles are capable of responding to an external field. Herein, we propose a strategy to address both the conformability and sustainability challenges simultaneously by introducing a chemically modified nickel nanoparticle TIM (DAMF-Ni). It involves grafting phase-change polymer segments onto polydopamine-coated nickel nanoparticles via reversible Diels-Alder bonds. This design yields a material with dual-mode interfacial adaptability through melt infiltration due to the phase-change shell and magnetic field-induced attachment due to the soft-magnetic properties of the nickel core. The resulting DAMF-Ni exhibits a 377.3% enhancement in thermal conductivity over the base PCM polymer (1.327 W m⁻¹ K⁻¹) and an low thermal contact resistance of 0.61 cm² K W⁻¹, enabling a maximum device temperature reduction of 27.3°C. Crucially, the reversible chemistry and magnetic functionality unlock three distinct recycling pathways: direct magnetic recovery for reuse and chemical recycling of its high-value components (nano-Ni and PCM polymer). Most significantly, the unique core-shell polymer brush structure also enables upcycling into functional nanofluids for rapid liquid cooling or enhanced phase-change composites for high-efficiency thermal storage. This work not only presents a high-performance TIM but also establishes a sustainable, circular-economy paradigm for thermal management in the electronics industry. Result and discussion 2.1 Design and Preparation of the DAMF-Ni Given the demand for TIMs with multi-channel recyclability and excellent surface adaptability, we engineered a magnetically responsive, phase-changeable nanocomposite, termed DAMF-Ni. Figure 1 a schematically illustrates the stepwise preparation process. Specifically, nickel nanoparticles (nano-Ni) were selected as the functional core due to their soft-magnetic properties, which not only benefits magnetic field-assisted interfacial adhesion to avoid high assembly pressures, but also provides a mechanism for direct magnetic recovery to achieve non-destructive disassembly [ 32 – 34 ]. Subsequently, the surface of the nano-Ni was coated with a polydopamine (PDA) layer. This mussel-inspired coating was chosen for its exceptional adhesion to diverse substrates and its ability to introduce a rich set of functional groups onto the nanoparticle surface, creating a versatile platform for subsequent chemical modification [ 35 , 36 ]. As shown in the detailed chemical reaction equations, after coating nano-Ni with PDA (P-Ni), furan groups were further introduced via a thiol-ene reaction to obtain furan-functionalized nano-Ni (f-Ni, Fig. S1 ). Eventually, the phase-change capability was imparted through a Diels-Alder (D-A) cycloaddition between the furan groups on f-Ni and maleimide-terminated polyethylene glycol (MIPEG). Notably, chemical modification of thermally conductive nanoparticles with phase-change chains can preserve the thermal conductivity of the inner organic materials to some extent, and achieve phase transition infiltrated interface adaption simultaneously to fill the microgrooves [ 37 – 39 ]. The designed DAMF-Ni has advantages in both interfacial heat transfer and multiple recycling methods, and is well suited to meet the demands of future TIMs. As shown in Fig. 1 b, the DAMF-Ni cast at the interface may exhibit poor initial contact due to its solid state, which leads to abundant tiny air gaps, and such gaps will inevitably result in significant heat accumulation at the interface. As the operating temperature of an electronic device rises and approaches the phase-change temperature of the grafted PEG segments on DAMF-Ni (~ 43°C), the modulus of the material drops sharply, transitioning it into a viscous fluid. This solid-liquid transition dramatically enhances its shape adaptability, allowing it to flow and infiltrate interfacial microgrooves. Concurrently, the soft-magnetic nature of the Ni cores enables a dual role under the magnetic field. At the macroscopic level, the magnetized material is magnetically attracted toward a substrate, improving overall contact. At the microscopic level, dipole-dipole interactions between adjacent nanoparticles drive their rearrangement into aligned structures that more effectively penetrate and fill surface asperities. This synergy between thermal and magnetic actuation constitutes the material's dual-mode interfacial conformability. A highlight of this work lies in the consideration of the material’s recycling and high-value reuse. As displayed in Fig. 1 c, DAMF-Ni is designed for multiple end-of-life pathways, including direct recycling, chemical recycling, and upcycling. By definition, direct recycling refers to magnetic recovery, which utilizes a magnetic field to disassemble DAMF-Ni TIM from the interface without destroy the device. Chemical recycling enables the recovery of valuable chemical reagents such as MIPEG via the reverse D-A reaction. Meanwhile, the raw nano-Ni can be converted back from the synchronously obtained f-Ni via acid treatment, with the surface organic modification layer removed. More interestingly, the unique core-shell structure of DAMF-Ni allows it to be repurposed as a functional additive. It disperses uniformly in ethylene glycol to create a high-performance nanofluid for liquid cooling systems, or in PEG 6000 to form an advanced phase-change fluid with enhanced photothermal conversion for solar-thermal energy storage. This approach transforms end-of-life TIMs from waste into valuable resources for entirely new applications. The interfacial adaptability and sustainability of DAMF-Ni position it as a promising candidate to meet the demands of next-generation thermal interface materials. 2.2 Morphological and structural characterization of DAMF-Ni In order to demonstrate the successful modification of the nano-Ni, the surface morphologies of nano-Ni, f-Ni, and DAMF-Ni were first observed via scanning electron microscopy (SEM). Figure 2 a reveals the microcosmic appearance of the pristine nano-Ni, which presented relatively smooth spheres with diameters predominantly ranging from 50 to 250 nm and an average size of ~ 163 nm. Following PDA coating and furan functionalization (f-Ni), a distinct core-shell structure became apparent (Fig. 2 b). The average particle diameter increased to ~ 376 nm, with the organic shell clearly visible in high-resolution SEM imaging, exhibiting a thickness of approximately 40 nm (Fig. S2). Upon grafting MIPEG via the D-A reaction, the resulting DAMF-Ni transformed from discrete nanoparticles into an interconnected agglomerate (Fig. 2 c). This clustered structure is highly advantageous for a TIM, as the interconnected structure optimizes the particle-particle interfaces and reduces the overall interfacial thermal resistance within the material. Subsequently, the chemical structures of f-Ni, MIPEG, and DAMF-Ni were analyzed using a Fourier Transform Infrared (FT-IR, Fig. 2 d) spectrometer, and it can be seen that a distinctive new peak appears at 1772 cm⁻¹ in the FTIR spectrum of DAMF-Ni, implying the formation of the succinimide ring formed by the D-A cycloaddition between furan and maleimide [ 40 ]. Meanwhile, the disappearance of the characteristic absorption peaks of maleimide at ~ 696 cm⁻¹ and furan moieties at ~ 747 cm⁻¹ confirmed the consumption of the reactive functional groups during the grafting process [ 11 , 41 ]. To further confirm the chemical structures of the DAMF-Ni and f-Ni, X-ray photoelectron spectroscopy (XPS) was employed to investigate the specific chemical states and verify the occurrence of the D-A reaction. The wide-scan spectrum is displayed in Fig. S3, In the high-resolution C 1s spectrum, the main C = C sp² and C-C sp³ peaks are located at ~ 284.6 eV and ~ 285.2 eV, and the peaks corresponding to C-S, C-O, C = O, and C-O-C are observed at ~ 283.2 eV, ~ 286.2 eV, ~ 287.7 eV, and ~ 290.7 eV, respectively (Fig. 2 e) [ 42 – 44 ]. The O 1s spectrum (Fig. S4) was particularly informative, revealing a dominant peak at ~ 589.7 eV assigned to Ni-O bonds between nano-Ni and the PDA layer, which confirms the chemical anchoring of the PDA coating layer to the nickel surface. Peaks corresponding to C = O (~ 531.3 eV) and O-H (~ 528.2 eV) from PDA were also evident [ 45 ]. X-ray diffraction (XRD) analysis confirmed the crystal structure of the involved materials. The introduce of the long PEG segments resulted in two new peaks which locate at 19.3° and 23.5°, corresponding to the (120) and (112) crystal planes. This confirms that the MIPEG segments were successfully attached and retain their phase-change ability [ 46 ]. Notably, all samples display the characteristic (111), (200), and (220) reflections of metallic Ni at ~ 44.5°, 51.9°, and 76.4°, respectively (Fig. 2 f) [ 47 ]. The phase transition behaviors of these two samples were further investigated via differential scanning calorimetry (DSC). As shown in Fig. 2 g, both MIPEG and DAMF-Ni present distinct melting and crystallization peaks. Specifically, the melting temperatures and enthalpy of DAMF-Ni are 53.0°C and 80.8 J·g⁻¹, respectively, which are lower than those of MIPEG (57.5°C and 155.5 J·g⁻¹). Obviously, covalent grafting and confinement effects also led to a decrease in the macroscopic phase-change performance of the PEG segment on DAMF-Ni compared to that of pure MIPEG, which is also reflected in XRD results. However, this is an also direct consequence of the high mass fraction of the non-melting Ni core (as determined by thermogravimetric analysis, Fig. S5). The rheological properties of DAMF-Ni are critical for its processability and phase-change conformability. The viscosity-temperature curve showed a sharp decrease in viscosity beginning at ~ 43°C, closely matching the onset of the PEG melting transition observed by DSC, as displayed in Fig. 2 h. This confirms the solid-to-liquid transition that underpins its melt-infiltration capability. At higher temperatures (> 150°C), a second, more gradual decrease in viscosity was observed, corresponding to the retro-D-A reaction, which decouples the PEG chains from the nanoparticles. In addition, vibrating sample magnetometry (VSM) confirmed that the desirable soft-magnetic properties of the nickel core are retained throughout the functionalization process (Fig. 2 i). All samples exhibited narrow hysteresis loops with low coercivity and remanence, characteristic of soft magnets [ 48 ]. As expected, the saturation magnetization (Mₛ) decreased progressively from pristine nano-Ni (57.2 emu g⁻¹) to f-Ni (38.1 emu g⁻¹) and finally to DAMF-Ni (18.5 emu g⁻¹), reflecting the increasing mass of the non-magnetic organic shell. It should be noted that the insets in Fig. 2 i demonstrate that DAMF-Ni remains strongly responsive to an external magnetic field both below and above its phase-change temperature, confirming its suitability for magnetic-assisted assembly and direct magnetic recovery. 