A polymeric CON energetic material and its preparation method

Abstract

This invention discloses a polymeric conjugate (CON) energetic material and its preparation method, belonging to the field of energetic materials technology. It solves the problem that the synthesis technology of polymeric CON materials in the prior art requires high pressure, making it difficult to achieve. The method includes: preparing a high-pressure device; placing a catalyst in the high-pressure chamber of the high-pressure device; assembling the anvil of the high-pressure device into a cryostat; introducing CO and N2 into the cryostat; cooling the cryostat along with the internal gas to liquefy the gaseous raw material and fill the high-pressure chamber of the high-pressure device; pressurizing the liquid raw material and encapsulating it inside the high-pressure chamber; raising the temperature to vaporize excess liquid raw material and completing post-processing, while simultaneously sealing the high-pressure chamber; applying the pressure at the sample location inside the high-pressure chamber to the target pressure and maintaining the pressure at room temperature; and obtaining the polymeric conjugate energetic material. The preparation method of this invention requires lower pressure.

Description

Technical Field

[0001] This invention belongs to the field of energetic materials technology, and specifically relates to a polymeric CON energetic material and its preparation method. Background Technology

[0002] With social progress and technological development, various application scenarios are placing higher demands on the safety, environmental friendliness, and energy density of energetic materials. Currently, the energy density of conventional hydrocarbon, nitrogen, and oxygen-based energetic materials has reached its limit, making the search for higher energy density energetic materials urgent. High-stretch bond energy-releasing materials refer to solid polymers formed from energetic gaseous molecular compounds under condensed-state physics. Theoretical predictions suggest that the energy of high-stretch bond energy-releasing materials can reach up to 100 times the TNT equivalent. The condensation effect of high-stretch bonds can help improve the energy density of energetic materials.

[0003] Due to the stringent synthesis conditions, reports on the preparation of high-tension bond energy release materials remain relatively scarce. Since the initial raw materials for these materials are generally gaseous molecules, the encapsulation of these raw materials is a significant factor limiting the widespread research and large-scale synthesis of high-tension bond energy release materials. In publicly available reports, high-pressure encapsulation of gaseous raw materials is typically achieved through high-pressure gas filling. The aforementioned high-pressure gas encapsulation usually targets diamond anvil cells, using relatively small amounts of raw material gas for laboratory material synthesis and property exploration. For the synthesis of high-tension bond energy release materials, the raw materials are typically highly toxic energetic gases with strong oxidizing, corrosive, flammable, and explosive properties. Under high pressure, the reactivity of these gas molecules is further enhanced, accelerating their interaction with metal equipment and ventilation pipes. Leaks could endanger the safety of laboratory personnel and the surrounding environment. Furthermore, the direct polymerization of gaseous raw materials to form solid polymers results in a volume shrinkage of more than 1000 times. Therefore, the preparation of high-tension bond energy release materials by loading gaseous raw materials under high pressure is difficult to scale up, limiting the engineering and application of energetic materials. Summary of the Invention

[0004] Based on the above analysis, the present invention aims to provide a polymeric CON energetic material and its preparation method to solve the following technical problems: the synthesis technology of polymeric CON materials in the prior art requires high pressure and harsh synthesis conditions, which are not easy to achieve.

[0005] The objective of this invention is mainly achieved through the following technical solutions:

[0006] On the one hand, the present invention provides a method for preparing a polymeric CON energetic material, the method comprising the following steps:

[0007] S1. Complete the preparation work for the high-pressure device; the high-pressure chamber of the high-pressure device contains a catalyst;

[0008] S2. Assemble the anvil of the high-pressure device into the low-temperature thermostat;

[0009] S3. Introduce CO and N2 into the low-temperature thermostat;

[0010] S4. Cool the low-temperature thermostat and its internal gas to a temperature between the melting and boiling points of CO and N2, so that the gaseous raw materials are liquefied and fill the high-pressure chamber of the high-pressure device.

[0011] S5. Pressurize the liquid raw material using the high-pressure anvil of the high-pressure device to encapsulate the liquid raw material inside the high-pressure chamber;

[0012] S6. Increase the temperature to vaporize the excess liquid raw material and complete the final processing, while sealing the high-pressure chamber;

[0013] S7. Under room temperature conditions, apply the pressure at the sample in the high-pressure chamber to the target pressure; and maintain the temperature and pressure to obtain the polymeric CON energetic material.

