Interfacial Engineering of Aluminum Powder with a Tannic Acid/Fe³⁺ Complex and Fluorosilane for High-Performance Energetic Composites

Interfacial Engineering of Aluminum Powder with a Tannic Acid/Fe³⁺ Complex and Fluorosilane for High-Performance Energetic Composites | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Interfacial Engineering of Aluminum Powder with a Tannic Acid/Fe³⁺ Complex and Fluorosilane for High-Performance Energetic Composites Bo Liu, Xiaodong Gou, Yingjun Li, Jiahao Liang, Shi Yan, Xueyong Guo, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8316616/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 07 Mar, 2026 Read the published version in Scientific Reports → Version 1 posted 13 You are reading this latest preprint version Abstract Constructing a multifunctional coating on aluminum (Al) powder is crucial for enhancing its energy release in propellants. However, existing methods face challenges such as complex processes, high costs, and poor controllability. This study proposes a simple self-assembly strategy to construct a dual core-shell structure on aluminum powder surfaces, consisting of an inner tannic acid-Fe³⁺ (TA-Fe) network and an outer fluorosilane (PDTTS) layer, thus successfully fabricating the Al@TA-Fe@PDTTS composite. Molecular dynamics simulations reveal a strong binding energy among the coating components, providing theoretical support for the successful realization of the self-assembly process. The resulting Al@TA-Fe@PDTTS composite exhibits excellent hydrophobicity (contact angle up to 123.7°) and significantly promotes the cracking of the inert alumina shell. Serving as a combined fuel and catalyst, the composite significantly lowers the high-temperature decomposition peak of ammonium perchlorate (AP) by 41.9°C. Furthermore, laser ignition tests confirm a substantially shortened ignition delay (from 13.2 ms for aluminum/AP mixtures to only 4.8 ms for the composite material) and a more intense combustion process, highlighting its great potential for advanced energetic applications. Physical sciences/Chemistry Physical sciences/Engineering Physical sciences/Materials science aluminum powder dual core-shell structure interface performance combustion ammonium perchlorate Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 Figure 10 Figure 11 Figure 12 Figure 13 Figure 14 1. Introduction Aluminum powder is widely used in the formulation of solid propellants due to its high energy density (30.98 kJ·mol − 1 ), active chemical properties, low price, and good compatibility with other materials in the propellant [ 1 – 4 ] . Adding aluminum powder to composite solid propellants can improve the oxygen balance of the propellant and increase the energy, specific impulse and combustion temperature of the propellant [ 5 – 8 ] . However, aluminum will spontaneously react with oxygen in the air to form a layer of aluminum oxide film with a thickness of several nanometers, which wraps the surface of the aluminum particles [ 9 – 10 ] . Since aluminum oxide has a high melting point (2054 ℃) and boiling point (2980 ℃), and low thermal conductivity, it will hinder the mass diffusion and interfacial reaction between the oxidant and aluminum powder, and hinder heat and mass transfer, thereby increasing the ignition temperature and ignition delay time of aluminum powder [ 11 – 13 ] . In the past few decades, the most commonly used method to improve the combustion performance of aluminum powder is to add fluorine-containing compounds. Fluorine not only reacts easily with aluminum, but also has been shown to stimulate the surface pre-ignition exothermic reaction with the Al 2 O 3 shell [ 14 – 16 ] , promoting the production of low-boiling point AlF 3 substances. Therefore, fluorine-containing compounds such as polytetrafluoroethylene (PTFE) [ 17 – 18 ] , polyvinylidene fluoride (PVDF) [ 19 – 22 ] , perfluoric acid [ 23 – 24 ] , and ammonium perfluorooctanoate (APFO) [ 25 ] etc. are used to improve the combustion performance of aluminum powder. Although some studies have shown that fluorine-containing compounds can be effectively combined with aluminum powder by ball milling, this changes the original spherical morphology of aluminum powder and limits its application in propellants [ 26 – 27 ] . In addition, the physical method of directly mixing fluorine-containing compounds and aluminum powder and adding them to solid propellants does not allow the fluorine-containing compounds to fully contact with the aluminum powder. Therefore, how to modify the surface of aluminum powder by directly coating fluorine-containing compounds on the surface of aluminum powder particles so that the fluorine-containing compounds and aluminum powder are in full contact without changing the morphology of aluminum powder, thereby changing the combustion performance of aluminum, has always been a research hotspot. At present, some studies have coated some materials (PTFE, PVDF, polydopamine (PDA), etc.) on the surface of aluminum powder particles to improve the combustion performance of aluminum powder. However, the method of coating the surface of aluminum powder also has many problems: the preparation method is complicated, the raw materials or preparation method are expensive, and the preparation process is difficult to control. Another important component in composite propellants is the oxidizer ammonium perchlorate (AP). The combustion performance of composite propellants is closely related to the thermal decomposition process of AP. The ignition delay time of the propellant can be shortened and the combustion rate can be increased by reducing the peak temperature of AP decomposition [ 28 – 31 ] . A large number of studies have shown that transition metal ion salts or transition metal ion compounds can effectively reduce the thermal decomposition temperature of AP [ 33 – 35 ] . However, these often require complex methods or specialized equipment to prepare. Therefore, in this work, we propose a novel interfacial engineering strategy that concurrently addresses the dual challenges of the inert Al₂O₃ shell and the poor interfacial compatibility. We successfully constructed a dual core-shell structured Al@TA-Fe@PDTTS composite. The design philosophy is twofold: the inner TA-Fe network, formed via the facile self-assembly of low-cost tannic acid and Fe³⁺ ions, is engineered to interact strongly with the native alumina layer and serve as a catalytic site. The outer fluorosilane (PDTTS) layer is designed to confer superior hydrophobicity and, upon decomposition, provide reactive fluorine species that corrode the oxide shell and promote its cracking. This rational design, verified by molecular dynamics simulations, not only ensures a robust coating architecture but also synergistically enhances both the reactivity and interfacial properties of aluminum. This work provides a new insight into the molecular-level interface control for designing advanced multifunctional metal fuels, offering a simple and effective pathway towards high-performance energetic composites. 2. Experimental section 2.1 Materials Aluminum powder was supplied by Hengda Aluminum Co., Ltd. (median particle size D 50 = 5 µm). Ammonium perchlorate was purchased from Liming Research Institute of Chemical Industry. Tannic acid (98%), 1H,1H,2H,2H-Perfluorodecyltriethoxysilane (PDTTS) (98%), FeCl 3 ·6H 2 O (99%),and n-Hexane (≥ 98%), Tris-Bis (99.5% purity), were purchased from Shanghai Macklin Biochemical Co., Ltd. Absolute ethanol (≥ 99.7%) was obtained from Shanghai Energy Chemical Co., Ltd. All chemicals are analytical grade. 2.2 Synthesis of Al@TA-Fe Composite The Al@TA-Fe composite was fabricated via a facile one-pot coordination-driven self-assembly process. In a typical procedure, 0.4 g of TA was first dissolved in 200 mL of deionized water under magnetic stirring to form a clear solution. Subsequently, 2 g of raw Al powder was introduced into the TA solution and uniformly dispersed via ultrasonication for 10 min. Then, 20 mL of an aqueous FeCl₃·6H₂O solution (0.065 g) was added dropwise into the mixture, which was allowed to react for 20 min. This step facilitates the rapid formation of a coordinated TA-Fe network on the Al surface. The pH of the reaction system was then adjusted to 8.0 using a Tris-Bis buffer solution to optimize the coordination environment and enhance the adhesion of the network. The resulting product was collected by filtration, thoroughly washed with deionized water, and dried overnight at ambient temperature to yield the Al@TA-Fe powder. 2.3 Construction of the Dual Core-Shell Structure (Al@TA-Fe@PDTTS) To impart hydrophobicity and introduce reactive fluorine species, the as-prepared Al@TA-Fe composite was further functionalized with PDTTS. Briefly, 10 g of Al@TA-Fe was fully dispersed in 100 mL of n-hexane via ultrasonication. Then, 1 g of PDTTS was added dropwise into the suspension. The mixture was left to stand for 24 h, allowing the silane groups of PDTTS to condense with the residual hydroxyl groups on the TA-Fe surface, forming a robust covalent interface. The final product, denoted as Al@TA-Fe@PDTTS, was obtained by filtration, washed three times with n-hexane to remove unreacted precursors, and dried at 50°C. A schematic illustration of the overall fabrication process is presented in Fig. 1 .The macroscopic morphologies of pure Al powder and A are shown in Fig.S1. 2.4 Characterization and Methods The sample was observed using a ZEISS Sigma 300 scanning electron microscope (SEM) and a Tecnai G2 F30 S-TWIN transmission electron microscope (TEM). Powder X-ray diffraction (PXRD) was performed on a Panaco Emoyrean instrument using a Cu target, scanning from 5° to 90° at 10°·min − 1 . Fourier transform infrared spectrometer (FT-IR) was performed using a Thermo Scientific Nicolet iS20 instrument. The test range is 4000 cm − 1 to 400 cm − 1 . X-ray Photoelectron Spectroscopy (XPS) was performed using a Thermo Scientific K-Alpha. The spot size is 400 µm, the working voltage is 12 kV, the filament current is 6 mA; the full spectrum scanning energy is 150 eV, and the step size is 1 eV. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) were performed on a Mettler Toledo -TGA/DSC 3 + with the heating rate of 10 K·min − 1 (or 20 K·min − 1 ) in the Ar atmosphere. The static contact angle was measured by the hypsometry method using the standard static drop method, using the JY-82B Kruss DSA type contact angle meter. To investigate the combustion products of the sample in an air atmosphere, 200 mg of the sample was placed in a transparent tube furnace (air atmosphere), heated to 600 ℃ (or 800 ℃) at a rate of 20 ℃·min − 1 , and kept warm for 10 min. The reaction products were collected after cooling to room temperature and characterize them by SEM and XRD. TRHW-7000C automatic oxygen bomb calorimeter was used to test the combustion calorific value of the sample. The combustion calorific value of each sample is measured in parallel three times, and the average value is taken as the final result. In high-speed photography experiments, Al and Al@TA-Fe@PDTTS was physically uniformly mixed with AP in a mass ratio of 9:1. Then, 100 mg of the sample was placed on the ignition platform and the sample was ignited using a CO 2 laser ignition system with an output power of 30 W and a duration of 500 ms under air atmosphere and atmospheric pressure conditions. After the mixed sample was ignited, the combustion process of the sample was recorded using a high-speed camera with a shooting rate of 10000 fps and an exposure time of 50 ms. 2.5 Model calculations and calculation conditions for molecular simulation experiments In this study, the aim was to evaluate the binding ability between Al, TA and PDTTS by molecular dynamics simulation and to prove the rationality of this experimental design. The molecular structures of Al, TA and PDTTS were established using the Visualizer module in the Materials Studio software package, as shown in Fig. 2 (a), Fig. 2 (b) and Fig. 2 (c), respectively. Based on the original molecular structure, Al was expanded into a 4×4×2 supercell, and 3D periodic boxes of 12 TA molecules and 30 PDTTS molecular chains were constructed using the Amorphous Cell module, as shown in Fig. 2 (d), Fig. 2 (e) and Fig. 2 (f), respectively. The structures and molecular dynamics simulations of the Al/TA, Al/PDTTS, and Al/TA/PDTTS molecular models were optimized using the Forcite module. COMPASS Ⅱ was used as the force field, NVT as the ensemble, the temperature was set to 298 K, the time step was 0.1 fs, the total simulation time was 1000 ps, and the last 500 ps of data were used for subsequent performance analysis. 3 Result and discussion 3.1. Binding energy Binding energy is an important parameter that reflects the magnitude of intermolecular interaction forces and can reflect the strength of different intermolecular interactions [ 37 ] . Binding energy (E bind ) can be defined as the negative value of intermolecular interaction energy (E inter ). Intermolecular interaction energy can be calculated from the total energy of each component in the equilibrium state of the mixed system, as shown in Eq. (1): E bind =-E inter =-(E A−B -E A(A−B) -E B(A−B) ) (1) In Eq. (1), E A−B represents the total energy of the composite system; E A(A−B) represents the energy of A in the composite system, and E B(A−B) represents the energy of B in the composite system. For a system to reach dynamic equilibrium, it is usually necessary to make the temperature and energy in the system reach equilibrium. In general, as long as the temperature and energy remain within the fluctuation range of 5% to 10%, it can be concluded that dynamic equilibrium has been achieved [ 38 ] . Figure 3 shows the fluctuation curves of temperature (Fig. 3 a-c) and energy (Fig. 3 d-f) during the molecular dynamics simulation of the systems Al 2 O 3 /TA, Al 2 O 3 /PDTTS, and Al 2 O 3 @TA/PDTTS. As time goes by, after 500ps, the fluctuations of the temperature and energy of the system are within 5%, and the system reaches equilibrium. The above results show that all simulation systems have reached dynamic equilibrium, which ensures the reliability of subsequent data collection and analysis. Figure 4 (a-d), Fig. 4 (b-e) and Fig. 4 (c-f) show the optimized model diagrams and final equilibrium structure diagrams of the mixed molecular systems Al 2 O 3 /TA, Al 2 O 3 /PDTTS and A l2 O 3 /TA/PDTTS, respectively. The binding energy calculation results of each system are shown in Table 1 . The binding energies of the systems Al 2 O 3 /TA, Al 2 O 3 /PDTTS and Al 2 O 3 @TA/PDTTS are 782.36 kcal⋅mol − 1 , 211.79 kcal⋅mol − 1 and 498.21 kcal⋅mol − 1 , respectively. The results show that TA molecules have good bonding ability with Al 2 O 3 , which explains why the TA interface layer can be well coated on the Al 2 O 3 surface, which is mainly due to the formation of hydrogen bonds between the H atoms in the TA molecules and the O atoms in the Al 2 O 3 . At the same time, the binding ability of PDTTS with TA is also much higher than that of PDTTS with Al 2 O 3 . This is mainly because the F atoms in PDTTS are more likely to form hydrogen bonds with the -OH in TA, making the binding ability between them stronger. The above results show that the binding ability of TA with the Al 2 O 3 crystal surface is better than that of PDTTS. For PDTTS, its binding ability on the TA surface layer is also significantly better than that of Al 2 O 3 particles. The results of simulation calculations show the rationality of the experimental design. Table 1 Binding energies of Al 2 O 3 /TA, Al 2 O 3 /PDTTS and Al 2 O 3 @TA/PDTTS System Al 2 O 3 /TA, Al 2 O 3 /PDTTS Al 2 O 3 @TA/PDTTS Binding energy (kcal·mol − 1 ) 782.36 211.79 498.21 3.2. Characterization of Al@TA-Fe@PDTTS Figure 5 shows the microscopic morphology of each sample. As can be seen from Fig. 5 (a) and Fig. 5 (c), the surfaces of pure Al particles and Al@PDTTS are smooth. The SEM image of Fig. 5 (b) shows that the surfaces of Al@TA-Fe particles and Al@TA-Fe@PDTTS are rougher than those of pure Al particles and Al@PDTTS particles. It can be clearly observed from the magnified image that many protrusions are formed on the surface of the aluminum particles, which is caused by the different thickness of the TA-Fe coating layer. Figure 5 (e) is the EDS spectrum of the surface of Al@TA-Fe@PDTTS particles. Compared with Al powder, the surface layer of Al@TA-Fe@PDTTS contains C, Fe, Si and F elements, confirming that the TA-Fe and PDTTS interface layer are successfully established. In order to further study the coating of TA-Fe layer and PDTTS layer on the surface of aluminum powder, TEM morphology detection and EDS surface scanning test were carried out on the Al@TA-Fe@PDTTS sample, and the results are shown in Fig. 6 . As can be seen from Fig. 6 (a) and Fig. 6 (b), there is an irregularly shaped coating layer on the surface of the aluminum powder particles. Combining the high-resolution image of the edge of a single particle and the element energy spectrum surface scanning image, it can be found that the surface of the Al@TA-Fe@PDTTS particle is roughly divided into three regions. The black part in the center is the Al core, the dark gray ring area is the aluminum oxide layer, and the TA-Fe and PDTTS coating layers are outside the aluminum oxide. According to Fig. 6 (b-e), it can be found that the TA-Fe and PDTTS layers are relatively uniformly dispersed on the surface of the aluminum powder particles. The above results successfully prove the core-shell structure of Al@TA-Fe@PDTTS. In order to further explore the surface of Al@TA-Fe@PDTTS particles, FT-IR analysis was performed, as shown in Fig. S2. The diffraction peak at 822 cm − 1 can be attributed to the asymmetric stretching vibration peak of -CF 2 , and the peak at 1055 cm − 1 is the characteristic absorption peak of Si-O-C in the PTTDS molecule [ 39 ] . The peak at 1193 cm − 1 is the stretching vibration peak of the ester group in TA [ 40 ] . The peak at 1336 cm − 1 is the C-O stretching vibration peak in the TA molecule. The peaks at 1572 cm − 1 and 1431 cm − 1 can be attributed to the C-C stretching vibration of the benzene ring in the TA molecule. The peak at 1689 cm − 1 belongs to the C = O stretching vibration peak in the TA molecule. The peak at 2937 cm − 1 belongs to the asymmetric stretching vibration absorption peak of the C-H bond in PDTTS, and the peak at 3351 cm − 1 can be attributed to the vibration peak of the hydroxyl group in TA. The FT-IR results show that the characteristic peaks of TA and PDTTS exist on the surface of Al@TA-Fe@PDTTS particles. This result also proves that the TA-Fe coating layer and the PDTTS coating layer are successfully coated on the surface of the aluminum powder particles. In addition, XPS was used to measure and characterize the element types and valence states on the surface of Al@TA-Fe@PDTTS particles, as shown in Fig. 7 . The full XPS spectrum of Al@TA-Fe@PDTTS shows that the surface layer of Al@TA-Fe@PDTTS contains C, O and F elements (Fig. 7 a), while the Al peak is not clearly detected. This may be because the surface layer of the aluminum particles is covered by the TA-Fe@PDTTS coating layer, which affects the detection of the internal aluminum element. At the same time, the detection of the Fe element is not obvious, which is mainly due to the low content of Fe in Al@TA-Fe@PDTTS. Figure 7 (b-d) shows the high-resolution XPS spectra of C, O and F elements. The spectrum of the C element can be divided into five peaks, namely the C-H peak at 284.3 eV, the C-C peak at 286.0 eV, the O-C = O peak at 287.9 eV, the -CF 2 peak at 291.0 eV and the -CF 3 peak at 293.3 eV [ 41 ] . The peak of the O element can be fitted by two peaks, the peak of 531.0 eV is attributed to the oxygen atom of C-O-C in TA, and the peak of 532.6 eV is attributed to the oxygen atom of -OH. In the XPS spectrum of the F element, the peak at 688.7 eV can be attributed to the peak of the F atom in C-F. The above results further show that Al@TA-Fe@PDTTS has a dual core-shell structure. 3.3 Interface performance of Al@TA-Fe@PDTTS In order to observe the interfacial properties of Al and Al@TA-Fe@PDTTS, the contact between Al and Al@TA-Fe@PDTTS and water was studied in detail, as shown in Fig. 8 . Pure Al gradually settles to the bottom of the water after being added to the water, and is dispersed in the water to form a suspension after vigorous shaking. In contrast, Al@TA-Fe@PDTTS float directly on the water after being added to water. Even after violent shaking, Al@TA-Fe@PDTTS can still float on the water. This result shows that the surface property of Al@TA-Fe@PDTTS has changed significantly relative to pure Al, In addition, it can also be concluded that the coating of Al@TA-Fe by PDTTS is dense. In addition, the static contact angles of the samples with water were tested, as shown in Fig. 8 . The average static contact angle of pure Al with water is only 21.0°, while the average static contact angles of Al@TA-Fe@PDTTS and Al@PDTTS with water can reach 123.7° and 83.9°, respectively. Even after 30 days in water, the average static contact angles of Al@TA-Fe@PDTTS and Al@PDTTS can still reach 102.7° and 73.3°. The contact angle of Al@TA-Fe@PDTTS with water is always larger than that of Al@PDTTS, which also shows that using TA-Fe as the intermediate layer can make PDTTS better coated on the surface of aluminum powder. These results indicate that the surface layer of aluminum particles is covered with hydrophobic C and F elements, which also reflects that Al@TA-Fe@PDTTS has better hydrophobicity and corrosion resistance than pure aluminum powder [ 42 ] . 