Integrated coating material based on moisture absorption prevention and synergistic energy release as well as preparation method and application of integrated coating material

Abstract

The invention relates to the technical field of solid propellants, in particular to an integrated coating material based on moisture absorption prevention and synergistic energy release as well as a preparation method and application of the integrated coating material. The ternary core-shell structure sequentially comprises an ammonium dinitramide core, an energy-containing covalent organic framework middle layer and a polytetrafluoroethylene nano-film outer layer from inside to outside, and the energy-containing covalent organic framework middle layer is combined with the surface of the ammonium dinitramide core through hydrogen bonds or p-pi conjugation; and the polytetrafluoroethylene nano-film outer layer coats the outer side of the energetic covalent organic framework middle layer in a continuous nano-scale film form. The problems that in the prior art, ADN is high in hygroscopicity and energy-containing characteristics are reduced due to a traditional coating technology are solved, long-term moisture absorption prevention of ADN is achieved, the long-term stability is improved, and meanwhile the combustion performance of ADN is improved.

Description

Technical Field

[0001] This invention relates to the field of solid propellant technology, and in particular to an integrated coating material based on moisture-proofing and synergistic energy release, its preparation method, and its application. Background Technology

[0002] Ammonium dinitramide (ADN) is a high-energy, pollution-free oxidant that can significantly reduce plume signal and decrease environmental pollution from HCl gas in combustion products. However, as a highly polar ionic compound, the negative charge on the crystal surface of ADN readily binds to water molecules in the air. This strong hygroscopicity limits the further application of ADN. Therefore, how to reduce the hygroscopicity of ADN while ensuring that its energetic properties do not decay has become a key challenge that urgently needs to be overcome to promote the large-scale application of ADN in propellants.

[0003] Currently, there are three main methods commonly used to reduce the hygroscopicity of ADN: ADN spheroidization, eutectic treatment, and surface treatment. Studies by Ma Yue et al. have shown that spheroidization of ADN can reduce its specific surface area, thereby reducing hygroscopicity, but this method cannot fundamentally solve the problem of ADN's hygroscopicity. Hu Yifei et al. calculated that the total saturated hygroscopicity of ADN / α-CD eutectic at 20℃ and 40% relative humidity was only 0.74%, significantly lower than the 15.35% of pure ADN. Eutectic treatment can significantly reduce hygroscopicity, but it also significantly reduces oxygen balance and energy performance. Surface treatment is one of the most commonly used methods to reduce ADN's hygroscopicity. Xu Huixiang et al. coated the surface of ADN with polyurethane; under conditions of around 10℃ and 50%–60% relative humidity, the hygroscopicity of the coated ADN after 30 days of exposure to air was only 0.136%. Rahman et al. used PS and HPTB to coat ADN, controlling the hygroscopicity of ADN below 30%, but the heat of decomposition of the composite energetic material showed a significant reduction.

[0004] Traditional moisture-proofing processes (such as spheroidization, eutectic, and physical coating) can block moisture in the short term, but they generally face difficulties such as insufficient long-term stability, energy density loss, or poor interfacial compatibility, making it difficult to meet the integrated requirements of the new generation of propellants for high-energy oxidizers: "high energy-low sensitivity-long storage". Summary of the Invention

[0005] The purpose of this invention is to provide an integrated coating material based on moisture resistance and synergistic energy release, its preparation method and application, to solve the problems of strong moisture absorption of ADN and the decline in energy content caused by traditional coating processes in the prior art, to achieve long-term moisture resistance of ADN, improve long-term stability, and improve the combustion performance of ADN.

[0006] To achieve the above objectives, the present invention provides an integrated coating material based on moisture resistance and synergistic energy release. The coating material has a ternary core-shell structure, which consists of an ammonium dinitramide (ADN) core, an energetic covalent organic framework (ECOF) intermediate layer, and a polytetrafluoroethylene (PTFE) nanofilm outer layer from the inside out. The energetic covalent organic framework intermediate layer is bonded to the surface of the ammonium dinitramide core through hydrogen bonds or p-π conjugation. The polytetrafluoroethylene nanofilm outer layer is coated on the outside of the energetic covalent organic framework intermediate layer in the form of a continuous nanoscale thin film.