[0014] Furthermore, in S1, the preparation work for the high-voltage device includes the following steps:

[0015] S01. Clean the surface of the anvil of the high-pressure device and use the anvil surface to pre-press the gasket so that an indentation appears in the center of the gasket.

[0016] S02. Drill a hole at the center of the indentation on the gasket; the hole serves as a high-pressure chamber for sample encapsulation and reaction.

[0017] S03. Deposit the catalyst onto the upper and lower anvils of the high-pressure device;

[0018] S04. To manufacture a metal sealing ring suitable for sealing raw materials in high-pressure equipment, serving as a container after gas liquefaction;

[0019] S05. Secure the gasket and metal sealing ring to the indentation position on the anvil surface under the high-pressure device;

[0020] S06. Fix the relative positions of the upper anvil, sealing gasket, metal sealing ring and lower anvil, wherein a certain distance is maintained between the upper anvil and the lower anvil, for the encapsulation of N2 and CO gaseous raw materials.

[0021] Furthermore, in S01, the gasket material is T301 stainless steel, rhenium metal, or tungsten metal.

[0022] Furthermore, in SO3, the catalyst is Pd, Pt, Au, Ru, Rh or Cu, as well as metal-supported CeO2 and TiO2.

[0023] Furthermore, the catalyst is deposited onto the surface of a high-pressure anvil via magnetron sputtering, existing in the form of a thin film.

[0024] Furthermore, the thickness of the catalyst film is 15–30 nm.

[0025] Furthermore, in S7, the target pressure is 9–23 GPa, and the heat preservation and pressure holding time is 0.5–4 h.

[0026] Furthermore, in S7, under room temperature conditions, the pressure at the sample in the high-pressure chamber is applied to the target pressure; the temperature at the sample in the high-pressure chamber is applied to the target temperature (above 700°C) through the heating system, and the temperature and pressure are maintained; then the heating is stopped, and the high-pressure chamber and sample are cooled to room temperature to obtain the polymeric CON energetic material.

[0027] Furthermore, in S7, the target pressure is 9–19 GPa, the target temperature is 700–1250 °C, and the heat and pressure holding time is 0.5–3 h.

[0028] The present invention also provides a polymeric CON energetic material, which is prepared by the above-described preparation method.

[0029] Compared with the prior art, the present invention can achieve at least one of the following technical effects:

[0030] 1) The preparation method of the polymeric CON energetic material of the present invention completes the gaseous raw material encapsulation through low-temperature liquefaction. Compared with the currently used high-pressure gas filling encapsulation method, the method of the present invention can complete the encapsulation of highly toxic gaseous materials and tail gas post-treatment, and has a small volume compression ratio, making it easy to scale up the process and beneficial to the preparation and application of novel high-tension bond energy release materials. The method of the present invention promotes the polymerization reaction of polymeric CON energetic material by using a catalyst, reducing the pressure required for the polymerization reaction of CO and N2. Compared with the polymerization reaction of CO and N2 without the addition of a catalyst, the synthesis pressure is reduced from the existing 40 GPa or more to 9-23 GPa, a reduction of 17-31 GPa or more, for example, a reduction of 26-35 GPa. By reducing the synthesis pressure, the preparation difficulty of polymeric CON energetic material can be greatly reduced, providing technical support for the mass production of polymeric CON energetic material.

[0031] 2) The preparation method of the polymeric CON energetic material of the present invention utilizes a synergistic approach of catalyst and high temperature to accelerate the polymerization reaction of the polymeric CON energetic material and reduce the pressure required for the polymerization reaction of CO and N2. Compared with the polymerization reaction of CO and N2 without catalyst, the synthesis pressure is reduced from the existing 40 GPa or more to 9-19 GPa, a reduction of 21-31 GPa or more, for example, a reduction of 33-40 GPa. By reducing the synthesis pressure, the preparation difficulty of polymeric CON energetic material can be greatly reduced, providing technical support for the mass production of polymeric CON energetic material.

[0032] 3) The density of the polymeric CON energetic material prepared by the method of the present invention is 4.1 g / cm³. 3 The above are high-energy-density materials, which have broad application prospects in many fields.

[0033] Other features and advantages of the invention will be set forth in the following description, and in part will be obvious from the description or may be learned by practicing the invention. The objects and other advantages of the invention may be realized and obtained by means of the structures particularly pointed out in the written description and the accompanying drawings. Attached Figure Description

[0034] The accompanying drawings are for illustrative purposes only and are not intended to limit the invention. Throughout the drawings, the same reference numerals denote the same parts.