2.3 Dual-Mode Interfacial Conformability and Thermal Transport Properties. Among the myriad performance metrics for TIMs, interfacial conformability is critical, as inadequate contact invariably leads to entrapped air pockets that act as thermal barriers and compromise device reliability [ 49 ]. To address this challenge, DAMF-Ni was engineered with a dual-mode conformability mechanism that synergistically combines phase-change-enabled infiltration with magnetic field-assisted attachment. The interfacial integration process of DAMF-Ni is illustrated in Fig. 3 a. Notably, magnetic field-assisted attachment is adopted instead of conventional compression assembly, which can be attributed to its easy magnetization characteristic. Owing to the suitable rheological properties of DAMF-Ni above its melting temperature, it can be dispensed onto the interface via a needle-tube extrusion method. As shown in Fig. 3 b, a commercial glue dispenser can be employed to achieve controllable application, highlighting its compatibility with existing manufacturing processes. Upon exposure to an external magnetic field, the embedded Ni nanoparticles become magnetized, generating dipole-dipole interactions between magnetized adjacent particles, which rearranges the alignment of magnetized nanoparticles along the direction of the magnetic field and promotes interfacial contact (Fig. 3 c inset) [ 50 , 51 ]. This field-induced reorganization was directly visualized by polarized optical microscopy (Fig. 3 c), revealing the formation of aligned chain-like structures oriented parallel to the applied field. Such alignment is expected to facilitate directional heat transport while simultaneously improving surface wetting. To quantitatively assess the conformability of DAMF-Ni, we fabricated model rough surfaces with well-defined microgrooves on silicone substrates using pulsed laser ablation. The distribution of Ni elements at the interface using Energy-dispersive X-ray spectroscopy (EDS) elemental mapping (Fig. 3 d), which confirms good adherence and distribution of Ni, which ensures homogenous thermal conduction and larger contact area of the DAMF-Ni (Fig. S6). Moreover, the SEM also provided direct evidence of the dual-mode enhancement mechanism. In the absence of magnetic field and below its phase-change temperature, DAMF-Ni exhibited poor contact with the substrate, with visible gaps persisting at the interface (Fig. 3 e). However, after heating above its melting point and applying it under magnetic field, the material flowed to achieve intimate, void-free contact (Fig. 3 f). Additionally, the contact performance of DAMF-Ni on different substrate materials were also evaluated, including metal-based copper plates, polymer films, and SiO 2 samples (Fig. S7), which underscores the versatility of DAMF-Ni for various packaging applications. The thermal contact resistance (TCR), which directly reflects interfacial heat transfer efficiency, was evaluated as a function of both temperature and pressure (Fig. 3 g and S8; see Supporting Information for calculation methodology). For samples with a thickness of ~ 1 mm, TCR exhibited a sharp decrease around 50°C, which is consistent with the onset temperature of the PEG fusion. This abrupt reduction confirms that the solid-to-liquid transformation enables the material to flow and conform to surface asperities, displacing insulating air and establishing more efficient thermal contact. Besides, above the melting point, TCR continued to decrease gradually and shows asymptotic behavior, reflecting progressive wetting and equilibration of the interface. Pressure-dependent measurements at 80°C revealed a monotonic decrease in TCR with increasing applied pressure from 10 to 60 psi, reaching a minimum value of 0.61 cm² K W⁻¹ at the highest pressure. This value compares favorably with state-of-the-art TIMs, demonstrating the effectiveness of the dual-mode conformability strategy [ 52 – 59 ]. Notably, the TCR values of DAMF‑Ni exhibit almost no change across the pressure range of 10 ~ 60 psi, indicating that DAMF‑Ni has already closely adhered to the interface under magnetic force, and further increasing the pressure has obscure influence on TCR. The inset of Fig. 3 g shows the thermal conductivity results of DAMF-Ni and MIPEG, which were tested via the laser flash technique. The thermal conductivity of MIPEG is as low as 0.278 W·m⁻¹·K⁻¹, while that of DAMF-Ni is 1.327 W·m⁻¹·K⁻¹, indicating an improvement of 377.5%. This substantial improvement is believed to result from both the intrinsically high thermal conductivity of the metallic Ni core and the formation of an interconnected particle network (evident in Fig. 2 c). 2.4 Interfacial thermal management performance of DAMF-Ni To further investigate the actual heat dissipation performance of DAMF-Ni, we constructed a model cooling system comprising an LED bead as the heat source, a heat sink, and various TIMs for comparison. Benchmark materials included a commercial thermally conductive silicone grease (Telesky, 1.93 W m⁻¹ K⁻¹) and a commercial thermal pad (Laird, 4 W m⁻¹ K⁻¹). DAMF-Ni was pre-conditioned by phase-change infiltration and magnetic-induced attachment, whereas the two reference samples were simply compressed. Figure 4 a shows the schematic diagram of the heat dissipation unit and the corresponding photographs of the assembled devices. To ensure a fair comparison, the coating thickness of DAMF-Ni and silicone grease was carefully controlled to match that of the commercial pad, eliminating thickness-induced variations in thermal resistance. Figure 4 b presents the infrared images of the hot spot at 3.5 V, as shown, the surface temperature of the raw LED rises from room temperature to 32.5°C after 10 s of operation, and further increases to 60.5°C at 60 s, which is not conducive to device lifespan and reliability. Incorporation of a TIM dramatically reduced the operating temperature, with the extent of cooling varying markedly among the tested materials. The commercial pad shows the poorest heat dissipation performance, as the LED temperature still reaches 45.6°C after 60 s of operation. This inferior performance is attributable to its limited surface conformability, which prevents intimate contact with the microscopically rough LED surface. Notably, DAMF-Ni outperformed even the high-conductivity silicone grease, demonstrating excellent cooling capability. Figure 4 c exhibits the temperature-time curve for all samples. The bare LED reached a peak temperature of 60.5°C after 60 s. The commercial pad reduced this to 45.6°C (ΔT = 14.9°C), while silicone grease achieved 34.3°C (ΔT = 26.2°C). Remarkably, DAMF-Ni lowered the LED temperature to just 33.2°C, corresponding to a maximum temperature reduction of 27.3°C relative to the bare device. This exceptional performance underscores the synergistic benefits of phase-change-enabled conformability and magnetic-induced attachment, despite its intrinsic thermal conductivity not being exceptionally high. An interesting observation also emerged in the temperature range of 40–50°C, in which a plateau appears due to the phase transition of the PEG segment. Therefore, within this temperature range, DAMF-Ni can effectively absorb the heat generated by the LED and reduce its operating temperature. Additionally, Fig. 4 d shows the cyclic stability performance, where measurements are recorded every ten cycles, and detailed cyclic performance is shown in Fig. S9. As shown, the temperature of the LED with DAMF-Ni remains highly stable within 100 switching cycles, and no discernible changes were observed, indicating its excellent long-term operational reliability in practical applications. This stability contrasts favorably with silicone grease, which is notoriously susceptible to pump-out and dry-out under cyclic thermal loading. In contrast, the covalently anchored polymer brush architecture of DAMF-Ni maintained superior stability even after long-term storage (Fig. S10). To further highlight the outstanding heat dissipation capacity, both the temperature reduction and interfacial heat flux of DAMF-Ni were compared with the commercial samples, as shown in Fig. 4 e. DAMF-Ni achieved a temperature reduction of 27.3°C and a heat flux of 18.5 kJ m⁻² s⁻¹, surpassing both the commercial pad (20.0°C, 9.7 kJ m⁻² s⁻¹) and silicone grease (26.2°C, 14.2 kJ m⁻² s⁻¹). Finally, in terms of thermal resistance (and corresponding thermal conductivity) and heat dissipation performance, DAMF-Ni also outperforms other previously reported phase-change TIMs (Fig. 4 f)[ 60 – 78 ]. The excellent interfacial thermal management performance of DAMF-Ni suggests that it holds great promise as a practical TIM. 2.5 Multiple recycling methods The rapid obsolescence of electronic devices has precipitated a continuous growth of global e-waste [ 79 ], with annual generation projected to reach 74.7 million tonnes by 2030 [ 80 , 81 ]. Extensive research has focused on recovering metallic [ 82 ], ceramic [ 83 ], or polymeric fractions from electronic waste [ 84 ]. As for TIMs, existing studies