[0007] Preferably, the energetic covalent organic framework in the intermediate layer includes one of Tp-DHT, Tp-DAT, or Tp-DAAT.

[0008] Preferably, Tp-DHT is generated by reacting 1,3,5-trialdehyde phloroglucinol (Tp) with 3,6-dihydrazino-1,2,4,5-tetraazine (DHT).

[0009] Preferably, Tp-DAT is generated by reacting 1,3,5-trialdehyde phloroglucinol (Tp) with 3,6-diamino-1,2,4,5-tetraazine (DAT).

[0010] Preferably, Tp-DAAT is generated by reacting 1,3,5-trialdehyde phloroglucinol (Tp) with 3,3'-azo-bis(6-amino-1,2,4,5-tetraazine) (DAAT).

[0011] The above-mentioned method for preparing an integrated coating material based on moisture absorption prevention and synergistic energy release includes the following steps:

[0012] S1. After mixing mesitylene, dioxane, and acetic acid, add an energetic monomer, dinitramide ammonium, and 1,3,5-trialdehyde phloroglucinol in sequence under stirring to obtain a mixed solution;

[0013] S2. Transfer the mixed solution to a Schlenk tube and freeze it rapidly in liquid nitrogen. After three freeze-thaw cycles, degas the solution and then purge it with nitrogen gas. Seal the tube and heat it for 2-4 days. Filter and collect the product. Wash the product with deionized water, dioxane, and THF and then dry it for 60-80 hours to obtain ADN@ECOFs.

[0014] S3. A polytetrafluoroethylene nanofilm was coated onto the surface of ADN@ECOFs using a vibration-type magnetron sputtering process to obtain a ternary core-shell structured coating material ADN@ECOFs@PTFE.

[0015] Preferably, in S1, the volume ratio of mesitylene, dioxane, and acetic acid is 0.5-1.5 mL: 2-4 mL: 0.4-0.8 mL;

[0016] The energetic monomer includes one or more of 3,6-dihydrazino-1,2,4,5-tetraazine, 3,6-diamino-1,2,4,5-tetraazine, and 3,3'-azo-bis(6-amino-1,2,4,5-tetraazine), and the molar ratio of the energetic monomer to 1,3,5-trialdehyde phloroglucinol is 0.02-0.04 mmol: 0.01-0.03 mmol.

[0017] Preferably, in S2, the temperature of the heating reaction is 60–100°C.

[0018] Preferably, in S3, the conditions for the vibration-type magnetron sputtering process are: the sputtering power source is an RF power source, argon gas is introduced into the chamber, and the working pressure in the chamber is controlled at 3 × 10⁻⁶. -2 The torr sputtering target cooling water circulation temperature is 18℃, and the vibration frequency is 1000-1300rpm.

[0019] The aforementioned integrated coating material based on moisture-proof and synergistic energy release is applied to high-energy oxidizers for solid propellants.

[0020] Mechanism of the invention:

[0021] This invention utilizes in-situ synthesis and vibrational magnetron sputtering to construct a structurally complete ADN@ECOFs@PTFE ternary core-shell structure, forming a "polarity gradient controlled" (strong polarity → weak polarity → non-polarity) interface transition to achieve synergistic moisture absorption and energy release. ECOFs bind to the ADN surface through hydrogen bonds and π-π conjugation, weakening the ADN surface polarity and reducing water molecule adsorption. Non-polar PTFE uniformly coats the ECOFs, forming a continuous nanofilm that blocks moisture penetration.

[0022] The energetic groups such as tetrazine in ECOFs participate in combustion and release additional energy. The confined pore structure and interlayer staggered arrangement of ECOFs form constraints, which in turn regulate the gas production and heat diffusion dynamics of ADN, forming a "micro-reaction chamber" effect, which allows the combustion pressure to be released in a concentrated manner.

[0023] The chemical combination of ADN and ECOFs accelerates decomposition, while the mechanical constraint of PTFE slows down energy diffusion. The ternary structure works synergistically to improve combustion performance.