3.4 Thermal reaction properties of Al@TA-Fe@PDTTS Figure 9 shows the DSC/TG curves of Al and Al@TA-Fe@PDTTS in an argon atmosphere. In the temperature range of 0-800°C, pure aluminum powder has a melting endothermic peak at 660°C and no weight loss process. The DSC curve of Al@TA-Fe@PDTTS shows that the peak at 327.7°C is the decomposition peak of TA, followed by a small exothermic peak for the decomposition peak of PDTTS; the peak at 660°C is the characteristic endothermic peak of aluminum. The peak at 653°C is the redox exothermic peak generated by the reaction between aluminum and the decomposition products of TA and PDTTS coating. The TG curve of Al@TA-Fe@PDTTS shows that it gradually decomposes and loses weight from 110°C, which is mainly caused by the thermal decomposition of TA. Al@TA-Fe@PDTTS begins to lose weight rapidly when the temperature reaches about 300°C, which is mainly due to the continuous decomposition of TA and the thermal decomposition of PDTTS [ 43 ] . The thermal weight loss process of Al@TA-Fe@PDTTS basically ends at around 510°C, and reaches the maximum thermal weight loss at 550°C, with a weight loss of about 25 wt%. It then undergoes a short weight gain process between 610°C and 655°C, corresponding to the redox exothermic peak at 653°C in the DSC curve. The results show that the sample Al@TA-Fe@PDTTS has begun to react before the melting point of aluminum, and the heat released by the reaction can promote the internal aluminum oxidation reaction. Pure aluminum powder cannot react at 660°C. in the Ar atmosphere. In addition, the combustion performance of Al and Al@TA-Fe@PDTTS in air was studied. Aluminum powder was reacted with Al@TA-Fe@PDTTS at different temperatures (600°C and 800°C) in air atmosphere for 10 min, and the combustion products were collected and analyzed. Figure 10 shows the SEM images of pure aluminum powder after reaction at 600°C and 800°C in air. The morphology of most aluminum particles in the reaction products of pure aluminum powder at 600°C did not change significantly, and they showed a regular spherical morphology. At 800°C, only a very small part of the aluminum powder underwent a typical shell-breaking reaction, while most of the aluminum powder still showed a complete and regular spherical morphology. Therefore, even at high temperatures, pure aluminum powder is difficult to completely oxidize in air. However, the morphology of a part of the Al@TA-Fe@PDTTS reaction products changed dramatically at 600°C, forming irregular fragments instead of spherical aluminum particles. When the temperature was increased to 800°C, this proportion increased significantly, forming a large number of irregular fragments. This indicates that Al@TA-Fe@PDTTS can react below the melting point of aluminum (660°C) and that the TA-Fe@PDTTS dual interface layer can promote the oxidation reaction of aluminum. 800 ◦C in the air atmosphere; (c) and (f) magnified images of the corresponding reaction products of Al and Al@TA-Fe@PDTTS at 800 ◦C. The combustion products of Al@TA-Fe@PDTTS were analyzed by XRD, as shown in Fig. 11 . The test results show that the combustion products are mainly A l2 O 3 , a small amount of AlF 3 and incompletely reacted Al. The above results show that the fluorine element decomposed in the PDTTS coating layer participates in the oxidation reaction of aluminum. The porous structure of AlF 3 not only increases the contact area between Al and the external oxidant, but also promotes the diffusion of Al through the porous channels, promoting the release of energy and the combustion kinetics reaction [ 23 ] . The above results all show that the Al@TA-Fe@PDTTS dual coating can greatly promote the oxidation reaction of aluminum, and can even catalyze the oxidation reaction of aluminum under conditions below the melting point of aluminum [ 14 , 19 , 44 ] . Based on the above experimental results, the thermal reaction mechanism of Al@TA-Fe@PDTTS during heating is proposed. As the temperature rises, the TA layer and PDTTS layer on the surface of Al@TA-Fe@PDTTS release strong oxidizing free radicals such as F· and C X F· during the thermal decomposition process. They react with the oxygen in the environment through the cracks and gaps in the Al 2 O 3 shell and the Al 2 O 3 film on the surface of the aluminum powder, corroding the aluminum oxide film to form AlF 3 . The evaporation point of AlF 3 is lower than that of aluminum oxide, and it is easier to volatilize from the surface of the aluminum powder, thereby exposing the internal aluminum and reacting with the external oxygen [ 15 – 16 ] . This explains why the reaction degree of Al@TA-Fe@PDTTS is higher than that of pure Al. 3.5 Effect of Al@TA-Fe@PDTTS on catalytic thermal decomposition of AP In order to study the catalytic decomposition of AP by Al@TA-Fe@PDTTS, Al@TA-Fe@PDTTS and AP were mixed at a mass ratio of 9:1, and then Al@TA-Fe@PDTTS/AP and AP were performed DSC analysis in an Ar atmosphere., as shown in Fig. 12 . It can be seen from the DSC curve that Al@TA-Fe@PDTTS/AP and AP have one endothermic peak and two exothermic peaks. The endothermic peak at 247°C is formed by the transformation of AP from an orthorhombic structure to a cubic structure. After adding Al@TA-Fe@PDTTS, the high temperature decomposition peak of AP dropped from 422.3 ◦C to 380.4 ◦C. In addition, the exothermic peak of the high-temperature decomposition stage of AP in Al@TA-Fe@PDTTS/AP is much larger than that of pure AP, which may be due to two reasons. One is that the decomposition temperature range of TA-Fe@PDTTS coincides with the high-temperature decomposition range of AP, and the other is that the TA-Fe layer significantly improves the thermal decomposition stage of AP. The results show that Al@TA-Fe@PDTTS can significantly reduce the peak temperature of high-temperature decomposition of AP. K·min − 1 in the Ar atmosphere. The heat release of combustion is an important parameter for measuring the energy materials. The energy release level of energetic materials can be intuitively seen through the combustion heat value. The combustion heat of Al/AP and Al@TA-Fe@PDTTS/AP mixtures was measured under different oxygen pressures (3 MPa, 2 MPa, 1 MPa, and 0.5 MPa) using an oxygen bomb calorimeter. Each sample was measured three times and the average value was taken. The results are shown in Fig. 13 . It can be found that when the oxygen pressure dropped from 3 MPa to 1 MPa, the combustion heat values of both samples decreased slightly. Under the same oxygen pressure, the combustion heat value of Al@TA-Fe@PDTTS/AP is always slightly higher than that of Al/AP. This is because although the composite structure can promote heat and mass transfer [ 45 ] , since the combustion of aluminum powder in an oxygen-rich environment is relatively complete, the introduction of TA-Fe and PDTTS coatings has limited effect on the improvement of the combustion heat value of Al. When the oxygen pressure drops from 1 MPa to 0.5 MPa, the combustion heat value of the Al/AP and Al@TA-Fe@PDTTS/AP mixtures decreases significantly from 25.716 kJ·mol − 1 and 26.027 kJ·mol − 1 (the difference between the two is 0.311 kJ·mol − 1 ) to 22.331 kJ·mol − 1 and 23.728 kJ·mol − 1 (the difference between the two is 1.397 kJ·mol − 1 ). The above results show that the coating layer on the surface of aluminum powder has a more significant effect on the combustion of aluminum powder in a low-oxygen environment, which also confirms our previous analysis of the thermal decomposition mechanism of Al@TA-Fe@PDTTS during heating. Ignition delay time is one of the indicators of ignition reliability and one of the important factors affecting the tactical performance and accuracy of energetic materials and equipment. The ignition delay time here is defined as the time delay required for the sample to ignite and burn normally after receiving laser energy stimulation. In the laser ignition experiment, the time difference between the appearance of the laser signal and the appearance of the sample ignition signal is identified as the ignition delay time. The results are shown in Fig. S3. The ignition delay times of Al/AP and Al@TA-Fe@PDTTS/AP are 13.2 ms and 4.8 ms, respectively. The introduction of TA-Fe and PDTTS coating layers can effectively shorten the ignition delay time of the mixture. The combustion process of Al/AP and Al@TA-Fe@PDTTS/AP is shown in Fig. 14 . The combustion time of the Al/AP mixture is 250 ms, while the combustion time of the Al@TA-Fe@PDTTS/AP mixture exceeds 500 ms. Comparing the combustion of the two samples, in the combustion process of the Al/AP mixture, the intense combustion lasts for a shorter time and the flame formed is smaller. The combustion of the Al@TA-Fe@PDTTS/AP mixture is more intense, the combustion area formed is larger, and the intense combustion lasts for a longer time. Compared with Al/AP, Al@TA-Fe@PDTTS/AP starts to burn violently earlier and forms more sparks. The above results show that the composite structure of Al@TA-Fe@PDTTS has a larger contact area, which is conducive to heat and mass transfer, resulting in a faster combustion response of the mixture and a higher degree of combustion. 4. Conclusion In this paper, an aluminum-based composite material Al@TA-Fe@PDTTS with a dual core-shell structure was successfully prepared. The morphology and component characterization show that both TA-Fe and PDTTS are uniformly coated on the surface of aluminum particles, and Al@TA-Fe@PDTTS has better hydrophobicity than pure aluminum powder. The molecular dynamics calculation results show that the binding energy between PDTTS and TA is 498.21 kcal⋅mol − 1 , while the binding energy between TA and Al 2 O 3 reaches 782.36 kcal⋅mol − 1 , which provids a theoretical basis for the establishment of the dual coating layer. In addition, the TA-Fe@PDTTS dual coating layer can change the reaction process of aluminum in air atmosphere, so that aluminum reacts below the melting point. When mixed with AP, the presence of Al@TA-Fe@PDTTS can reduce the peak temperature of AP's high-temperature decomposition by 41.9 ℃. Moreover, the combustion heat value of the Al@TA-Fe@PDTTS/AP mixture is always higher than that of Al/AP, especially in a low oxygen pressure environment. Combustion experiments show that Al@TA-Fe@PDTTS/AP has a faster combustion response and a higher degree of combustion than Al/AP, and the ignition delay time is reduced from 13.2 ms to 4.8 ms. 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. Funding This work was supported by the National Natural Science Foundation of China [grant number 22175026]. Role of the funding source： The funding agency had no role in the study design, collection, analysis, interpretation of data, writing of the manuscript, or decision to submit it for publication. 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Cite Share Download PDF Status: Published Journal Publication published 07 Mar, 2026 Read the published version in Scientific Reports → Version 1 posted Editorial decision: Revision requested 19 Jan, 2026 Reviews received at journal 12 Jan, 2026 Reviewers agreed at journal 05 Jan, 2026 Reviews received at journal 02 Jan, 2026 Reviewers agreed at journal 29 Dec, 2025 Reviewers agreed at journal 18 Dec, 2025 Reviews received at journal 17 Dec, 2025 Reviewers agreed at journal 17 Dec, 2025 Reviewers invited by journal 16 Dec, 2025 Editor invited by journal 16 Dec, 2025 Editor assigned by journal 11 Dec, 2025 Submission checks completed at journal 11 Dec, 2025 First submitted to journal 09 Dec, 2025 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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17:08:54","extension":"png","order_by":30,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":20259,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage9.