have primarily emphasized self-healing properties to extend their service life, rather than addressing post-consumer recovery [ 85 – 87 ]. Accordingly, in this work, recyclability was taken into account at the initial stage of DAMF-Ni design. In detail, DAMF-Ni can be recycled via multiple pathways, including direct magnetic recycling, reversible chemical recycling, and upcycling into functional nanofluids or phase change fluids. The soft-magnetic properties of the Ni core enable a simple recycling process by magnetic attraction (Fig. 5 a). After device disassembly, DAMF-Ni can be physically collected from the interface using a strong permanent magnet or an electromagnet, which enables reversible detachment for next use. Notably, after magnetic recovery, DAMF-Ni exhibits excellent reusability, and it can be re-melted and re-spread without any observable degradation in performance (Fig. 5 a, right panel). Moreover, the specific chemical structure of the modified layer constructed via D-A bonds enables the recycling of different chemical components. In addition to direct magnetic recovery, DAMF-Ni can also be recycled using chemical methods (Fig. 5 b). DAMF-Ni can be converted into f-Ni and MIPEG through a reversible D-A reaction, with the FT-IR spectra of MIPEG and re-MIPEG displayed in Fig. 5 b, and as shown, the FT-IR spectrum of the recycled MIPEG (re-MIPEG) is consistent with that of fresh MIPEG, indicating that the chemical recycling method can effectively recover the functional components materials of DAMF-Ni. Moreover, the organic layer on f-Ni can be further chemically removed by acid pickling to obtain recycled nano-Ni; the corresponding SEM image is shown in Fig. 5 b, which exhibits almost the same morphological characteristics as the original nano-Ni. This chemical recycling approach enables the recovery of high-value constituents for reuse in new material formulations, closing the material loop at the component level. Most innovatively, the unique core-shell structure of DAMF-Ni enables its upcycling into value-added products for entirely new applications. As expected, the hydrophilic PEG brush of DAMF-Ni endows it with excellent hydrophilicity, as its water contact angle is as low as 16.3° (Fig. S11). This merit allows it to stably disperse in hydrophilic media. Given that DAMF-Ni with good thermal conductivity, dispersing it in coolant allows nanofluid application. As a proof-of-concept, DAMF-Ni was dispersed in ethylene glycol (EG) which serve as a commonly used liquid-cooling medium to apply in liquid cooling systems. The assembly diagram of the functional nanofluid (DAMF-Ni/EG) is shown at the top of Fig. 5 c, from which it can be observed that DAMF-Ni exhibits uniform dispersion in EG at only 1 wt.% addition. In a liquid cooling demonstration, a chip heater without coolant reached a steady-state temperature exceeding 70°C. In comparison, the DAMF-Ni/EG nanofluid achieved a dramatic temperature reduction of 44°C, outperforming the pure EG with temperature reduction of 42.5°C. This upcycling pathway transforms spent TIMs into performance-enhancing additives for advanced cooling applications. Similarly, DAMF-Ni can be dispersed in PEG 6000 to create a magnetic-controllable phase-change composite with thermal storage and solar-thermal conversion capabilities. The weight ratio of DAMF-Ni to PEG 6000 was 1:9. The intrinsic dark color of DAMF-Ni, imparted by the polydopamine coating, enables efficient broadband light absorption. SEM and POM confirmed the uniform dispersion of DAMF-Ni within the PEG 6000 matrix. DSC revealed that the resulting DAMF-Ni/PEG 6000 composite exhibits a high latent heat of approximately 175 J g⁻¹ due to both components contribute to the phase-change heat storage capacity. Meanwhile, the magnetic Ni cores render the optical absorber magnetically tunable, which is a feature with potential for adaptive solar-thermal harvesting systems, as illustrated in Fig. 5 d (bottom left) [ 88 ]. Furthermore, in a model house constructed from insulating panels with the composite applied to the roof, the DAMF-Ni/PEG 6000 system effectively buffered temperature fluctuations under simulated solar illumination, demonstrating its potential for passive building temperature regulation (Fig. 5 d, bottom right). Both the functional nanofluid and phase change fluid verify the upcycling potential of DAMF-Ni, which is highly consistent with the future demands for eco-friendly TIMs. Conclusion In conclusion, we have successfully designed and synthesized a thermal interface paste, DAMF-Ni, which possesses multiple recycling routes, favorable heat dissipation performance, and dual-mode surface adaptability. By synergistically combining thermally induced phase-change infiltration with magnetic field-assisted particle rearrangement, DAMF-Ni achieves exceptional surface wetting that effectively eliminates interfacial air gaps. As a result, DAMF-Ni shows a low thermal contact resistance of 0.61 cm²·K·W⁻¹ without manual pressing. The metallic core also endows DAMF-Ni with a good thermal conductivity of 1.327 W·m⁻¹·K⁻¹, an improvement of 377.5% over the pure phase-change material MIPEG. In practical device-level validation, DAMF-Ni reduced LED operating temperature by up to 27.3°C, outperforming both commercial silicone grease and thermal pads, while maintaining excellent reliability. Benefiting from its soft-magnetic characteristics and specific chemical structure with reversible D-A bonds, DAMF-Ni possesses the capabilities of direct magnetic recycling and chemical recycling, respectively. Magnetic recycling allows for reuse without sacrificing performance, while chemical recycling recovers high-value nano-Ni and MIPEG. Most significantly, we have pioneered an upcycling paradigm: the waste DAMF-Ni can be repurposed as a functional additive in EG to create high-performance nanofluids for liquid cooling, or in PEG 6000 to formulate advanced phase-change composite. The proposed strategy demonstrates the feasibility of developing high-performance TIMs with enhanced interface adaptability and multi-channel recyclability, which can simultaneously deliver state-of-the-art thermal management and contribute to a circular economy. Declarations Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Author Contribution X. Z.: Writing–original draft, Visualization, Validation, Methodology, Data curation, Investigation. Y. L.: Writing–original draft, Writing–review & editing, Visualization, Formal analysis. J. L.: Writing–original draft, Writing–review & editing, Validation, Project administration, Methodology, Conceptualization. X. F.: Resources, Investigation. Z. L.: Methodology, Formal analysis. X. L.: Writing–review & editing, Supervision, Resources, Project administration, Funding acquisition. Acknowledgement The authors are grateful for the financial support from by National Natural Science Foundation of China (52403150), Natural Science Foundation of Guizhou (Qiankehe-ZK[2022] KEY002), Xinjiang Tianchi Talents Program-Young Doctor Project (BT-2025-TCYC-0012), Xinjiang NJ Project (Tier B Funding), Tarim University President's Fund (TDZKSS202507, TDZKBS202546), General Program of Basic Research Projects of Xinjiang Region (2025DA045), Science and Technology Tackling Program of Alar City (2025GX03). References Zhang Y, Park M, Park S-J (2019) Implication of thermally conductive nanodiamond-interspersed graphite nanoplatelet hybrids in thermoset composites with superior thermal management capability. Sci Rep 9(1). https://doi.org/10.1038/s41598-019-39127-z Li J, Fu Y, Zhou J, Yao K, Ma X, Gao S, Wang Z, Dai J-G, Lei D, Yu X Ultrathin, soft, radiative cooling interfaces for advanced thermal management in skin electronics. 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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-9241480","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":641461591,"identity":"12bb91db-81ed-4316-b17b-22ae632c3af1","order_by":0,"name":"Xinbei Zhu","email":"","orcid":"","institution":"Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences","correspondingAuthor":false,"prefix":"","firstName":"Xinbei","middleName":"","lastName":"Zhu","suffix":""},{"id":641461592,"identity":"b7b03543-56ff-448c-950d-5e8ff5d6b766","order_by":1,"name":"Yuan Liu","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA60lEQVRIiWNgGAWjYBACNvbGxgcSBhI8bOwNUKEDBLTw8Rw+bGBRYSMDZBCpRU4iLU2i4kyajZxEMpFa2BhyDCRuth3mYZN8f/BzZRuDHN+NBMbPBXi1nDEwnAnSIp3MLHm2jcFY8kYCs/QMfFoYewySJSFaGCQb2xgSN9xIYGPmwaeFmcfg8F+www4z/wRqqSeshY0tsUHiTBoPmwQzG8iWBAOCWniYDzNIVNjwsPEkm1k2nJMwnHnmYbM0Pi3y8x+2/wBGpb18+8HHNxvKbOT5jicf/IxPCzqQAGLGBhI0jIJRMApGwSjABgCSvETR6DerYgAAAABJRU5ErkJggg==","orcid":"","institution":"Tarim University","correspondingAuthor":true,"prefix":"","firstName":"Yuan","middleName":"","lastName":"Liu","suffix":""},{"id":641461595,"identity":"5e4f4fcc-e6a2-41cf-a1c6-f972f9fa18d7","order_by":2,"name":"Jingkai Liu","email":"","orcid":"","institution":"Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences","correspondingAuthor":false,"prefix":"","firstName":"Jingkai","middleName":"","lastName":"Liu","suffix":""},{"id":641461596,"identity":"ae470a3e-2e2e-43f7-8054-c9a8a4e40f6f","order_by":3,"name":"Xiaoqin Feng","email":"","orcid":"","institution":"Tarim University","correspondingAuthor":false,"prefix":"","firstName":"Xiaoqin","middleName":"","lastName":"Feng","suffix":""},{"id":641461598,"identity":"a8e6ff60-4877-4a8f-a83a-7f733dcbb41c","order_by":4,"name":"Ziyu Liu","email":"","orcid":"","institution":"Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences","correspondingAuthor":false,"prefix":"","firstName":"Ziyu","middleName":"","lastName":"Liu","suffix":""},{"id":641461599,"identity":"a88e8f70-4b10-4746-921a-83444e3b9fd6","order_by":5,"name":"Xiaoqing Liu","email":"","orcid":"","institution":"Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences","correspondingAuthor":false,"prefix":"","firstName":"Xiaoqing","middleName":"","lastName":"Liu","suffix":""}],"badges":[],"createdAt":"2026-03-27 07:25:23","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-9241480/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-9241480/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":109459926,"identity":"e4a5ea44-3a73-49af-9d8e-12c699a4c5e1","added_by":"auto","created_at":"2026-05-18 10:47:49","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":674161,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Schematic illustration for the preparation process of DAMF-Ni. (b) The dual-mode interfacial adaptability function of DAMF-Ni including phase-change infiltration and magnetic-induced attachment. (c) Three recycling methods of DAMF-Ni including direct magnetic recycling, chemical recycling, and upcycling.