[0024] The beneficial effects of this invention are:

[0025] (1) In this invention, ECOFs (including Tp-DHT, Tp-DAT, Tp-DAAT, etc.) were synthesized in situ on the surface of ADN, and a hydrophobic PTFE nanofilm was coated on it using a vibrational magnetron sputtering process. A ternary core-shell structure ADN@ECOFs@PTFE was successfully designed and constructed. This achieved long-lasting hydrophobic and moisture-proof modification of ADN and efficient synergistic energy release.

[0026] (2) The energetic covalent organic framework (ECOFs) of the present invention introduces energetic groups to enable ECOFs to meet the performance requirements of coating materials, so that the coating materials have higher energetic characteristics, faster combustion rate, higher decomposition energy, etc.

[0027] The technical solution of the present invention will be further described in detail below with reference to the accompanying drawings and embodiments. Attached Figure Description

[0028] Figure 1 These are the infrared spectra of ADN, Tp-DHT, ADN@Tp-DHT, and ADN@Tp-DHT@PTFE of the present invention;

[0029] Figure 2 This is a SEM image of the ADN@Tp-DHT of this invention. Figure 2 In the image, 'a' represents the SEM image of ADN@Tp-DHT at a magnification of 10 μm. Figure 2 In the image, b represents the SEM image of ADN@Tp-DHT at a magnification of 500 nm.

[0030] Figure 3 This is the EDS diagram of ADN@Tp-DHT of the present invention. Figure 3 In the image, 'a' represents the SEM image of ADN@Tp-DHT at a magnification of 20 μm. Figure 3 In this context, b represents the surface EDS energy spectrum of ADN@Tp-DHT. Figure 3 In the diagram, 'c' represents the elemental distribution of C on the ADN@Tp-DHT surface. Figure 3 In the diagram, d represents the elemental distribution of N on the ADN@Tp-DHT surface. Figure 3 In the diagram, 'e' represents the elemental distribution of O on the ADN@Tp-DHT surface. Figure 3 f in the figure represents the elemental distribution of F on the ADN@Tp-DHT surface.

[0031] Figure 4 This is a SEM image of ADN@Tp-DHT@PTFE from the present invention. Figure 4 In the image, 'a' represents the SEM image of ADN@Tp-DHT@PTFE at a magnification of 10 μm. Figure 4 In the image, b represents the SEM image of ADN@Tp-DHT@PTFE at a magnification of 500 nm.

[0032] Figure 5 This is the EDS diagram of ADN@Tp-DHT@PTFE of the present invention. Figure 5 In the image, 'a' represents the SEM image of ADN@Tp-DHT@PTFE at a magnification of 9 μm. Figure 5In this context, b represents the surface EDS energy spectrum of ADN@Tp-DHT@PTFE. Figure 5 In the diagram, 'c' represents the elemental distribution of C on the surface of the ADN@Tp-DH@PTFET. Figure 5 In the diagram, d represents the elemental distribution of N on the ADN@Tp-DHT@PTFE surface. Figure 5 In this context, 'e' represents the elemental distribution of O on the ADN@Tp-DHT@PTFE surface. Figure 5 f in the figure represents the elemental distribution of F on the ADN@Tp-DHT@PTFE surface.

[0033] Figure 6 This is a comparison chart of the hygroscopicity tests of ADN, Tp-DHT, ADN@Tp-DHT and ADN@Tp-DHT@PTFE according to the present invention;

[0034] Figure 7 This is a comparison chart of the combustion pressures of ADN, ADN / DHT, Tp-DHT, ADN@Tp-DHT and ADN@Tp-DHT@PTFE according to the present invention;

[0035] Figure 8 This is a comparison diagram of the combustion heat of ADN, ADN / DHT, Tp-DHT, ADN@Tp-DHT and ADN@Tp-DHT@PTFE of the present invention;

[0036] Figure 9 This is a schematic diagram of the combustion process of ADN, ADN / DHT, Tp-DHT, ADN@Tp-DHT and ADN@Tp-DHT@PTFE of the present invention. Detailed Implementation

[0037] The present invention will be further described below with reference to the accompanying drawings and embodiments. Unless otherwise defined, the technical or scientific terms used in this invention should be understood in their ordinary sense by those skilled in the art. The features mentioned above or in the specific examples mentioned in this invention can be combined arbitrarily, and these specific embodiments are only used to illustrate the invention and are not intended to limit the scope of the invention.