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/1377bf129036a2df1e8792ff.png"},{"id":98517796,"identity":"6ccd7a1d-8cf0-4c05-85c8-47d95c79d48b","added_by":"auto","created_at":"2025-12-18 12:56:33","extension":"xml","order_by":31,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":109299,"visible":true,"origin":"","legend":"","description":"","filename":"ae4f2567ecff4d53b5c4d7a5405106911structuring.xml","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/7a6ab382fe9d69c13c16e3a5.xml"},{"id":98625211,"identity":"32beaf00-f9ab-40d8-9ef1-75b981047957","added_by":"auto","created_at":"2025-12-19 17:08:59","extension":"html","order_by":32,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":119292,"visible":true,"origin":"","legend":"","description":"","filename":"earlyproof.html","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/68b1cdde656c0a227d4d98c9.html"},{"id":98517756,"identity":"f9a5a03f-3719-4649-8ec7-e4f36390f820","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":221120,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic diagram of the preparation process and experimental process of Al@TA-Fe@PDTTS.\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/d56013c2c859f4a256717a89.png"},{"id":98517757,"identity":"3639d18f-75c4-48c9-aad4-a16898427e59","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":404823,"visible":true,"origin":"","legend":"\u003cp\u003e(a), (b), and (c) are the molecular structure of Al, TA and PDTTS, respectively; (d) shows the super cell of Al; (e) and (f) are the 3D AC boxes of TA and PDTTS, respectively.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/4eff5629b9d2af670bf14ac7.png"},{"id":98517759,"identity":"ff115cfd-4ea2-4a62-a6aa-45a65794d480","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":210573,"visible":true,"origin":"","legend":"\u003cp\u003e(a) and (d), (b) and (e), and (c) and (f) are the temperature and energy fluctuation curves of the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA system, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS system, and Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA/PDTTS system in equilibrium, respectively.\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/bb6f85c4180a3e0d1b86f68e.png"},{"id":98517766,"identity":"1228276b-5c26-4668-b0f7-0825039c1a08","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":828846,"visible":true,"origin":"","legend":"\u003cp\u003ePictures (a) and (d), (b) and (e), and (c) and (f) are optimized models and equilibrium structures of Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS and Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e@TA/PDTTS.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/b91cca172119e8e72b1ebef0.png"},{"id":98517760,"identity":"3e32bc41-29c8-4e5a-8069-ec92a593c906","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":979354,"visible":true,"origin":"","legend":"\u003cp\u003eSEM images of (a) Al, (b) Al@TA-Fe (c) Al@PDTTS and (d) Al@TA-Fe@PDTTS; (e) EDS mapping of Al@TA-Fe@PDTTS.\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/e3ff0c8c280ba1cc0f691fd3.png"},{"id":98624943,"identity":"88c28cac-26a7-4866-b81d-d89e735b45ee","added_by":"auto","created_at":"2025-12-19 17:08:51","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":539398,"visible":true,"origin":"","legend":"\u003cp\u003eTEM image and energy spectrum scanning of Al@TA-Fe@PDTTS single particle.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/db414f5d065d5c7302443108.png"},{"id":98624935,"identity":"f6ddd5c9-a042-4ce0-a6e1-8a37a096f5e2","added_by":"auto","created_at":"2025-12-19 17:08:50","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":109683,"visible":true,"origin":"","legend":"\u003cp\u003eSurvey XPS binding energy spectra and the high-resolution XPS spectra of C 1s, O 1s, and F 1s peaks of Al@TA-Fe@PDTTS.\u003c/p\u003e","description":"","filename":"floatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/e81009628cdb280c21274207.png"},{"id":98624394,"identity":"1c12747e-e9d2-443c-8336-9c70a6f391f5","added_by":"auto","created_at":"2025-12-19 17:08:23","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":490024,"visible":true,"origin":"","legend":"\u003cp\u003ePhotographs of (a) Al, (b) Al@PDTTS and (c) Al@TA-Fe@PDTTS entering the water, and after severe shaking; Static water contact angles of (d) Al, (e) Al@TA-Fe@PDTTS and (f) Al@PDTTS, and (g) Al@TA-Fe@PDTTS and (h) Al@PDTTS after 30 days in water.\u003c/p\u003e","description":"","filename":"floatimage8.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/b6fc55cedde5cf245a2b32c4.png"},{"id":98517774,"identity":"0c9fa070-d461-497c-9c76-cb3a1dd482d7","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":83977,"visible":true,"origin":"","legend":"\u003cp\u003eTG/DSC curves of Al and Al@TA-Fe@PDTTS with the heating rate of 10 K/min\u003c/p\u003e\n\u003cp\u003ein the Ar atmosphere.\u003c/p\u003e","description":"","filename":"floatimage9.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/84228397717fa8426d7f68d6.png"},{"id":98625025,"identity":"b6acd524-b4d0-4301-836d-7aa850edfccc","added_by":"auto","created_at":"2025-12-19 17:08:53","extension":"png","order_by":10,"title":"Figure 10","display":"","copyAsset":false,"role":"figure","size":1089263,"visible":true,"origin":"","legend":"\u003cp\u003eSEM images of the reaction products of Al powder at (a) 600 ◦C and (b) 800 ◦C in the air atmosphere; SEM images of the reaction products of Al@TA-Fe@PDTTS at (d) 600 ◦C and (e)\u003c/p\u003e\n\u003cp\u003e800 ◦C in the air atmosphere; (c) and (f) magnified images of the corresponding reaction products of Al and Al@TA-Fe@PDTTS at 800 ◦C.\u003c/p\u003e","description":"","filename":"floatimage10.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/196c2fe78ffa9dd063a4cad1.png"},{"id":98624714,"identity":"ba6f072d-ed14-4a5c-97ea-afcc3ca4e1af","added_by":"auto","created_at":"2025-12-19 17:08:40","extension":"png","order_by":11,"title":"Figure 11","display":"","copyAsset":false,"role":"figure","size":60874,"visible":true,"origin":"","legend":"\u003cp\u003eXRD patterns of (a) pure Al and (b) Al@TA-Fe@PDTTS calcined products (800 ℃).\u003c/p\u003e","description":"","filename":"floatimage11.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/4214519806a77e89d25413e1.png"},{"id":98625267,"identity":"a8f04047-d92f-4537-9159-b84179dcfa3e","added_by":"auto","created_at":"2025-12-19 17:09:00","extension":"png","order_by":12,"title":"Figure 12","display":"","copyAsset":false,"role":"figure","size":33744,"visible":true,"origin":"","legend":"\u003cp\u003eDSC curves of pure AP and Al@TA-Fe@PDTTS/AP with the heating rate of 10 K·min\u003csup\u003e-1\u003c/sup\u003e in the Ar atmosphere.\u003c/p\u003e","description":"","filename":"floatimage12.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/d8d13ab2873f67ae77e2587e.png"},{"id":98517771,"identity":"13132f6a-f098-4bd9-9dac-e4a0cb1335b4","added_by":"auto","created_at":"2025-12-18 12:56:31","extension":"png","order_by":13,"title":"Figure 13","display":"","copyAsset":false,"role":"figure","size":40952,"visible":true,"origin":"","legend":"\u003cp\u003eCombustion heat values of samples at different oxygen pressures.\u003c/p\u003e","description":"","filename":"floatimage13.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/13f8f8ed4218c00f7c70704c.png"},{"id":98517786,"identity":"93724605-81a0-413c-9f61-d964f6589626","added_by":"auto","created_at":"2025-12-18 12:56:32","extension":"png","order_by":14,"title":"Figure 14","display":"","copyAsset":false,"role":"figure","size":245981,"visible":true,"origin":"","legend":"\u003cp\u003eLaser ignition combustion process of Al/AP and Al@TA-Fe@PDTTS/AP samples.\u003c/p\u003e","description":"","filename":"floatimage14.png","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/8f5d05cdef819b93b19ed253.png"},{"id":104252140,"identity":"14d73683-0dd1-42ad-b619-819c6c39e48e","added_by":"auto","created_at":"2026-03-09 16:17:21","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":6475959,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8316616/v1/6ffa2b43-a722-4905-a734-5222f8611bbb.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Interfacial Engineering of Aluminum Powder with a Tannic Acid/Fe³⁺ Complex and Fluorosilane for High-Performance Energetic Composites","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eAluminum powder is widely used in the formulation of solid propellants due to its high energy density (30.98 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), active chemical properties, low price, and good compatibility with other materials in the propellant\u003csup\u003e[\u003cspan additionalcitationids=\"CR2 CR3\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e]\u003c/sup\u003e. Adding aluminum powder to composite solid propellants can improve the oxygen balance of the propellant and increase the energy, specific impulse and combustion temperature of the propellant\u003csup\u003e[\u003cspan additionalcitationids=\"CR6 CR7\" citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]\u003c/sup\u003e. However, aluminum will spontaneously react with oxygen in the air to form a layer of aluminum oxide film with a thickness of several nanometers, which wraps the surface of the aluminum particles\u003csup\u003e[\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]\u003c/sup\u003e. Since aluminum oxide has a high melting point (2054 ℃) and boiling point (2980 ℃), and low thermal conductivity, it will hinder the mass diffusion and interfacial reaction between the oxidant and aluminum powder, and hinder heat and mass transfer, thereby increasing the ignition temperature and ignition delay time of aluminum powder\u003csup\u003e[\u003cspan additionalcitationids=\"CR12\" citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eIn the past few decades, the most commonly used method to improve the combustion performance of aluminum powder is to add fluorine-containing compounds. Fluorine not only reacts easily with aluminum, but also has been shown to stimulate the surface pre-ignition exothermic reaction with the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e shell\u003csup\u003e[\u003cspan additionalcitationids=\"CR15\" citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]\u003c/sup\u003e, promoting the production of low-boiling point AlF\u003csub\u003e3\u003c/sub\u003e substances. Therefore, fluorine-containing compounds such as polytetrafluoroethylene (PTFE)\u003csup\u003e[\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e]\u003c/sup\u003e, polyvinylidene fluoride (PVDF)\u003csup\u003e[\u003cspan additionalcitationids=\"CR20 CR21\" citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]\u003c/sup\u003e, perfluoric