\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/2b12c6f898714c09f9c049cb.png"},{"id":109799537,"identity":"c0ae72b4-ebf4-47e0-b80d-8cc266e516f8","added_by":"auto","created_at":"2026-05-22 15:30:51","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":636682,"visible":true,"origin":"","legend":"\u003cp\u003eSEM images of (a) Ni nanoparticles, (b) f-Ni, and (c) DAMF-Ni. Insets show schematic illustrations of the corresponding materials and the detailed particle size distributions. (d) FT-IR spectra of f-Ni, MIPEG, and DAMF-Ni. (e) C 1s XPS spectra of f-Ni and DAMF-Ni. (f) XRD patterns of Ni, f-Ni, and DAMF-Ni. (g) DSC curves of MIPEG and DAMF-Ni. (h) Viscosity–temperature curve of DAMF-Ni. Insets illustrate the melting phase transition of DAMF-Ni at ~43 °C and the retro-Diels–Alder reaction at ~162 °C. (i) Magnetic hysteresis loops of Ni, f-Ni, and DAMF-Ni with a maximum magnetic field of 20 kOe. Insets show photographs of the magnetically controllable adhesion and recovery of DAMF-Ni before and after phase transition.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/133f4759677c0d4b5636dec1.png"},{"id":109459928,"identity":"8d354e39-bfa0-46a1-9ee1-eb51a11d69aa","added_by":"auto","created_at":"2026-05-18 10:47:49","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":926876,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Schematic illustration of the interfacial integration process of DAMF-Ni. (b) Digital image of DAMF-Ni applied using a commercial glue dispenser. (c) POM image of magnetized DAMF-Ni. Inset shows the magnetization process of DAMF-Ni. (d) Ni elemental mapping in the microgrooves. SEM images of the interfacial contact for the sample before (e) and after (f)magnetic field induction. (g) Total thermal resistance and contact thermal resistance as functions of temperature. Inset shows the thermal conductivity of MIPEG and DAMF-Ni.\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/bd66c385b6b9698e5f0c54d2.png"},{"id":109459929,"identity":"1212b60e-d995-4b82-8fef-0fd2b4715654","added_by":"auto","created_at":"2026-05-18 10:47:49","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":315249,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Schematic configuration of the hot-spot cooling system and corresponding digital photographs. (b) The heat dissipation performance of DAMF-Ni and the comparison samples. Infrared images of each group at a voltage of 3.5 V. (c) Temperature–time curves of the bare LED and the same device using a commercial phase-change pad, silicone grease, and DAMF-Ni as TIMs. (d) Cycling stability of DAMF-Ni at a voltage of 3 V. (e) Temperature reduction and interfacial heat flux results. (f) Comparison of thermal conductivity of DAMF-NI with other phase-change TIMs reported in previous studies.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/1ab0c260071f059b58ab603a.png"},{"id":109459930,"identity":"ac1eab6e-fddc-458b-93e7-a8d19f648314","added_by":"auto","created_at":"2026-05-18 10:47:49","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":721185,"visible":true,"origin":"","legend":"\u003cp\u003eMultiple recyclability of DAMF-Ni: (a) Direct magnetic recycling. The left panel shows a schematic diagram of magnetic-assisted recovery, while the right panel presents digital images of DAMF-Ni re-spreading under magnetic force after recycling. (b) Chemical recycling. The upper panel illustrates the retro-Diels–Alder reaction of DAMF-Ni; the bottom-left panel depicts a schematic diagram for the recovery of nano-Ni from f-Ni (the product of the retro-Diels–Alder reaction) via acid washing; the bottom-middle panel displays the SEM image of the recovered nano-Ni; the bottom-right panel presents the FTIR spectra of the recovered MIPEG and fresh MIPEG. (c) Upcycling of DAMF-Ni (I). The upper panel illustrates a schematic diagram for recycling DAMF-Ni into ethylene glycol to prepare nanofluids for thermal management; the lower panel shows the temperature of the heating element and those after applying pure EG and EG/DAMF-Ni suspension, respectively. (d) Upcycling of DAMF-Ni (II). The upper-left panel shows the SEM and POM images of DAMF-Ni/PEG 6000; the upper-right panel presents the DSC curves of DAMF-Ni/PEG 6000; the bottom-left panel shows a schematic diagram of DAMF-Ni/PEG 6000 applied in a thermal-insulating model house; the bottom-right panel displays the temperature–time curves for insulating plates with and without DAMF-Ni/PEG 6000.\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/2986e8fcb080738508ee47ae.png"},{"id":109911916,"identity":"09ac5002-78cf-4aac-b30c-fbe3ea5f15e3","added_by":"auto","created_at":"2026-05-25 07:25:33","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3278738,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/0be91bb2-0aab-46ce-961a-7ee1f2b8bae5.pdf"},{"id":109459925,"identity":"eae9b5f2-941c-4a30-b4f4-548580a52856","added_by":"auto","created_at":"2026-05-18 10:47:49","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":2678467,"visible":true,"origin":"","legend":"","description":"","filename":"SI20260327.docx","url":"https://assets-eu.researchsquare.com/files/rs-9241480/v1/4742d4d6ab851a6a5bff97e2.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"Nano‑Ni-Based Multi-Channel Recyclable Thermal Interface Material with Dual-Mode Interface Adaptability","fulltext":[{"header":"Introduction","content":"\u003cp\u003eDriven by the rapid miniaturization and integration of electronic devices, soaring power densities lead to substantial internal heat accumulation, which severely compromises device performance, reliability, and service lifespan [\u003cspan additionalcitationids=\"CR2\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]. The principal bottleneck in heat dissipation is the ubiquitous solid-solid interface, where microscale air gaps act as thermal insulators. Thermal interface materials (TIMs) are therefore indispensable, serving as \u0026ldquo;thermal bridges\u0026rdquo; that fill these gaps to establish an efficient heat flow path between heat-generating components and heat sinks [\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e]. However, the surge in electronic device usage has also exacerbated the global electronic waste (e-waste) crisis. Conventional TIMs, typically involving the use of polymer matrix/adhesive filled with thermally conductive particles, are designed for stability, not for disposal. This phenomenon makes them difficult to be recycled at end-of-life and creating a pressing need for sustainable TIM solutions.\u003c/p\u003e \u003cp\u003eAccording to market outlook, the global market for TIMs has exceeded US\u003cspan\u003e$\u003c/span\u003e3\u0026nbsp;billion and is growing at an annual growth rate of more than 10%[\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]. Meanwhile, the increasing e-waste with an estimated growth rate of 3\u0026ndash;5% annually is generated and discarded globally [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e], highlighting the urgent demand for recyclable TIMs at the same time [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]. Most recycling strategies for polymeric materials focus on constructing dynamic covalent networks [\u003cspan additionalcitationids=\"CR10\" citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e] or reversible supramolecular interactions (e.g., hydrogen or ionic bonds) [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e, \u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e] to enable thermal reshaping or chemical depolymerization. While these approaches have been successfully applied to create self-healing or reprocessable TIMs [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e, \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e], they are inherently limited. They primarily aim to extend the service life of the material in situ or recover its raw chemical components. However, polymer-containing TIMs often suffer from performance degradation during reuse, which constitutes downcycling, and the destructive disassembly caused by cohesive failure tends to incur additional losses [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e]. Critically, reports on the upcycling of spent TIMs into higher-value applications are scarce. This suggests that the recycling efficiency of TIMs is far from optimal and holds great potential for further enhancement.