[0038] Example 1

[0039] This invention provides an integrated coating material based on moisture resistance and synergistic energy release, which is a ternary core-shell structured ADN@Tp-DHT@PTFE. Its preparation method includes the following steps:

[0040] S1. Prepare a solution of methylbenzene:dioxane:acetic acid (6M) = 1 mL:3 mL:0.6 mL. Add 3,6-diazidoxy-1,2,4,5-tetraazine (DHT, 0.03 mmol) while stirring at 600 rpm. After thorough dispersion, add 0.2 g of ADN and continue stirring. Finally, add 1,3,5-trialdehyde phloroglucinol (Tp, 0.02 mmol) to obtain a mixed solution.

[0041] S2. The mixed solution was quickly transferred to a 10 mL Schlenk tube and rapidly frozen in liquid nitrogen. After three freeze-thaw cycles, the solution was degassed and then purged with nitrogen. The tube was then sealed and heated at 80 °C for 3 days. The product was collected by filtration and washed with deionized water, dioxane, and THF to obtain a dark red solid. The solid was dried for 72 hours to obtain ADN@Tp-DHT.

[0042] S3. Place the ADN@Tp-DHT on the sample stage of the vibratory magnetron sputtering coating instrument, set the sputtering power supply to RF, introduce argon gas into the chamber, and control the working pressure in the chamber at 3×10⁻⁶. -2 The sputtering target cooling water circulation temperature was 18℃, the vibration frequency was 1300rpm, and a polytetrafluoroethylene nanofilm was coated on the surface of ADN@Tp-DHT to obtain a ternary core-shell structured coating material ADN@Tp-DHT@PTFE.

[0043] Example 2

[0044] This invention provides an integrated coating material based on moisture resistance and synergistic energy release, which is a ternary core-shell structured ADN@Tp-DAT@PTFE. Its preparation method includes the following steps:

[0045] S1. Prepare a solution of methylbenzene:dioxane:acetic acid (6M) = 1 mL:3 mL:0.6 mL. Add 3,6-diamino-1,2,4,5-tetraazine (DAT, 0.03 mmol) while stirring at 600 rpm. After thorough dispersion, add 0.2 g of ADN and continue stirring. Finally, add 1,3,5-trialdehyde phloroglucinol (Tp, 0.02 mmol) to obtain a mixed solution.

[0046] S2. The mixed solution was quickly transferred to a 10 mL Schlenk tube and rapidly frozen in liquid nitrogen. After three freeze-thaw cycles, the solution was degassed, then purged with nitrogen gas. The tube was sealed and heated at 100 °C for 3 days. The product was collected by filtration. After washing with deionized water, dioxane, and THF, a dark red solid was obtained. The solid was dried for 72 hours to obtain ADN@Tp-DAT.

[0047] S3. Place the ADN@Tp-DAT on the sample stage of the vibratory magnetron sputtering coating instrument, set the sputtering power supply to RF, introduce argon gas into the chamber, and control the working pressure in the chamber at 3×10⁻⁶. -2 The sputtering target cooling water circulation temperature was 18℃, the vibration frequency was 1300rpm, and a polytetrafluoroethylene nanofilm was coated on the surface of ADN@Tp-DAT to obtain a ternary core-shell structured coating material ADN@Tp-DAT@PTFE.

[0048] Example 3

[0049] This invention provides an integrated coating material based on moisture resistance and synergistic energy release, which is a ternary core-shell structured ADN@Tp-DAAT@PTFE. Its preparation method includes the following steps:

[0050] S1. Prepare a solution of methylbenzene:dioxane:acetic acid (6M) = 1 mL:3 mL:0.6 mL. While stirring at 600 rpm, add 3,3'-azobis(6-amino-1,2,4,5-tetraazine) (DAAT, 0.03 mmol), and after thorough dispersion, add 0.2 g of ADN and continue stirring. Finally, add 1,3,5-trialdehyde phloroglucinol (Tp, 0.02 mmol) to obtain a mixed solution.