acid\u003csup\u003e[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]\u003c/sup\u003e, and ammonium perfluorooctanoate (APFO)\u003csup\u003e[\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]\u003c/sup\u003e etc. are used to improve the combustion performance of aluminum powder. Although some studies have shown that fluorine-containing compounds can be effectively combined with aluminum powder by ball milling, this changes the original spherical morphology of aluminum powder and limits its application in propellants\u003csup\u003e[\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]\u003c/sup\u003e. In addition, the physical method of directly mixing fluorine-containing compounds and aluminum powder and adding them to solid propellants does not allow the fluorine-containing compounds to fully contact with the aluminum powder. Therefore, how to modify the surface of aluminum powder by directly coating fluorine-containing compounds on the surface of aluminum powder particles so that the fluorine-containing compounds and aluminum powder are in full contact without changing the morphology of aluminum powder, thereby changing the combustion performance of aluminum, has always been a research hotspot. At present, some studies have coated some materials (PTFE, PVDF, polydopamine (PDA), etc.) on the surface of aluminum powder particles to improve the combustion performance of aluminum powder. However, the method of coating the surface of aluminum powder also has many problems: the preparation method is complicated, the raw materials or preparation method are expensive, and the preparation process is difficult to control.\u003c/p\u003e \u003cp\u003eAnother important component in composite propellants is the oxidizer ammonium perchlorate (AP). The combustion performance of composite propellants is closely related to the thermal decomposition process of AP. The ignition delay time of the propellant can be shortened and the combustion rate can be increased by reducing the peak temperature of AP decomposition\u003csup\u003e[\u003cspan additionalcitationids=\"CR29 CR30\" citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]\u003c/sup\u003e. A large number of studies have shown that transition metal ion salts or transition metal ion compounds can effectively reduce the thermal decomposition temperature of AP\u003csup\u003e[\u003cspan additionalcitationids=\"CR34\" citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]\u003c/sup\u003e. However, these often require complex methods or specialized equipment to prepare.\u003c/p\u003e \u003cp\u003eTherefore, in this work, we propose a novel interfacial engineering strategy that concurrently addresses the dual challenges of the inert Al₂O₃ shell and the poor interfacial compatibility. We successfully constructed a dual core-shell structured Al@TA-Fe@PDTTS composite. The design philosophy is twofold: the inner TA-Fe network, formed via the facile self-assembly of low-cost tannic acid and Fe\u0026sup3;⁺ ions, is engineered to interact strongly with the native alumina layer and serve as a catalytic site. The outer fluorosilane (PDTTS) layer is designed to confer superior hydrophobicity and, upon decomposition, provide reactive fluorine species that corrode the oxide shell and promote its cracking. This rational design, verified by molecular dynamics simulations, not only ensures a robust coating architecture but also synergistically enhances both the reactivity and interfacial properties of aluminum. This work provides a new insight into the molecular-level interface control for designing advanced multifunctional metal fuels, offering a simple and effective pathway towards high-performance energetic composites.\u003c/p\u003e"},{"header":"2. Experimental section","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Materials\u003c/h2\u003e \u003cp\u003eAluminum powder was supplied by Hengda Aluminum Co., Ltd. (median particle size D\u003csub\u003e50\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;5 \u0026micro;m). Ammonium perchlorate was purchased from Liming Research Institute of Chemical Industry. Tannic acid (98%), 1H,1H,2H,2H-Perfluorodecyltriethoxysilane (PDTTS) (98%), FeCl\u003csub\u003e3\u003c/sub\u003e\u0026middot;6H\u003csub\u003e2\u003c/sub\u003eO (99%),and n-Hexane (\u0026ge;\u0026thinsp;98%), Tris-Bis (99.5% purity), were purchased from Shanghai Macklin Biochemical Co., Ltd. Absolute ethanol (\u0026ge;\u0026thinsp;99.7%) was obtained from Shanghai Energy Chemical Co., Ltd. All chemicals are analytical grade.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Synthesis of Al@TA-Fe Composite\u003c/h2\u003e \u003cp\u003eThe Al@TA-Fe composite was fabricated via a facile one-pot coordination-driven self-assembly process. In a typical procedure, 0.4 g of TA was first dissolved in 200 mL of deionized water under magnetic stirring to form a clear solution. Subsequently, 2 g of raw Al powder was introduced into the TA solution and uniformly dispersed via ultrasonication for 10 min. Then, 20 mL of an aqueous FeCl₃\u0026middot;6H₂O solution (0.065 g) was added dropwise into the mixture, which was allowed to react for 20 min. This step facilitates the rapid formation of a coordinated TA-Fe network on the Al surface. The pH of the reaction system was then adjusted to 8.0 using a Tris-Bis buffer solution to optimize the coordination environment and enhance the adhesion of the network. The resulting product was collected by filtration, thoroughly washed with deionized water, and dried overnight at ambient temperature to yield the Al@TA-Fe powder.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Construction of the Dual Core-Shell Structure (Al@TA-Fe@PDTTS)\u003c/h2\u003e \u003cp\u003eTo impart hydrophobicity and introduce reactive fluorine species, the as-prepared Al@TA-Fe composite was further functionalized with PDTTS. Briefly, 10 g of Al@TA-Fe was fully dispersed in 100 mL of n-hexane via ultrasonication. Then, 1 g of PDTTS was added dropwise into the suspension. The mixture was left to stand for 24 h, allowing the silane groups of PDTTS to condense with the residual hydroxyl groups on the TA-Fe surface, forming a robust covalent interface. The final product, denoted as Al@TA-Fe@PDTTS, was obtained by filtration, washed three times with n-hexane to remove unreacted precursors, and dried at 50\u0026deg;C. A schematic illustration of the overall fabrication process is presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e.The macroscopic morphologies of pure Al powder and A are shown in Fig.S1.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e2.4 Characterization and Methods\u003c/h2\u003e \u003cp\u003eThe sample was observed using a ZEISS Sigma 300 scanning electron microscope (SEM) and a Tecnai G2 F30 S-TWIN transmission electron microscope (TEM). Powder X-ray diffraction (PXRD) was performed on a Panaco Emoyrean instrument using a Cu target, scanning from 5\u0026deg; to 90\u0026deg; at 10\u0026deg;\u0026middot;min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Fourier transform infrared spectrometer (FT-IR) was performed using a Thermo Scientific Nicolet iS20 instrument. The test range is 4000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e to 400 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. X-ray Photoelectron Spectroscopy (XPS) was performed using a Thermo Scientific K-Alpha. The spot size is 400 \u0026micro;m, the working voltage is 12 kV, the filament current is 6 mA; the full spectrum scanning energy is 150 eV, and the step size is 1 eV. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) were performed on a Mettler Toledo -TGA/DSC 3\u0026thinsp;+\u0026thinsp;with the heating rate of 10 K\u0026middot;min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (or 20 K\u0026middot;min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) in the Ar atmosphere. The static contact angle was measured by the hypsometry method using the standard static drop method, using the JY-82B Kruss DSA type contact angle meter.\u003c/p\u003e \u003cp\u003eTo investigate the combustion products of the sample in an air atmosphere, 200 mg of the sample was placed in a transparent tube furnace (air atmosphere), heated to 600 ℃ (or 800 ℃) at a rate of 20 ℃\u0026middot;min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and kept warm for 10 min. The reaction products were collected after cooling to room temperature and characterize them by SEM and XRD.\u003c/p\u003e \u003cp\u003eTRHW-7000C automatic oxygen bomb calorimeter was used to test the combustion calorific value of the sample. The combustion calorific value of each sample is measured in parallel three times, and the average value is taken as the final result. In high-speed photography experiments, Al and Al@TA-Fe@PDTTS was physically uniformly mixed with AP in a mass ratio of 9:1. Then, 100 mg of the sample was placed on the ignition platform and the sample was ignited using a CO\u003csub\u003e2\u003c/sub\u003e laser ignition system with an output power of 30 W and a duration of 500 ms under air atmosphere and atmospheric pressure conditions. After the mixed sample was ignited, the combustion process of the sample was recorded using a high-speed camera with a shooting rate of 10000 fps and an exposure time of 50 ms.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e2.5 Model calculations and calculation conditions for molecular simulation experiments\u003c/h2\u003e \u003cp\u003eIn this study, the aim was to evaluate the binding ability between Al, TA and PDTTS by molecular dynamics simulation and to prove the rationality of this experimental design. The molecular structures of Al, TA and PDTTS were established using the Visualizer module in the Materials Studio software package, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(a), Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(b) and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(c), respectively. Based on the original molecular structure, Al was expanded into a 4\u0026times;4\u0026times;2 supercell, and 3D periodic boxes of 12 TA molecules and 30 PDTTS molecular chains were constructed using the Amorphous Cell module, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(d), Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(e) and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(f), respectively. The structures and molecular dynamics simulations of the Al/TA, Al/PDTTS, and Al/TA/PDTTS molecular models were optimized using the Forcite module. COMPASS Ⅱ was used as the force field, NVT as the ensemble, the temperature was set to 298 K, the time step was 0.1 fs, the total simulation time was 1000 ps, and the last 500 ps of data were used for subsequent performance analysis.