[0035] Figure 1 The X-ray diffraction patterns are those of the polymeric CON energetic materials prepared in Examples 1-2 of this invention. Detailed Implementation

[0036] The following detailed description of a polymeric CON energetic material and its preparation method, with reference to specific embodiments, is provided. These embodiments are for comparative and illustrative purposes only, and the present invention is not limited to these embodiments.

[0037] Through in-depth research, the inventors applied a catalyst to the preparation process of polymerized CON energetic materials in order to reduce the pressure required for the preparation process and precisely controlled the temperature of the preparation process, thereby reducing the pressure required for the preparation of polymerized CON energetic materials.

[0038] This invention provides a method for preparing a polymeric CON energetic material, comprising the following steps:

[0039] S1. Complete the preparation work for the high-pressure device; the high-pressure chamber of the high-pressure device contains a catalyst;

[0040] S2. Assemble the anvil of the high-pressure device into the low-temperature thermostat;

[0041] S3. Introduce CO and N2 into the low-temperature thermostat;

[0042] S4. Cool the low-temperature thermostat and its internal gas to a temperature between the melting and boiling points of CO and N2, so that the gaseous raw materials are liquefied and fill the high-pressure chamber of the high-pressure device.

[0043] S5. Pressurize the liquid raw material using the high-pressure anvil of the high-pressure device to encapsulate the liquid raw material inside the high-pressure chamber;

[0044] S6. Increase the temperature to vaporize the excess liquid raw material and complete the final processing, while sealing the high-pressure chamber;

[0045] S7. Under room temperature conditions, apply the pressure at the sample in the high-pressure chamber to the target pressure; and maintain the temperature and pressure.

[0046] S8. Unload the pressure to obtain the polymeric CON energetic material.

[0047] Specifically, in S1 above, the high-pressure device is selected from a multi-face top press, a two-face top press, or a ring press.

[0048] Specifically, in S1 above, the multi-face top press is a six-face top press.

[0049] Specifically, in S1 above, the double-sided press is either a Paris-Edinburgh press or a diamond anvil device.

[0050] Specifically, in S1 above, the preparation work for the high-voltage device is carried out through the following steps:

[0051] S01. Clean the surface of the anvil of the high-pressure device and use the anvil surface to pre-press the gasket so that an indentation appears in the center of the gasket.

[0052] S02. Then, a hole with a diameter of 300μm to 10mm is punched at the center of the indentation of the sealing gasket. This hole serves as a high-pressure chamber for sample encapsulation and reaction.

[0053] S03. Deposit the catalyst onto the upper and lower anvils of the high-pressure device, with the thickness of the deposited catalyst film being 15–30 nm;

[0054] S04. To manufacture a metal sealing ring suitable for sealing raw materials in high-pressure equipment, serving as a container after gas liquefaction;

[0055] S05. Secure the gasket and metal sealing ring to the indentation position on the anvil surface under the high-pressure device;

[0056] S06. Fix the relative positions of the upper anvil, sealing gasket, metal sealing ring and lower anvil, wherein a certain distance is maintained between the upper anvil and the lower anvil, for the encapsulation of N2 and CO gaseous raw materials.

[0057] Specifically, in S01 above, the gasket material is made of T301 stainless steel, rhenium metal, or tungsten metal, etc.

[0058] Specifically, in S02 above, the drilling is performed by laser drilling or mechanical drilling.

[0059] Specifically, in S05 above, the distance between the upper and lower pressing anvils is 2 to 5 mm.

[0060] Specifically, in the aforementioned S03, the catalyst is deposited onto the surface of a high-pressure anvil by magnetron sputtering and exists in the form of a thin film.

[0061] Specifically, in the aforementioned SO3, the catalyst can be metals such as Pd, Pt, Au, Ru, Rh, and Cu, as well as metal-supported CeO2 and TiO2. Considering that if the catalyst film thickness is too small, it is easy to fall off during the process, and if the catalyst film thickness is too large, the catalytic effect will be insufficient and it will affect the pressure required for polymerization, therefore, the thickness of the catalyst film is controlled to be 15-30 nm, for example, 16 nm, 17 nm, 18 nm, 19 nm, 20 nm, 21 nm, 22 nm, 23 nm, 24 nm, 25 nm, 26 nm, 27 nm, 28 nm, and 29 nm.

[0062] Specifically, in S2 above, the low-temperature thermostat is used to control the liquefaction temperature of gaseous raw materials.