[0051] S2. The mixed solution was quickly transferred to a 10 mL Schlenk tube and rapidly frozen in liquid nitrogen. After three freeze-thaw cycles, the solution was degassed, then purged with nitrogen gas. The tube was sealed and heated at 100 °C for 3 days. The product was collected by filtration. After washing with deionized water, dioxane, and THF, a dark red solid was obtained. The solid was dried for 72 hours to obtain ADN@Tp-DAAT.

[0052] S3. Place the ADN@Tp-DAAT on the sample stage of the vibratory magnetron sputtering coating instrument, set the sputtering power supply to RF, introduce argon gas into the chamber, and control the working pressure in the chamber at 3×10⁻⁶. -2 The sputtering target cooling water circulation temperature was 18℃, the vibration frequency was 1300rpm, and a polytetrafluoroethylene nanofilm was coated on the surface of ADN@Tp-DAAT to obtain a ternary core-shell structured coating material ADN@Tp-DAAT@PTFE.

[0053] Comparative Example 1

[0054] It is pure ADN material.

[0055] Comparative Example 2

[0056] The difference from Example 1 is that step S3 was not performed to coat the polytetrafluoroethylene nanofilm, and the resulting product was ADN@Tp-DHT.

[0057] Characterization detection

[0058] The pure ADN (ammonium dinitramide), Tp-DHT, ADN@Tp-DHT, and ADN@Tp-DHT@PTFE prepared in Example 1 were tested using a Fourier transform infrared spectroscopy (FTIR) instrument. The infrared spectra are shown below. Figure 1 As shown.

[0059] Depend on Figure 1 It can be known that at approximately 1420-1450cm - The sharp peak at 1540 cm⁻¹ is due to the stretching vibration of the azo group (N=N) in ADN, a characteristic of its molecular skeleton. - 1 corresponds to the C=N characteristic peak in ADN, and is related to the molecular conjugated system. 1408 cm⁻¹ - 1 is the characteristic peak of CN in Tp-DHT, at 1644 cm⁻¹. - The peak at position 1 is a characteristic N=N peak in the tetrazine structure, which largely coincides with the position of the carbonyl structure (C=O) present in Tp-DHT. (3280 cm⁻¹) - The broad peak at position 1 corresponds to the NH stretching vibration in the -NHC= structure unique to β-ketoenamine COFs, proving the successful connection between Tp and DHT. In ADN@Tp-DHT, the N=N peak and the C=O peak of Tp-DHT coexist, but some peaks are shifted (e.g., the C=N peak shifts to a lower frequency to 1527 cm⁻¹). -1 This demonstrates that ADN and Tp-DHT interact through π-π conjugation or hydrogen bonding (e.g., between the N=N of ADN and the C=O of Tp-DHT), leading to a change in electron cloud density. In ADN@Tp-DHT@PTFE, the electron cloud density changes by 1150-1250 cm⁻¹. - 1 belongs to the symmetric / antisymmetric stretching vibration of the CF bond in PTFE, proving that PTFE was successfully encapsulated.

[0060] ADN@Tp-DHT was analyzed using scanning electron microscopy (SEM), such as... Figure 2 As shown, EDS analysis was performed simultaneously using images and energy-dispersive X-ray spectroscopy, such as... Figure 3 As shown. By Figures 2 to 3 As can be seen, ADN@Tp-DHT exhibits a clustered aggregate structure, formed by ECOF particles adsorbed onto the ADN surface through physical adsorption or weak interactions (such as van der Waals forces). C, N, and O elements are uniformly distributed on the surface of the composite material.