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"3 Result and discussion","content":"\u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003e3.1. Binding energy\u003c/h2\u003e \u003cp\u003eBinding energy is an important parameter that reflects the magnitude of intermolecular interaction forces and can reflect the strength of different intermolecular interactions\u003csup\u003e[\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e]\u003c/sup\u003e. Binding energy (E\u003csub\u003ebind\u003c/sub\u003e) can be defined as the negative value of intermolecular interaction energy (E\u003csub\u003einter\u003c/sub\u003e). Intermolecular interaction energy can be calculated from the total energy of each component in the equilibrium state of the mixed system, as shown in Eq.\u0026nbsp;(1):\u003c/p\u003e \u003cp\u003eE\u003csub\u003ebind\u003c/sub\u003e=-E\u003csub\u003einter\u003c/sub\u003e=-(E\u003csub\u003eA\u0026minus;B\u003c/sub\u003e-E\u003csub\u003eA(A\u0026minus;B)\u003c/sub\u003e-E\u003csub\u003eB(A\u0026minus;B)\u003c/sub\u003e) (1)\u003c/p\u003e \u003cp\u003eIn Eq.\u0026nbsp;(1), E\u003csub\u003eA\u0026minus;B\u003c/sub\u003e represents the total energy of the composite system; E\u003csub\u003eA(A\u0026minus;B)\u003c/sub\u003e represents the energy of A in the composite system, and E\u003csub\u003eB(A\u0026minus;B)\u003c/sub\u003e represents the energy of B in the composite system.\u003c/p\u003e \u003cp\u003eFor a system to reach dynamic equilibrium, it is usually necessary to make the temperature and energy in the system reach equilibrium. In general, as long as the temperature and energy remain within the fluctuation range of 5% to 10%, it can be concluded that dynamic equilibrium has been achieved\u003csup\u003e[\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e]\u003c/sup\u003e. Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e shows the fluctuation curves of temperature (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea-c) and energy (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed-f) during the molecular dynamics simulation of the systems Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS, and Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e@TA/PDTTS. As time goes by, after 500ps, the fluctuations of the temperature and energy of the system are within 5%, and the system reaches equilibrium. The above results show that all simulation systems have reached dynamic equilibrium, which ensures the reliability of subsequent data collection and analysis.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(a-d), Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(b-e) and Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(c-f) show the optimized model diagrams and final equilibrium structure diagrams of the mixed molecular systems Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS and A\u003csub\u003el2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA/PDTTS, respectively. The binding energy calculation results of each system are shown in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. The binding energies of the systems Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS and Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e@TA/PDTTS are 782.36 kcal\u0026sdot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 211.79 kcal\u0026sdot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 498.21 kcal\u0026sdot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. The results show that TA molecules have good bonding ability with Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, which explains why the TA interface layer can be well coated on the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e surface, which is mainly due to the formation of hydrogen bonds between the H atoms in the TA molecules and the O atoms in the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e. At the same time, the binding ability of PDTTS with TA is also much higher than that of PDTTS with Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e. This is mainly because the F atoms in PDTTS are more likely to form hydrogen bonds with the -OH in TA, making the binding ability between them stronger. The above results show that the binding ability of TA with the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e crystal surface is better than that of PDTTS. For PDTTS, its binding ability on the TA surface layer is also significantly better than that of Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e particles. The results of simulation calculations show the rationality of the experimental design.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eBinding energies of Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA, Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS and Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e@TA/PDTTS\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"4\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eSystem\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eAl\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/TA,\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAl\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e/PDTTS\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eAl\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e@TA/PDTTS\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBinding energy (kcal\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e782.36\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e211.79\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e498.21\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec10\" class=\"Section2\"\u003e \u003ch2\u003e3.2. Characterization of Al@TA-Fe@PDTTS\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e shows the microscopic morphology of each sample. As can be seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(a) and Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(c), the surfaces of pure Al particles and Al@PDTTS are smooth. The SEM image of Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(b) shows that the surfaces of Al@TA-Fe particles and Al@TA-Fe@PDTTS are rougher than those of pure Al particles and Al@PDTTS particles. It can be clearly observed from the magnified image that many protrusions are formed on the surface of the aluminum particles, which is caused by the different thickness of the TA-Fe coating layer. Figure\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(e) is the EDS spectrum of the surface of Al@TA-Fe@PDTTS particles. Compared with Al powder, the surface layer of Al@TA-Fe@PDTTS contains C, Fe, Si and F elements, confirming that the TA-Fe and PDTTS interface layer are successfully established.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIn order to further study the coating of TA-Fe layer and PDTTS layer on the surface of aluminum powder, TEM morphology detection and EDS surface scanning test were carried out on the Al@TA-Fe@PDTTS sample, and the results are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e. As can be seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e(a) and Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e(b), there is an irregularly shaped coating layer on the surface of the aluminum powder particles. Combining the high-resolution image of the edge of a single particle and the element energy spectrum surface scanning image, it can be found that the surface of the Al@TA-Fe@PDTTS particle is roughly divided into three regions. The black part in the center is the Al core, the dark gray ring area is the aluminum oxide layer, and the TA-Fe and PDTTS coating layers are outside the aluminum oxide. According to Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e(b-e), it can be found that the TA-Fe and PDTTS layers are relatively uniformly dispersed on the surface of the aluminum powder particles. The above results successfully prove the core-shell structure of Al@TA-Fe@PDTTS.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIn order to further explore the surface of Al@TA-Fe@PDTTS particles, FT-IR analysis was performed, as shown in Fig. S2. The diffraction peak at 822 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e can be attributed to the asymmetric stretching vibration peak of -CF\u003csub\u003e2\u003c/sub\u003e, and the peak at 1055 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e is the characteristic absorption peak of Si-O-C in the PTTDS molecule\u003csup\u003e[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]\u003c/sup\u003e. The peak at 1193 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e is the stretching vibration peak of the ester group in TA\u003csup\u003e[\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]\u003c/sup\u003e. The peak at 1336 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e is the C-O stretching vibration peak in the TA molecule. The peaks at 1572 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 1431 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e can be attributed to the C-C stretching vibration of the benzene ring in the TA molecule. The peak at 1689 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e belongs to the C\u0026thinsp;=\u0026thinsp;O stretching vibration peak in the TA molecule. The peak at 2937 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e belongs to the asymmetric stretching vibration absorption peak of the C-H bond in PDTTS, and the peak at 3351 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e can be attributed to the vibration peak of the hydroxyl group in TA. The FT-IR results show that the characteristic peaks of TA and PDTTS exist on the surface of Al@TA-Fe@PDTTS particles. This result also proves that the TA-Fe coating layer and the PDTTS coating layer are successfully coated on the surface of the aluminum powder particles.\u003c/p\u003e \u003cp\u003eIn addition, XPS was used to measure and characterize the element types and valence states on the surface of Al@TA-Fe@PDTTS particles, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e. The full XPS spectrum of Al@TA-Fe@PDTTS shows that the surface layer of Al@TA-Fe@PDTTS contains C, O and F elements (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea), while the Al peak is not clearly detected. This may be because the surface layer of the aluminum particles is covered by the TA-Fe@PDTTS coating layer, which affects the detection of the internal aluminum element. At the same time, the detection of the Fe element is not obvious, which is mainly due to the low content of Fe in Al@TA-Fe@PDTTS. Figure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e(b-d) shows the high-resolution XPS spectra of C, O and F elements. The spectrum of the C element can be divided into five peaks, namely the C-H peak at 284.3 eV, the C-C peak at 286.0 eV, the O-C\u0026thinsp;=\u0026thinsp;O peak at 287.9 eV, the -CF\u003csub\u003e2\u003c/sub\u003e peak at 291.0 eV and the -CF\u003csub\u003e3\u003c/sub\u003e peak at 293.3 eV\u003csup\u003e[\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e]\u003c/sup\u003e. The peak of the O element can be fitted by two peaks, the peak of 531.0 eV is attributed to the oxygen atom of C-O-C in TA, and the peak of 532.6 eV is attributed to the oxygen atom of -OH. In the XPS spectrum of the F element, the peak at 688.7 eV can be attributed to the peak of the F atom in C-F. The above results further show that Al@TA-Fe@PDTTS has a dual core-shell structure.