\u003c/p\u003e \u003cp\u003eAlongside the end-of-life issue, optimal interface adaptability of a TIM to alleviate mismatch and scattering at the interface presents another formidable challenge [\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]. In this context, extensive research has focused on improving the intrinsic thermal conductivity of the materials. The combination of different nanomaterials, such as \u0026ldquo;1D\u0026thinsp;+\u0026thinsp;2D\u0026rdquo;, can construct heterostructured structures with unexpected enhancement [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]. Moreover, external field-induced orientation enables increased directional thermal conductivity, including vertically aligned boron nitride[\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e], magnetically oriented graphite[\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e], and directionally arranged two-dimensional nanosheets[\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]. However, high filler loading and high orientation often contradict low modulus, posing an additional challenge to the critical function of TIMs in achieving flawless interfacial contact[\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. The common forms of TIMs also have their own limitations in this regard, including thermally conductive pads[\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e], grease[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e], adhesives[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e], and phase change materials (PCMs)[\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e, \u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]. For examples, thermally conductive pads suffer from high contact resistance due to their rigidity [\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]; thermal greases, despite high conductivity, are prone to pump-out and dry-out, leading to long-term reliability issues [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]. and while phase change materials (PCMs) offer improved conformability, their low intrinsic thermal conductivity often necessitates a compromise [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. Although multilevel structures represented by using liquid metals can effectively fill gaps, they simultaneously introduce more interfaces or increase the risk of pump-out [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. A more elegant solution lies in chemically modifying inorganic nanoparticles with phase-change materials, a strategy that synergistically combines the high thermal conductivity of the former with the superior surface-wetting capability of the latter during melting [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. This wetting contact is expected to be further enhanced when the inner nanoparticles are capable of responding to an external field.\u003c/p\u003e \u003cp\u003eHerein, we propose a strategy to address both the conformability and sustainability challenges simultaneously by introducing a chemically modified nickel nanoparticle TIM (DAMF-Ni). It involves grafting phase-change polymer segments onto polydopamine-coated nickel nanoparticles via reversible Diels-Alder bonds. This design yields a material with dual-mode interfacial adaptability through melt infiltration due to the phase-change shell and magnetic field-induced attachment due to the soft-magnetic properties of the nickel core. The resulting DAMF-Ni exhibits a 377.3% enhancement in thermal conductivity over the base PCM polymer (1.327 W m⁻\u0026sup1; K⁻\u0026sup1;) and an low thermal contact resistance of 0.61 cm\u0026sup2; K W⁻\u0026sup1;, enabling a maximum device temperature reduction of 27.3\u0026deg;C. Crucially, the reversible chemistry and magnetic functionality unlock three distinct recycling pathways: direct magnetic recovery for reuse and chemical recycling of its high-value components (nano-Ni and PCM polymer). Most significantly, the unique core-shell polymer brush structure also enables upcycling into functional nanofluids for rapid liquid cooling or enhanced phase-change composites for high-efficiency thermal storage. This work not only presents a high-performance TIM but also establishes a sustainable, circular-economy paradigm for thermal management in the electronics industry.\u003c/p\u003e"},{"header":"Result and discussion","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Design and Preparation of the DAMF-Ni\u003c/h2\u003e \u003cp\u003eGiven the demand for TIMs with multi-channel recyclability and excellent surface adaptability, we engineered a magnetically responsive, phase-changeable nanocomposite, termed DAMF-Ni. Figure\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea schematically illustrates the stepwise preparation process. Specifically, nickel nanoparticles (nano-Ni) were selected as the functional core due to their soft-magnetic properties, which not only benefits magnetic field-assisted interfacial adhesion to avoid high assembly pressures, but also provides a mechanism for direct magnetic recovery to achieve non-destructive disassembly [\u003cspan additionalcitationids=\"CR33\" citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. Subsequently, the surface of the nano-Ni was coated with a polydopamine (PDA) layer. This mussel-inspired coating was chosen for its exceptional adhesion to diverse substrates and its ability to introduce a rich set of functional groups onto the nanoparticle surface, creating a versatile platform for subsequent chemical modification [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e, \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. As shown in the detailed chemical reaction equations, after coating nano-Ni with PDA (P-Ni), furan groups were further introduced via a thiol-ene reaction to obtain furan-functionalized nano-Ni (f-Ni, Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e). Eventually, the phase-change capability was imparted through a Diels-Alder (D-A) cycloaddition between the furan groups on f-Ni and maleimide-terminated polyethylene glycol (MIPEG). Notably, chemical modification of thermally conductive nanoparticles with phase-change chains can preserve the thermal conductivity of the inner organic materials to some extent, and achieve phase transition infiltrated interface adaption simultaneously to fill the microgrooves [\u003cspan additionalcitationids=\"CR38\" citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eThe designed DAMF-Ni has advantages in both interfacial heat transfer and multiple recycling methods, and is well suited to meet the demands of future TIMs. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb, the DAMF-Ni cast at the interface may exhibit poor initial contact due to its solid state, which leads to abundant tiny air gaps, and such gaps will inevitably result in significant heat accumulation at the interface. As the operating temperature of an electronic device rises and approaches the phase-change temperature of the grafted PEG segments on DAMF-Ni (~\u0026thinsp;43\u0026deg;C), the modulus of the material drops sharply, transitioning it into a viscous fluid. This solid-liquid transition dramatically enhances its shape adaptability, allowing it to flow and infiltrate interfacial microgrooves. Concurrently, the soft-magnetic nature of the Ni cores enables a dual role under the magnetic field. At the macroscopic level, the magnetized material is magnetically attracted toward a substrate, improving overall contact. At the microscopic level, dipole-dipole interactions between adjacent nanoparticles drive their rearrangement into aligned structures that more effectively penetrate and fill surface asperities. This synergy between thermal and magnetic actuation constitutes the material's dual-mode interfacial conformability. A highlight of this work lies in the consideration of the material\u0026rsquo;s recycling and high-value reuse. As displayed in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec, DAMF-Ni is designed for multiple end-of-life pathways, including direct recycling, chemical recycling, and upcycling. By definition, direct recycling refers to magnetic recovery, which utilizes a magnetic field to disassemble DAMF-Ni TIM from the interface without destroy the device. Chemical recycling enables the recovery of valuable chemical reagents such as MIPEG via the reverse D-A reaction. Meanwhile, the raw nano-Ni can be converted back from the synchronously obtained f-Ni via acid treatment, with the surface organic modification layer removed. More interestingly, the unique core-shell structure of DAMF-Ni allows it to be repurposed as a functional additive. It disperses uniformly in ethylene glycol to create a high-performance nanofluid for liquid cooling systems, or in PEG 6000 to form an advanced phase-change fluid with enhanced photothermal conversion for solar-thermal energy storage. This approach transforms end-of-life TIMs from waste into valuable resources for entirely new applications. The interfacial adaptability and sustainability of DAMF-Ni position it as a promising candidate to meet the demands of next-generation thermal interface materials.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Morphological and structural characterization of DAMF-Ni\u003c/h2\u003e \u003cp\u003eIn order to demonstrate the successful modification of the nano-Ni, the surface morphologies of nano-Ni, f-Ni, and DAMF-Ni were first observed via scanning electron microscopy (SEM). Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea reveals the microcosmic appearance of the pristine nano-Ni, which presented relatively smooth spheres with diameters predominantly ranging from 50 to 250 nm and an average size of ~\u0026thinsp;163 nm. Following PDA coating and furan functionalization (f-Ni), a distinct core-shell structure became apparent (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb). The average particle diameter increased to ~\u0026thinsp;376 nm, with the organic shell clearly visible in high-resolution SEM imaging, exhibiting a thickness of approximately 40 nm (Fig. S2). Upon grafting MIPEG via the D-A reaction, the resulting DAMF-Ni transformed from discrete nanoparticles into an interconnected agglomerate (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec). This clustered structure is highly advantageous for a TIM, as the interconnected structure optimizes the particle-particle interfaces and reduces the overall interfacial thermal resistance within the material. Subsequently, the chemical structures of f-Ni, MIPEG, and DAMF-Ni were analyzed using a Fourier Transform Infrared (FT-IR, Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed) spectrometer, and it can be seen that a distinctive new peak appears at 1772 cm⁻\u0026sup1; in the FTIR spectrum of DAMF-Ni, implying the formation of the succinimide ring formed by the D-A cycloaddition between furan and maleimide [\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]. Meanwhile, the disappearance of the characteristic absorption peaks of maleimide at ~\u0026thinsp;696 cm⁻\u0026sup1; and furan moieties at ~\u0026thinsp;747 cm⁻\u0026sup1; confirmed the consumption of the reactive functional groups during the grafting process [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e, \u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eTo further confirm the chemical structures of the DAMF-Ni and f-Ni, X-ray photoelectron spectroscopy (XPS) was employed to investigate the specific chemical states and verify the occurrence of the D-A reaction. The wide-scan spectrum is displayed in Fig. S3, In the high-resolution C 1s spectrum, the main C\u0026thinsp;=\u0026thinsp;C sp\u0026sup2; and C-C sp\u0026sup3; peaks are located at ~\u0026thinsp;284.6 eV and ~\u0026thinsp;285.2 eV, and the peaks corresponding to C-S, C-O, C\u0026thinsp;=\u0026thinsp;O, and C-O-C are observed at ~\u0026thinsp;283.2 eV, ~\u0026thinsp;286.2 eV, ~\u0026thinsp;287.7 eV, and ~\u0026thinsp;290.7 eV, respectively (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee) [\u003cspan additionalcitationids=\"CR43\" citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e]. The O 1s spectrum (Fig. S4) was particularly informative, revealing a dominant peak at ~\u0026thinsp;589.7 eV assigned to Ni-O bonds between nano-Ni and the PDA layer, which confirms the chemical anchoring of the PDA coating layer to the nickel surface. Peaks corresponding to C\u0026thinsp;=\u0026thinsp;O (~\u0026thinsp;531.3 eV) and O-H (~\u0026thinsp;528.2 eV) from PDA were also evident [\u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e]. X-ray diffraction (XRD) analysis confirmed the crystal structure of the involved materials. The introduce of the long PEG segments resulted in two new peaks which locate at 19.3\u0026deg; and 23.5\u0026deg;, corresponding to the (120) and (112) crystal planes. This confirms that the MIPEG segments were successfully attached and retain their phase-change ability [\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]. Notably, all samples display the characteristic (111), (200), and (220) reflections of metallic Ni at ~\u0026thinsp;44.5\u0026deg;, 51.9\u0026deg;, and 76.4\u0026deg;, respectively (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef) [\u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e]. The phase transition behaviors of these two samples were further investigated via differential scanning calorimetry (DSC). As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg, both MIPEG and DAMF-Ni present distinct melting and crystallization peaks. Specifically, the melting temperatures and enthalpy of DAMF-Ni are 53.0\u0026deg;C and 80.8 J\u0026middot;g⁻\u0026sup1;, respectively, which are lower than those of MIPEG (57.5\u0026deg;C and 155.5 J\u0026middot;g⁻\u0026sup1;). Obviously, covalent grafting and confinement effects also led to a decrease in the macroscopic phase-change performance of the PEG segment on DAMF-Ni compared to that of pure MIPEG, which is also reflected in XRD results. However, this is an also direct consequence of the high mass fraction of the non-melting Ni core (as determined by thermogravimetric analysis, Fig. S5).\u003c/p\u003e \u003cp\u003eThe rheological properties of DAMF-Ni are critical for its processability and phase-change conformability. The viscosity-temperature curve showed a sharp decrease in viscosity beginning at ~\u0026thinsp;43\u0026deg;C, closely matching the onset of the PEG melting transition observed by DSC, as displayed in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eh. This confirms the solid-to-liquid transition that underpins its melt-infiltration capability. At higher temperatures (\u0026gt;\u0026thinsp;150\u0026deg;C), a second, more gradual decrease in viscosity was observed, corresponding to the retro-D-A reaction, which decouples the PEG chains from the nanoparticles. In addition, vibrating sample magnetometry (VSM) confirmed that the desirable soft-magnetic properties of the nickel core are retained throughout the functionalization process (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei). All samples exhibited narrow hysteresis loops with low coercivity and remanence, characteristic of soft magnets [\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e]. As expected, the saturation magnetization (Mₛ) decreased progressively from pristine nano-Ni (57.2 emu g⁻\u0026sup1;) to f-Ni (38.1 emu g⁻\u0026sup1;) and finally to DAMF-Ni (18.5 emu g⁻\u0026sup1;), reflecting the increasing mass of the non-magnetic organic shell. It should be noted that the insets in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei demonstrate that DAMF-Ni remains strongly responsive to an external magnetic field both below and above its phase-change temperature, confirming its suitability for magnetic-assisted assembly and direct magnetic recovery.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Dual-Mode Interfacial Conformability and Thermal Transport Properties.\u003c/h2\u003e \u003cp\u003eAmong the myriad performance metrics for TIMs, interfacial conformability is critical, as inadequate contact invariably leads to entrapped air pockets that act as thermal barriers and compromise device reliability [\u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]. To address this challenge, DAMF-Ni was engineered with a dual-mode conformability mechanism that synergistically combines phase-change-enabled infiltration with magnetic field-assisted attachment. The interfacial integration process of DAMF-Ni is illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea. Notably, magnetic field-assisted attachment is adopted instead of conventional compression assembly, which can be attributed to its easy magnetization characteristic. Owing to the suitable rheological properties of DAMF-Ni above its melting temperature, it can be dispensed onto the interface via a needle-tube extrusion method. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb, a commercial glue dispenser can be employed to achieve controllable application, highlighting its compatibility with existing manufacturing processes. Upon exposure to an external magnetic field, the embedded Ni nanoparticles become magnetized, generating dipole-dipole interactions between magnetized adjacent particles, which rearranges the alignment of magnetized nanoparticles along the direction of the magnetic field and promotes interfacial contact (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec inset) [\u003cspan citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e, \u003cspan citationid=\"CR51\" class=\"CitationRef\"\u003e51\u003c/span\u003e]. This field-induced reorganization was directly visualized by polarized optical microscopy (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec), revealing the formation of aligned chain-like structures oriented parallel to the applied field. Such alignment is expected to facilitate directional heat transport while simultaneously improving surface wetting. To quantitatively assess the conformability of DAMF-Ni, we fabricated model rough surfaces with well-defined microgrooves on silicone substrates using pulsed laser ablation. The distribution of Ni elements at the interface using Energy-dispersive X-ray spectroscopy (EDS) elemental mapping (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed), which confirms good adherence and distribution of Ni, which ensures homogenous thermal conduction and larger contact area of the DAMF-Ni (Fig. S6). Moreover, the SEM also provided direct evidence of the dual-mode enhancement mechanism. In the absence of magnetic field and below its phase-change temperature, DAMF-Ni exhibited poor contact with the substrate, with visible gaps persisting at the interface (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee). However, after heating above its melting point and applying it under magnetic field, the material flowed to achieve intimate, void-free contact (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef). Additionally, the contact performance of DAMF-Ni on different substrate materials were also evaluated, including metal-based copper plates, polymer films, and SiO\u003csub\u003e2\u003c/sub\u003e samples (Fig. S7), which underscores the versatility of DAMF-Ni for various packaging applications.\u003c/p\u003e \u003cp\u003eThe thermal contact resistance (TCR), which directly reflects interfacial heat transfer efficiency, was evaluated as a function of both temperature and pressure (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eg and S8; see Supporting Information for calculation methodology). For samples with a thickness of ~\u0026thinsp;1 mm, TCR exhibited a sharp decrease around 50\u0026deg;C, which is consistent with the onset temperature of the PEG fusion. This abrupt reduction confirms that the solid-to-liquid transformation enables the material to flow and conform to surface asperities, displacing insulating air and establishing more efficient thermal contact. Besides, above the melting point, TCR continued to decrease gradually and shows asymptotic behavior, reflecting progressive wetting and equilibration of the interface. Pressure-dependent measurements at 80\u0026deg;C revealed a monotonic decrease in TCR with increasing applied pressure from 10 to 60 psi, reaching a minimum value of 0.61 cm\u0026sup2; K W⁻\u0026sup1; at the highest pressure. This value compares favorably with state-of-the-art TIMs, demonstrating the effectiveness of the dual-mode conformability strategy [\u003cspan additionalcitationids=\"CR53 CR54 CR55 CR56 CR57 CR58\" citationid=\"CR52\" class=\"CitationRef\"\u003e52\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR59\" class=\"CitationRef\"\u003e59\u003c/span\u003e]. Notably, the TCR values of DAMF‑Ni exhibit almost no change across the pressure range of 10\u0026thinsp;~\u0026thinsp;60 psi, indicating that DAMF‑Ni has already closely adhered to the interface under magnetic force, and further increasing the pressure has obscure influence on TCR. The inset of Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eg shows the thermal conductivity results of DAMF-Ni and MIPEG, which were tested via the laser flash technique. The thermal conductivity of MIPEG is as low as 0.278 W\u0026middot;m⁻\u0026sup1;\u0026middot;K⁻\u0026sup1;, while that of DAMF-Ni is 1.327 W\u0026middot;m⁻\u0026sup1;\u0026middot;K⁻\u0026sup1;, indicating an improvement of 377.5%. This substantial improvement is believed to result from both the intrinsically high thermal conductivity of the metallic Ni core and the formation of an interconnected particle network (evident in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e2.4 Interfacial thermal management performance of DAMF-Ni\u003c/h2\u003e \u003cp\u003eTo further investigate the actual heat dissipation performance of DAMF-Ni, we constructed a model cooling system comprising an LED bead as the heat source, a heat sink, and various TIMs for comparison. Benchmark materials included a commercial thermally conductive silicone grease (Telesky, 1.93 W m⁻\u0026sup1; K⁻\u0026sup1;) and a commercial thermal pad (Laird, 4 W m⁻\u0026sup1; K⁻\u0026sup1;). DAMF-Ni was pre-conditioned by phase-change infiltration and magnetic-induced attachment, whereas the two reference samples were simply compressed. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea shows the schematic diagram of the heat dissipation unit and the corresponding photographs of the assembled devices. To ensure a fair comparison, the coating thickness of DAMF-Ni and silicone grease was carefully controlled to match that of the commercial pad, eliminating thickness-induced variations in thermal resistance. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb presents the infrared images of the hot spot at 3.5 V, as shown, the surface temperature of the raw LED rises from room temperature to 32.5\u0026deg;C after 10 s of operation, and further increases to 60.5\u0026deg;C at 60 s, which is not conducive to device lifespan and reliability. Incorporation of a TIM dramatically reduced the operating temperature, with the extent of cooling varying markedly among the tested materials. The commercial pad shows the poorest heat dissipation performance, as the LED temperature still reaches 45.6\u0026deg;C after 60 s of operation. This inferior performance is attributable to its limited surface conformability, which prevents intimate contact with the microscopically rough LED surface. Notably, DAMF-Ni outperformed even the high-conductivity silicone grease, demonstrating excellent cooling capability.\u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec exhibits the temperature-time curve for all samples. The bare LED reached a peak temperature of 60.5\u0026deg;C after 60 s. The commercial pad reduced this to 45.6\u0026deg;C (ΔT\u0026thinsp;=\u0026thinsp;14.9\u0026deg;C), while silicone grease achieved 34.3\u0026deg;C (ΔT\u0026thinsp;=\u0026thinsp;26.2\u0026deg;C). Remarkably, DAMF-Ni lowered the LED temperature to just 33.2\u0026deg;C, corresponding to a maximum temperature reduction of 27.3\u0026deg;C relative to the bare device. This exceptional performance underscores the synergistic benefits of phase-change-enabled conformability and magnetic-induced attachment, despite its intrinsic thermal conductivity not being exceptionally high. An interesting observation also emerged in the temperature range of 40\u0026ndash;50\u0026deg;C, in which a plateau appears due to the phase transition of the PEG segment. Therefore, within this temperature range, DAMF-Ni can effectively absorb the heat generated by the LED and reduce its operating temperature. Additionally, Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed shows the cyclic stability performance, where measurements are recorded every ten cycles, and detailed cyclic performance is shown in Fig. S9. As shown, the temperature of the LED with DAMF-Ni remains highly stable within 100 switching cycles, and no discernible changes were observed, indicating its excellent long-term operational reliability in practical applications. This stability contrasts favorably with silicone grease, which is notoriously susceptible to pump-out and dry-out under cyclic thermal loading. In contrast, the covalently anchored polymer brush architecture of DAMF-Ni maintained superior stability even after long-term storage (Fig. S10). To further highlight the outstanding heat dissipation capacity, both the temperature reduction and interfacial heat flux of DAMF-Ni were compared with the commercial samples, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee. DAMF-Ni achieved a temperature reduction of 27.3\u0026deg;C and a heat flux of 18.5 kJ m⁻\u0026sup2; s⁻\u0026sup1;, surpassing both the commercial pad (20.0\u0026deg;C, 9.7 kJ m⁻\u0026sup2; s⁻\u0026sup1;) and silicone grease (26.2\u0026deg;C, 14.2 kJ m⁻\u0026sup2; s⁻\u0026sup1;). Finally, in terms of thermal resistance (and corresponding thermal conductivity) and heat dissipation performance, DAMF-Ni also outperforms other previously reported phase-change TIMs (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef)[\u003cspan additionalcitationids=\"CR61 CR62 CR63 CR64 CR65 CR66 CR67 CR68 CR69 CR70 CR71 CR72 CR73 CR74 CR75 CR76 CR77\" citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR78\" class=\"CitationRef\"\u003e78\u003c/span\u003e]. The excellent interfacial thermal management performance of DAMF-Ni suggests that it holds great promise as a practical TIM.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e2.5 Multiple recycling methods\u003c/h2\u003e \u003cp\u003eThe rapid obsolescence of electronic devices has precipitated a continuous growth of global e-waste [\u003cspan citationid=\"CR79\" class=\"CitationRef\"\u003e79\u003c/span\u003e], with annual generation projected to reach 74.7\u0026nbsp;million tonnes by 2030 [\u003cspan citationid=\"CR80\" class=\"CitationRef\"\u003e80\u003c/span\u003e, \u003cspan citationid=\"CR81\" class=\"CitationRef\"\u003e81\u003c/span\u003e]. Extensive research has focused on recovering metallic [\u003cspan citationid=\"CR82\" class=\"CitationRef\"\u003e82\u003c/span\u003e], ceramic [\u003cspan citationid=\"CR83\" class=\"CitationRef\"\u003e83\u003c/span\u003e], or polymeric fractions from electronic waste [\u003cspan citationid=\"CR84\" class=\"CitationRef\"\u003e84\u003c/span\u003e]. As for TIMs, existing studies have primarily emphasized self-healing properties to extend their service life, rather than addressing post-consumer recovery [\u003cspan additionalcitationids=\"CR86\" citationid=\"CR85\" class=\"CitationRef\"\u003e85\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR87\" class=\"CitationRef\"\u003e87\u003c/span\u003e]. Accordingly, in this work, recyclability was taken into account at the initial stage of DAMF-Ni design. In detail, DAMF-Ni can be recycled via multiple pathways, including direct magnetic recycling, reversible chemical recycling, and upcycling into functional nanofluids or phase change fluids. The soft-magnetic properties of the Ni core enable a simple recycling process by magnetic attraction (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea). After device disassembly, DAMF-Ni can be physically collected from the interface using a strong permanent magnet or an electromagnet, which enables reversible detachment for next use. Notably, after magnetic recovery, DAMF-Ni exhibits excellent reusability, and it can be re-melted and re-spread without any observable degradation in performance (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea, right panel). Moreover, the specific chemical structure of the modified layer constructed via D-A bonds enables the recycling of different chemical components. In addition to direct magnetic recovery, DAMF-Ni can also be recycled using chemical methods (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb). DAMF-Ni can be converted into f-Ni and MIPEG through a reversible D-A reaction, with the FT-IR spectra of MIPEG and re-MIPEG displayed in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb, and as shown, the FT-IR spectrum of the recycled MIPEG (re-MIPEG) is consistent with that of fresh MIPEG, indicating that the chemical recycling method can effectively recover the functional components materials of DAMF-Ni. Moreover, the organic layer on f-Ni can be further chemically removed by acid pickling to obtain recycled nano-Ni; the corresponding SEM image is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb, which exhibits almost the same morphological characteristics as the original nano-Ni. This chemical recycling approach enables the recovery of high-value constituents for reuse in new material formulations, closing the material loop at the component level.\u003c/p\u003e \u003cp\u003eMost innovatively, the unique core-shell structure of DAMF-Ni enables its upcycling into value-added products for entirely new applications. As expected, the hydrophilic PEG brush of DAMF-Ni endows it with excellent hydrophilicity, as its water contact angle is as low as 16.3\u0026deg; (Fig. S11). This merit allows it to stably disperse in hydrophilic media. Given that DAMF-Ni with good thermal conductivity, dispersing it in coolant allows nanofluid application. As a proof-of-concept, DAMF-Ni was dispersed in ethylene glycol (EG) which serve as a commonly used liquid-cooling medium to apply in liquid cooling systems. The assembly diagram of the functional nanofluid (DAMF-Ni/EG) is shown at the top of Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec, from which it can be observed that DAMF-Ni exhibits uniform dispersion in EG at only 1 wt.