[0061] The ADN@Tp-DHT@PTFE prepared in Example 1 was analyzed by scanning electron microscopy (SEM). Figure 4 As shown, EDS analysis was performed simultaneously using images and energy-dispersive X-ray spectroscopy, such as... Figure 5 As shown. By Figures 4 to 5 It can be seen that the porous structure of the original Tp-DHT has completely disappeared, and the surface is covered by a continuous coating layer. High-magnification SEM shows that there are nanoscale protrusions on the surface of the clusters, which are micro-regional crystallization of the PTFE coating layer or localized accumulation of ADN molecules. The fluorine element is uniformly distributed on the surface of ADN@Tp-DHT@PTFE, and the PTFE coats the composite material in the form of a nanoscale thin film. No fluorine element deficiency was observed in some areas, indicating that the PTFE coating layer has excellent continuity and sealing properties.

[0062] Hygroscopicity test

[0063] The hygroscopicity of pure ADN (ammonium dinitramide), Tp-DHT, ADN@Tp-DHT and ADN@Tp-DHT@PTFE prepared in Example 1 was tested and the hygroscopicity rate was calculated.

[0064] Test procedure: ADN, Tp-DHT, ADN@Tp-DHT, and ADN@Tp-DHT@PTFE were respectively placed in a freeze dryer and dried for 3 hours. The mass was then measured and recorded as m. dry Then place it in a constant temperature and humidity chamber at 25℃-75%RH for 72 hours, remove and weigh the sample, and record the mass as m. wet The test results are as follows Figure 6 As shown. The moisture absorption rate is calculated using the following formula:

[0065]

[0066] from Figure 6 It can be seen that the pure ADN material rapidly absorbs water within 24 hours, reaching a moisture absorption rate of 40.2%, and continues to absorb water within 72 hours, reaching saturation at 62.7% after 72 hours. The water absorption rate of Tp-DHT reaches its highest point at 48 hours, at 11.4%, and decreases to 7.7% after 72 hours. The water absorption rate of ADN@Tp-DHT is lower than that of ADN and Tp-DHT, with a water absorption rate of 7.3% after 72 hours, which is 11.6% and 94.8% of the water absorption rates of ADN and Tp-DHT, respectively. The water absorption rate of ADN@Tp-DHT@PTFE reaches its highest point at 3.3% after 72 hours, which is only 5.3% of the water absorption rate of ADN. The water absorption rate curve is almost horizontal within 72 hours (slope 0.14% / h), indicating that the PTFE layer has long-term stability.

[0067] Flammability test

[0068] Combustion pressure and heat of combustion were tested in a 1 MPa argon atmosphere after mixing ADN, ADN@Tp-DHT, and ADN@Tp-DHT@PTFE with aluminum powder. Figure 7 and Figure 8 As shown, a snapshot of the combustion process was taken using a high-speed camera, such as... Figure 9 As shown. A control group was prepared by mixing DHT (4 wt%) adsorbed on the surface of ADN with aluminum powder, denoted as ADN / DHT.

[0069] from Figures 7 to 9 The results show that the pressure and heat generated by the complete combustion of pure ADN mixed with aluminum powder are 2381.9 kPa and 7888 J / g, respectively. Since DHT itself is an energetic material, the combustion pressure is increased during combustion. Therefore, the pressure and heat generated by the complete combustion of Al / ADN / DHT reach 2790.0 kPa and 8952 J / g, respectively, which are 17.1% and 13.5% higher than Al / ADN. The confined pore structure and interlayer staggered arrangement of Tp-DHT can effectively form constraints and thus regulate the gas production and heat diffusion dynamics of ADN, forming a "micro-reaction chamber" effect. This results in the combustion pressure of Al / ADN@Tp-DHT reaching 2920.7 kPa, which is 22.6% higher than Al / ADN. However, since the reaction precursor Tp of Tp-DHT is a non-energetic material, the heat of combustion is slightly lower than that of Al / ADN / DHT, at 8671 J / g, but still 109.9% of that of Al / ADN. Although the presence of PTFE film as a non-energetic material can form a confinement, the combustion pressure and heat of Al / ADN@Tp-DHT@PTFE are lower than those of Al / ADN@Tp-DHT, at 2875.4 kPa and 8525 J / g, respectively. However, these figures are still 20.7% and 8.08% higher than those of Al / ADN. In other words, the ADN@Tp-DHT@PTFE of the present invention has a stronger gas generation capacity (combustion pressure), more complete combustion heat release, and a faster combustion rate than pure ADN.