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec11\" class=\"Section2\"\u003e \u003ch2\u003e3.3 Interface performance of Al@TA-Fe@PDTTS\u003c/h2\u003e \u003cp\u003eIn order to observe the interfacial properties of Al and Al@TA-Fe@PDTTS, the contact between Al and Al@TA-Fe@PDTTS and water was studied in detail, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e8\u003c/span\u003e. Pure Al gradually settles to the bottom of the water after being added to the water, and is dispersed in the water to form a suspension after vigorous shaking. In contrast, Al@TA-Fe@PDTTS float directly on the water after being added to water. Even after violent shaking, Al@TA-Fe@PDTTS can still float on the water. This result shows that the surface property of Al@TA-Fe@PDTTS has changed significantly relative to pure Al, In addition, it can also be concluded that the coating of Al@TA-Fe by PDTTS is dense.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIn addition, the static contact angles of the samples with water were tested, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e8\u003c/span\u003e. The average static contact angle of pure Al with water is only 21.0\u0026deg;, while the average static contact angles of Al@TA-Fe@PDTTS and Al@PDTTS with water can reach 123.7\u0026deg; and 83.9\u0026deg;, respectively. Even after 30 days in water, the average static contact angles of Al@TA-Fe@PDTTS and Al@PDTTS can still reach 102.7\u0026deg; and 73.3\u0026deg;. The contact angle of Al@TA-Fe@PDTTS with water is always larger than that of Al@PDTTS, which also shows that using TA-Fe as the intermediate layer can make PDTTS better coated on the surface of aluminum powder. These results indicate that the surface layer of aluminum particles is covered with hydrophobic C and F elements, which also reflects that Al@TA-Fe@PDTTS has better hydrophobicity and corrosion resistance than pure aluminum powder\u003csup\u003e[\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec12\" class=\"Section2\"\u003e \u003ch2\u003e3.4 Thermal reaction properties of Al@TA-Fe@PDTTS\u003c/h2\u003e \u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig9\" class=\"InternalRef\"\u003e9\u003c/span\u003e shows the DSC/TG curves of Al and Al@TA-Fe@PDTTS in an argon atmosphere. In the temperature range of 0-800\u0026deg;C, pure aluminum powder has a melting endothermic peak at 660\u0026deg;C and no weight loss process. The DSC curve of Al@TA-Fe@PDTTS shows that the peak at 327.7\u0026deg;C is the decomposition peak of TA, followed by a small exothermic peak for the decomposition peak of PDTTS; the peak at 660\u0026deg;C is the characteristic endothermic peak of aluminum. The peak at 653\u0026deg;C is the redox exothermic peak generated by the reaction between aluminum and the decomposition products of TA and PDTTS coating. The TG curve of Al@TA-Fe@PDTTS shows that it gradually decomposes and loses weight from 110\u0026deg;C, which is mainly caused by the thermal decomposition of TA. Al@TA-Fe@PDTTS begins to lose weight rapidly when the temperature reaches about 300\u0026deg;C, which is mainly due to the continuous decomposition of TA and the thermal decomposition of PDTTS\u003csup\u003e[\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e]\u003c/sup\u003e. The thermal weight loss process of Al@TA-Fe@PDTTS basically ends at around 510\u0026deg;C, and reaches the maximum thermal weight loss at 550\u0026deg;C, with a weight loss of about 25 wt%. It then undergoes a short weight gain process between 610\u0026deg;C and 655\u0026deg;C, corresponding to the redox exothermic peak at 653\u0026deg;C in the DSC curve. The results show that the sample Al@TA-Fe@PDTTS has begun to react before the melting point of aluminum, and the heat released by the reaction can promote the internal aluminum oxidation reaction. Pure aluminum powder cannot react at 660\u0026deg;C.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003ein the Ar atmosphere.\u003c/p\u003e \u003cp\u003eIn addition, the combustion performance of Al and Al@TA-Fe@PDTTS in air was studied. Aluminum powder was reacted with Al@TA-Fe@PDTTS at different temperatures (600\u0026deg;C and 800\u0026deg;C) in air atmosphere for 10 min, and the combustion products were collected and analyzed. Figure\u0026nbsp;\u003cspan refid=\"Fig10\" class=\"InternalRef\"\u003e10\u003c/span\u003e shows the SEM images of pure aluminum powder after reaction at 600\u0026deg;C and 800\u0026deg;C in air. The morphology of most aluminum particles in the reaction products of pure aluminum powder at 600\u0026deg;C did not change significantly, and they showed a regular spherical morphology. At 800\u0026deg;C, only a very small part of the aluminum powder underwent a typical shell-breaking reaction, while most of the aluminum powder still showed a complete and regular spherical morphology. Therefore, even at high temperatures, pure aluminum powder is difficult to completely oxidize in air. However, the morphology of a part of the Al@TA-Fe@PDTTS reaction products changed dramatically at 600\u0026deg;C, forming irregular fragments instead of spherical aluminum particles. When the temperature was increased to 800\u0026deg;C, this proportion increased significantly, forming a large number of irregular fragments. This indicates that Al@TA-Fe@PDTTS can react below the melting point of aluminum (660\u0026deg;C) and that the TA-Fe@PDTTS dual interface layer can promote the oxidation reaction of aluminum.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e800 ◦C in the air atmosphere; (c) and (f) magnified images of the corresponding reaction products of Al and Al@TA-Fe@PDTTS at 800 ◦C.\u003c/p\u003e \u003cp\u003eThe combustion products of Al@TA-Fe@PDTTS were analyzed by XRD, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig11\" class=\"InternalRef\"\u003e11\u003c/span\u003e. The test results show that the combustion products are mainly A\u003csub\u003el2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, a small amount of AlF\u003csub\u003e3\u003c/sub\u003e and incompletely reacted Al. The above results show that the fluorine element decomposed in the PDTTS coating layer participates in the oxidation reaction of aluminum. The porous structure of AlF\u003csub\u003e3\u003c/sub\u003e not only increases the contact area between Al and the external oxidant, but also promotes the diffusion of Al through the porous channels, promoting the release of energy and the combustion kinetics reaction\u003csup\u003e[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]\u003c/sup\u003e. The above results all show that the Al@TA-Fe@PDTTS dual coating can greatly promote the oxidation reaction of aluminum, and can even catalyze the oxidation reaction of aluminum under conditions below the melting point of aluminum\u003csup\u003e[\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e, \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e, \u003cspan citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eBased on the above experimental results, the thermal reaction mechanism of Al@TA-Fe@PDTTS during heating is proposed. As the temperature rises, the TA layer and PDTTS layer on the surface of Al@TA-Fe@PDTTS release strong oxidizing free radicals such as F\u0026middot; and C\u003csub\u003eX\u003c/sub\u003eF\u0026middot; during the thermal decomposition process. They react with the oxygen in the environment through the cracks and gaps in the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e shell and the Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e film on the surface of the aluminum powder, corroding the aluminum oxide film to form AlF\u003csub\u003e3\u003c/sub\u003e. The evaporation point of AlF\u003csub\u003e3\u003c/sub\u003e is lower than that of aluminum oxide, and it is easier to volatilize from the surface of the aluminum powder, thereby exposing the internal aluminum and reacting with the external oxygen\u003csup\u003e[\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]\u003c/sup\u003e. This explains why the reaction degree of Al@TA-Fe@PDTTS is higher than that of pure Al.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec13\" class=\"Section2\"\u003e \u003ch2\u003e3.5 Effect of Al@TA-Fe@PDTTS on catalytic thermal decomposition of AP\u003c/h2\u003e \u003cp\u003eIn order to study the catalytic decomposition of AP by Al@TA-Fe@PDTTS, Al@TA-Fe@PDTTS and AP were mixed at a mass ratio of 9:1, and then Al@TA-Fe@PDTTS/AP and AP were performed DSC analysis in an Ar atmosphere., as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig12\" class=\"InternalRef\"\u003e12\u003c/span\u003e. It can be seen from the DSC curve that Al@TA-Fe@PDTTS/AP and AP have one endothermic peak and two exothermic peaks. The endothermic peak at 247\u0026deg;C is formed by the transformation of AP from an orthorhombic structure to a cubic structure. After adding Al@TA-Fe@PDTTS, the high temperature decomposition peak of AP dropped from 422.3 ◦C to 380.4 ◦C. In addition, the exothermic peak of the high-temperature decomposition stage of AP in Al@TA-Fe@PDTTS/AP is much larger than that of pure AP, which may be due to two reasons. One is that the decomposition temperature range of TA-Fe@PDTTS coincides with the high-temperature decomposition range of AP, and the other is that the TA-Fe layer significantly improves the thermal decomposition stage of AP. The results show that Al@TA-Fe@PDTTS can significantly reduce the peak temperature of high-temperature decomposition of AP.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eK\u0026middot;min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e in the Ar atmosphere.\u003c/p\u003e \u003cp\u003eThe heat release of combustion is an important parameter for measuring the energy materials. The energy release level of energetic materials can be intuitively seen through the combustion heat value. The combustion heat of Al/AP and Al@TA-Fe@PDTTS/AP mixtures was measured under different oxygen pressures (3 MPa, 2 MPa, 1 MPa, and 0.5 MPa) using an oxygen bomb calorimeter. Each sample was measured three times and the average value was taken. The results are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig13\" class=\"InternalRef\"\u003e13\u003c/span\u003e. It can be found that when the oxygen pressure dropped from 3 MPa to 1 MPa, the combustion heat values of both samples decreased slightly. Under the same oxygen pressure, the combustion heat value of Al@TA-Fe@PDTTS/AP is always slightly higher than that of Al/AP. This is because although the composite structure can promote heat and mass transfer\u003csup\u003e[\u003cspan citationid=\"CR45\" class=\"CitationRef\"\u003e45\u003c/span\u003e]\u003c/sup\u003e, since the combustion of aluminum powder in an oxygen-rich environment is relatively complete, the introduction of TA-Fe and PDTTS coatings has limited effect on the improvement of the combustion heat value of Al. When the oxygen pressure drops from 1 MPa to 0.5 MPa, the combustion heat value of the Al/AP and Al@TA-Fe@PDTTS/AP mixtures decreases significantly from 25.716 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 26.027 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (the difference between the two is 0.311 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) to 22.331 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 23.728 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e (the difference between the two is 1.397 kJ\u0026middot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e). The above results show that the coating layer on the surface of aluminum powder has a more significant effect on the combustion of aluminum powder in a low-oxygen environment, which also confirms our previous analysis of the thermal decomposition mechanism of Al@TA-Fe@PDTTS during heating.