% addition. In a liquid cooling demonstration, a chip heater without coolant reached a steady-state temperature exceeding 70\u0026deg;C. In comparison, the DAMF-Ni/EG nanofluid achieved a dramatic temperature reduction of 44\u0026deg;C, outperforming the pure EG with temperature reduction of 42.5\u0026deg;C. This upcycling pathway transforms spent TIMs into performance-enhancing additives for advanced cooling applications.\u003c/p\u003e \u003cp\u003eSimilarly, DAMF-Ni can be dispersed in PEG 6000 to create a magnetic-controllable phase-change composite with thermal storage and solar-thermal conversion capabilities. The weight ratio of DAMF-Ni to PEG 6000 was 1:9. The intrinsic dark color of DAMF-Ni, imparted by the polydopamine coating, enables efficient broadband light absorption. SEM and POM confirmed the uniform dispersion of DAMF-Ni within the PEG 6000 matrix. DSC revealed that the resulting DAMF-Ni/PEG 6000 composite exhibits a high latent heat of approximately 175 J g⁻\u0026sup1; due to both components contribute to the phase-change heat storage capacity. Meanwhile, the magnetic Ni cores render the optical absorber magnetically tunable, which is a feature with potential for adaptive solar-thermal harvesting systems, as illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed (bottom left) [\u003cspan citationid=\"CR88\" class=\"CitationRef\"\u003e88\u003c/span\u003e]. Furthermore, in a model house constructed from insulating panels with the composite applied to the roof, the DAMF-Ni/PEG 6000 system effectively buffered temperature fluctuations under simulated solar illumination, demonstrating its potential for passive building temperature regulation (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed, bottom right). Both the functional nanofluid and phase change fluid verify the upcycling potential of DAMF-Ni, which is highly consistent with the future demands for eco-friendly TIMs.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"Conclusion","content":"\u003cp\u003eIn conclusion, we have successfully designed and synthesized a thermal interface paste, DAMF-Ni, which possesses multiple recycling routes, favorable heat dissipation performance, and dual-mode surface adaptability. By synergistically combining thermally induced phase-change infiltration with magnetic field-assisted particle rearrangement, DAMF-Ni achieves exceptional surface wetting that effectively eliminates interfacial air gaps. As a result, DAMF-Ni shows a low thermal contact resistance of 0.61 cm\u0026sup2;\u0026middot;K\u0026middot;W⁻\u0026sup1; without manual pressing. The metallic core also endows DAMF-Ni with a good thermal conductivity of 1.327 W\u0026middot;m⁻\u0026sup1;\u0026middot;K⁻\u0026sup1;, an improvement of 377.5% over the pure phase-change material MIPEG. In practical device-level validation, DAMF-Ni reduced LED operating temperature by up to 27.3\u0026deg;C, outperforming both commercial silicone grease and thermal pads, while maintaining excellent reliability. Benefiting from its soft-magnetic characteristics and specific chemical structure with reversible D-A bonds, DAMF-Ni possesses the capabilities of direct magnetic recycling and chemical recycling, respectively. Magnetic recycling allows for reuse without sacrificing performance, while chemical recycling recovers high-value nano-Ni and MIPEG. Most significantly, we have pioneered an upcycling paradigm: the waste DAMF-Ni can be repurposed as a functional additive in EG to create high-performance nanofluids for liquid cooling, or in PEG 6000 to formulate advanced phase-change composite. The proposed strategy demonstrates the feasibility of developing high-performance TIMs with enhanced interface adaptability and multi-channel recyclability, which can simultaneously deliver state-of-the-art thermal management and contribute to a circular economy.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e \u003ch2\u003eDeclaration of competing interest\u003c/h2\u003e \u003cp\u003eThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eX. Z.: Writing\u0026ndash;original draft, Visualization, Validation, Methodology, Data curation, Investigation. Y. L.: Writing\u0026ndash;original draft, Writing\u0026ndash;review \u0026amp; editing, Visualization, Formal analysis. J. L.: Writing\u0026ndash;original draft, Writing\u0026ndash;review \u0026amp; editing, Validation, Project administration, Methodology, Conceptualization. X. F.: Resources, Investigation. Z. L.: Methodology, Formal analysis. X. L.: Writing\u0026ndash;review \u0026amp; editing, Supervision, Resources, Project administration, Funding acquisition.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThe authors are grateful for the financial support from by National Natural Science Foundation of China (52403150), Natural Science Foundation of Guizhou (Qiankehe-ZK[2022] KEY002), Xinjiang Tianchi Talents Program-Young Doctor Project (BT-2025-TCYC-0012), Xinjiang NJ Project (Tier B Funding), Tarim University President's Fund (TDZKSS202507, TDZKBS202546), General Program of Basic Research Projects of Xinjiang Region (2025DA045), Science and Technology Tackling Program of Alar City (2025GX03).\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eZhang Y, Park M, Park S-J (2019) Implication of thermally conductive nanodiamond-interspersed graphite nanoplatelet hybrids in thermoset composites with superior thermal management capability. 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IEEE Photonics J 14(1):1\u0026ndash;6. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1109/JPHOT.2021.3132795\u003c/span\u003e\u003cspan address=\"10.1109/JPHOT.2021.3132795\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"advanced-composites-and-hybrid-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"achm","sideBox":"Learn more about [Advanced Composites and Hybrid Materials](https://link.springer.com/journal/42114)","snPcode":"42114","submissionUrl":"https://submission.nature.com/new-submission/42114/3","title":"Advanced Composites and Hybrid Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Nanocomposite, Thermal interface material, Recycling and upcycling, Phase change materials, Interface conformability","lastPublishedDoi":"10.21203/rs.3.rs-9241480/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-9241480/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe rapid miniaturization and integration of electronic devices demand highly efficient thermal management while concurrently exacerbating the global electronic waste (e-waste) crisis. Although thermal interface materials (TIMs) are important for heat dissipation, their end-of-life recycling remains a formidable challenge due to stable polymers usually serve as an essential component. Herein, we develop a polymer-grafted Nickel nanoparticles as thermal interface paste (DAMF-Ni) that features dual-mode interface conformability and multi-pathway recyclability. By integrating phase-change polymer segments onto the surface of nickel nanoparticles via reversible covalent bonds, DAMF-Ni achieves enhanced interfacial adaptability through melt infiltration and magnetic-induced attachment, while enabling both chemical and physical recycling via dynamic reactions and magnetic force. Consequently, the material exhibits a remarkably low thermal contact resistance of 0.61 cm\u0026sup2; K W⁻\u0026sup1;, enabling a maximum temperature reduction of 27.3\u0026deg;C at the device interface. Also, its core-shell polymer brush structure allows for upcycling into nanofluids and phase-change composites after end-of-life, demonstrating attractive potential in liquid cooling and thermal storage applications. This work not only broadens the design paradigm of TIMs with interface adaptability but also establishes a sustainable paradigm for mitigating e-waste in thermal management systems.\u003c/p\u003e","manuscriptTitle":"Nano‑Ni-Based Multi-Channel Recyclable Thermal Interface Material with Dual-Mode Interface Adaptability","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-05-18 10:47:45","doi":"10.21203/rs.3.rs-9241480/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"editorInvitedReview","content":"","date":"2026-05-12T10:21:02+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"132472166242662147710059540433348848231","date":"2026-05-11T07:56:09+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"277940864469353626769496109015432220422","date":"2026-05-11T06:51:43+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2026-05-07T08:19:21+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2026-05-04T15:02:09+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2026-03-28T01:22:06+00:00","index":"","fulltext":""},{"type":"submitted","content":"Advanced Composites and Hybrid Materials","date":"2026-03-27T07:13:56+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"advanced-composites-and-hybrid-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"achm","sideBox":"Learn more about [Advanced Composites and Hybrid Materials](https://link.springer.com/journal/42114)","snPcode":"42114","submissionUrl":"https://submission.nature.com/new-submission/42114/3","title":"Advanced Composites and Hybrid Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"271db02d-d6cf-4750-9421-44c2415c1a49","owner":[],"postedDate":"May 18th, 2026","published":true,"recentEditorialEvents":[{"type":"editorInvitedReview","content":"","date":"2026-05-12T10:21:02+00:00","index":29,"fulltext":""},{"type":"reviewerAgreed","content":"132472166242662147710059540433348848231","date":"2026-05-11T07:56:09+00:00","index":26,"fulltext":""},{"type":"reviewerAgreed","content":"277940864469353626769496109015432220422","date":"2026-05-11T06:51:43+00:00","index":25,"fulltext":""},{"type":"reviewersInvited","content":"15","date":"2026-05-07T08:19:21+00:00","index":"","fulltext":""}],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2026-05-18T10:47:45+00:00","versionOfRecord":[],"versionCreatedAt":"2026-05-18 10:47:45","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-9241480","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-9241480","identity":"rs-9241480","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}