[0070] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and not to limit them. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can still be made to the technical solutions of the present invention, and these modifications or equivalent substitutions cannot cause the modified technical solutions to deviate from the spirit and scope of the technical solutions of the present invention.

Claims

1. An integrated coating material based on moisture absorption prevention and synergistic energy release, characterized in that: The coating material has a ternary core-shell structure, which consists of a dinitramide ammonium core, an energetic covalent organic framework intermediate layer, and a polytetrafluoroethylene nanofilm outer layer from the inside out. The energetic covalent organic framework intermediate layer is bonded to the surface of the dinitramide ammonium core through hydrogen bonds or p-π conjugation, and the polytetrafluoroethylene nanofilm outer layer is coated on the outside of the energetic covalent organic framework intermediate layer in the form of a continuous nanoscale film.

2. The integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 1, characterized in that: The energetic covalent organic framework in the intermediate layer of the energetic covalent organic framework includes one of Tp-DHT, Tp-DAT or Tp-DAAT.

3. The integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 2, characterized in that: Tp-DHT is generated by the reaction of 1,3,5-trialdehyde-resorcinol with 3,6-dihydrazino-1,2,4,5-tetraazine.

4. The integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 2, characterized in that: Tp-DAT is generated by the reaction of 1,3,5-trialdehyde phloroglucinol with 3,6-diamino-1,2,4,5-tetraazine.

5. The integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 2, characterized in that: Tp-DAAT is generated by the reaction of 1,3,5-trialdehyde phloroglucinol with 3,3'-azobis(6-amino-1,2,4,5-tetraazine).

6. A method for preparing an integrated coating material based on moisture-wicking and synergistic energy release as described in any one of claims 1-5, characterized in that, Includes the following steps: S1. After mixing mesitylene, dioxane, and acetic acid, add an energetic monomer, dinitramide ammonium, and 1,3,5-trialdehyde phloroglucinol in sequence under stirring to obtain a mixed solution; S2. Transfer the mixed solution to a Schlenk tube and freeze it rapidly in liquid nitrogen. After three freeze-thaw cycles, degas the solution and then purge it with nitrogen gas. Seal the tube and heat it for 2-4 days. Filter and collect the product. Wash the product with deionized water, dioxane, and THF and then dry it for 60-80 hours to obtain ADN@ECOFs. S3. A polytetrafluoroethylene nanofilm was coated onto the surface of ADN@ECOFs using a vibration-type magnetron sputtering process to obtain a ternary core-shell structured coating material ADN@ECOFs@PTFE.

7. The method for preparing the integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 6, characterized in that: In S1, the volume ratio of mesitylene, dioxane, and acetic acid is 0.5-1.5 mL: 2-4 mL: 0.4-0.8 mL; The energetic monomer includes one or more of 3,6-dihydrazino-1,2,4,5-tetraazine, 3,6-diamino-1,2,4,5-tetraazine, and 3,3'-azo-bis(6-amino-1,2,4,5-tetraazine), and the molar ratio of the energetic monomer to 1,3,5-trialdehyde phloroglucinol is 0.02-0.04 mmol: 0.01-0.03 mmol.

8. The method for preparing the integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 7, characterized in that: In S2, the heating reaction temperature is 60–100℃.

9. The method for preparing the integrated coating material based on moisture absorption prevention and synergistic energy release according to claim 7, characterized in that: In S3, the conditions for the vibration-type magnetron sputtering process are: the sputtering power source is an RF power source, argon gas is introduced into the chamber, and the working pressure in the chamber is controlled at 3 × 10⁻⁶. -2 The torr sputtering target cooling water circulation temperature is 18℃, and the vibration frequency is 1000-1300rpm.

10. An application of an integrated coating material based on moisture absorption prevention and synergistic energy release as described in any one of claims 1-5, characterized in that: It is used in high-energy oxidizers for solid propellants.

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