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIgnition delay time is one of the indicators of ignition reliability and one of the important factors affecting the tactical performance and accuracy of energetic materials and equipment. The ignition delay time here is defined as the time delay required for the sample to ignite and burn normally after receiving laser energy stimulation. In the laser ignition experiment, the time difference between the appearance of the laser signal and the appearance of the sample ignition signal is identified as the ignition delay time. The results are shown in Fig. S3. The ignition delay times of Al/AP and Al@TA-Fe@PDTTS/AP are 13.2 ms and 4.8 ms, respectively. The introduction of TA-Fe and PDTTS coating layers can effectively shorten the ignition delay time of the mixture.\u003c/p\u003e \u003cp\u003eThe combustion process of Al/AP and Al@TA-Fe@PDTTS/AP is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig14\" class=\"InternalRef\"\u003e14\u003c/span\u003e. The combustion time of the Al/AP mixture is 250 ms, while the combustion time of the Al@TA-Fe@PDTTS/AP mixture exceeds 500 ms. Comparing the combustion of the two samples, in the combustion process of the Al/AP mixture, the intense combustion lasts for a shorter time and the flame formed is smaller. The combustion of the Al@TA-Fe@PDTTS/AP mixture is more intense, the combustion area formed is larger, and the intense combustion lasts for a longer time. Compared with Al/AP, Al@TA-Fe@PDTTS/AP starts to burn violently earlier and forms more sparks. The above results show that the composite structure of Al@TA-Fe@PDTTS has a larger contact area, which is conducive to heat and mass transfer, resulting in a faster combustion response of the mixture and a higher degree of combustion.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"4. Conclusion","content":"\u003cp\u003eIn this paper, an aluminum-based composite material Al@TA-Fe@PDTTS with a dual core-shell structure was successfully prepared. The morphology and component characterization show that both TA-Fe and PDTTS are uniformly coated on the surface of aluminum particles, and Al@TA-Fe@PDTTS has better hydrophobicity than pure aluminum powder. The molecular dynamics calculation results show that the binding energy between PDTTS and TA is 498.21 kcal\u0026sdot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, while the binding energy between TA and Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e reaches 782.36 kcal\u0026sdot;mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, which provids a theoretical basis for the establishment of the dual coating layer. In addition, the TA-Fe@PDTTS dual coating layer can change the reaction process of aluminum in air atmosphere, so that aluminum reacts below the melting point. When mixed with AP, the presence of Al@TA-Fe@PDTTS can reduce the peak temperature of AP's high-temperature decomposition by 41.9 ℃. Moreover, the combustion heat value of the Al@TA-Fe@PDTTS/AP mixture is always higher than that of Al/AP, especially in a low oxygen pressure environment. Combustion experiments show that Al@TA-Fe@PDTTS/AP has a faster combustion response and a higher degree of combustion than Al/AP, and the ignition delay time is reduced from 13.2 ms to 4.8 ms.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eDeclaration of competing interest\u003c/strong\u003e\u003c/p\u003e\n\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.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFunding\u003c/strong\u003e\u003cbr\u003e\u0026nbsp;This work was supported by the National Natural Science Foundation of China [grant number 22175026].\u003c/p\u003e\n\u003cp\u003eRole of the funding source：\u0026nbsp;The funding agency had no role in the study design, collection, analysis, interpretation of data, writing of the manuscript, or decision to submit it for publication.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCredit authorship contribution statement\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eBo Liu:\u0026nbsp;\u003c/strong\u003eMethodology, Data curation, Formal analysis, Writing-original draft, Writing-review \u0026amp; editing. \u003cstrong\u003eXiaodong Gou:\u0026nbsp;\u003c/strong\u003eFormal analysis, Data curation. \u003cstrong\u003eYingjun Li:\u0026nbsp;\u003c/strong\u003eConceptualization. \u003cstrong\u003eJiahao Liang:\u0026nbsp;\u003c/strong\u003eData curation. \u003cstrong\u003eShi Yan:\u0026nbsp;\u003c/strong\u003eProject administration. \u003cstrong\u003eXueyong Guo:\u003c/strong\u003e Resources,\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003eProject administration.\u003cstrong\u003e\u0026nbsp;Jianxin Nie:\u0026nbsp;\u003c/strong\u003eInvestigation, Resources, Project administration.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors thank National Natural Science Foundation of China [grant number 22175026] for technical assistance.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eData will be made available on request.\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eTrache, D., Maggi, F., Palmucci, I. \u0026amp; DeLuca, L. 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Enhance thermal response behavior of energetic composite by doping fluorinated graphene. \u003cem\u003eCombust. Flame\u003c/em\u003e. \u003cb\u003e265\u003c/b\u003e, 113484 (2024).\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":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"scientific-reports","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"scirep","sideBox":"Learn more about [Scientific Reports](http://www.nature.com/srep/)","snPcode":"","submissionUrl":"","title":"Scientific Reports","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Scientific Reports","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"aluminum powder, dual core-shell structure, interface performance, combustion, ammonium perchlorate","lastPublishedDoi":"10.21203/rs.3.rs-8316616/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8316616/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eConstructing a multifunctional coating on aluminum (Al) powder is crucial for enhancing its energy release in propellants. However, existing methods face challenges such as complex processes, high costs, and poor controllability. This study proposes a simple self-assembly strategy to construct a dual core-shell structure on aluminum powder surfaces, consisting of an inner tannic acid-Fe\u0026sup3;⁺ (TA-Fe) network and an outer fluorosilane (PDTTS) layer, thus successfully fabricating the Al@TA-Fe@PDTTS composite. Molecular dynamics simulations reveal a strong binding energy among the coating components, providing theoretical support for the successful realization of the self-assembly process. The resulting Al@TA-Fe@PDTTS composite exhibits excellent hydrophobicity (contact angle up to 123.7\u0026deg;) and significantly promotes the cracking of the inert alumina shell. Serving as a combined fuel and catalyst, the composite significantly lowers the high-temperature decomposition peak of ammonium perchlorate (AP) by 41.9\u0026deg;C. Furthermore, laser ignition tests confirm a substantially shortened ignition delay (from 13.2 ms for aluminum/AP mixtures to only 4.8 ms for the composite material) and a more intense combustion process, highlighting its great potential for advanced energetic applications.\u003c/p\u003e","manuscriptTitle":"Interfacial Engineering of Aluminum Powder with a Tannic Acid/Fe³⁺ Complex and Fluorosilane for High-Performance Energetic Composites","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-12-18 12:56:26","doi":"10.21203/rs.3.rs-8316616/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2026-01-19T08:08:04+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-01-12T15:55:43+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"247585419352814600191569171266167849590","date":"2026-01-05T15:26:06+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2026-01-02T08:23:34+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"219891919763525222908096515235647848340","date":"2025-12-29T08:32:03+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"173345584830046128188432865360155160558","date":"2025-12-18T13:51:21+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-12-17T12:25:19+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"161342314548270414265959916868045642644","date":"2025-12-17T05:54:13+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2025-12-16T12:00:58+00:00","index":"","fulltext":""},{"type":"editorInvited","content":"","date":"2025-12-16T07:48:19+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2025-12-12T01:11:14+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2025-12-12T01:10:50+00:00","index":"","fulltext":""},{"type":"submitted","content":"Scientific Reports","date":"2025-12-09T10:25:46+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"scientific-reports","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"scirep","sideBox":"Learn more about [Scientific Reports](http://www.nature.com/srep/)","snPcode":"","submissionUrl":"","title":"Scientific Reports","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Scientific Reports","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"bd9e2aa6-7434-499a-8ac4-f9c7b9d8ba44","owner":[],"postedDate":"December 18th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":59818498,"name":"Physical sciences/Chemistry"},{"id":59818499,"name":"Physical sciences/Engineering"},{"id":59818500,"name":"Physical sciences/Materials science"}],"tags":[],"updatedAt":"2026-03-09T16:14:02+00:00","versionOfRecord":{"articleIdentity":"rs-8316616","link":"https://doi.org/10.1038/s41598-026-43316-y","journal":{"identity":"scientific-reports","isVorOnly":false,"title":"Scientific Reports"},"publishedOn":"2026-03-07 15:58:59","publishedOnDateReadable":"March 7th, 2026"},"versionCreatedAt":"2025-12-18 12:56:26","video":"","vorDoi":"10.1038/s41598-026-43316-y","vorDoiUrl":"https://doi.org/10.1038/s41598-026-43316-y","workflowStages":[]},"version":"v1","identity":"rs-8316616","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8316616","identity":"rs-8316616","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}