[0063] Specifically, in S3 above, a gas flow meter is used to control the proportion of each component gas introduced.

[0064] Specifically, in S3 above, the molar ratio of CO to N2 is (1-9):(1-9).

[0065] Specifically, in the above S4, the cryogenic medium used for cooling mainly includes ice-salt bath, dry ice solvent bath, liquid nitrogen solvent bath and liquid helium solvent bath.

[0066] Specifically, in S5 above, the pressure required for encapsulating the liquid material is 0.2 to 15 GPa; for example, 0.5 GPa, 1 GPa, 1.5 GPa, 2 GPa, 2.5 GPa, 3 GPa, 3.5 GPa, 4 GPa, 4.5 GPa, 5 GPa, 5.5 GPa, 6 GPa, 7 GPa, 8 GPa, 9 GPa, 10 GPa, 11 GPa, 12 GPa, 13 GPa, and 14 GPa.

[0067] Specifically, in S6 above, the excess carbon monoxide and nitrogen are post-processed by being compressed and stored in spare cylinders under high pressure.

[0068] Specifically, in S7 above, the target pressure is 9 to 23 GPa, such as 14 GPa, 15 GPa, 16 GPa, 17 GPa, 18 GPa, 19 GPa, 20 GPa, 21 GPa, and 22 GPa; the heat preservation and pressure holding time is 0.5 to 4 hours, such as 1 hour, 2 hours, and 3 hours.

[0069] Specifically, in S7 above, when only the pressure at the sample within the high-pressure chamber is applied to the target pressure without further increasing the temperature, the target pressure is 13–23 GPa, for example, 14 GPa, 15 GPa, 16 GPa, 17 GPa, 18 GPa, 19 GPa, 20 GPa, 21 GPa, or 22 GPa; the holding time is 0.5–4 hours, for example, 1 hour, 2 hours, or 3 hours. The specific control of the target pressure and the holding time is as follows:

[0070] When the molar ratio of CO to N2 is 1:1, the catalyst is Pd, the target pressure is 19.5–20.5 GPa, and the holding time is 2–3 h.

[0071] When the molar ratio of CO to N2 is 2:1, the catalyst is Pd, the target pressure is 14.5–15.5 GPa, and the holding time is 2–3 h.

[0072] When the molar ratio of CO to N2 is 1:2, the catalyst is Pt, the target pressure is 21.5–22.5 GPa, and the heat and pressure holding time is 2–3 h.

[0073] When the molar ratio of CO to N2 is 1:4, the catalyst is Pt@CeO2, the target pressure is 19.5–20.5 GPa, and the holding time is 2–3 h.

[0074] Specifically, in S7 above, under room temperature conditions, the pressure at the sample in the high-pressure chamber is applied to the target pressure; the temperature at the sample in the high-pressure chamber is applied to the target temperature (above 700°C) through the heating system, and the temperature and pressure are maintained; then the heating is stopped, and the high-pressure chamber and sample are cooled to room temperature to obtain the polymeric CON energetic material.

[0075] Specifically, in S7 above, the target pressure is 9–19 GPa, the target temperature is 700–1250℃, and the heat and pressure holding time is 0.5–3 h.

[0076] Specifically, in the above S7, the molar ratio of CO to N2 is 1:1, the target pressure is 14.5 to 15.5 GPa when the catalyst is Pd, the target temperature is 950 to 1050 °C, and the holding time is 0.5 to 1 h.

[0077] Specifically, in the above S7, the molar ratio of CO to N2 is 2:1, the target pressure is 9.5 to 10.5 GPa when the catalyst is Pd, the target temperature is 950 to 1050 °C, and the holding time is 1.5 to 3 h.

[0078] Specifically, in the above S7, the molar ratio of CO to N2 is 1:2, the catalyst is Pt, the target pressure is 17.5 to 18.5 GPa, the target temperature is 850 to 950 °C, and the holding time is 0.5 to 1 h.

[0079] Specifically, in the above S7, the molar ratio of CO to N2 is 1:4, the catalyst is Pt@CeO2, the target pressure is 12.5~13.5GPa, the target temperature is 750~850℃, and the holding time is 0.5~1h.

[0080] Specifically, temperature and pressure sensors are installed inside the thermostat cavity to monitor the temperature and pressure conditions inside the cavity in real time.

[0081] Specifically, in S7 above, an excessively high pressurization rate can easily generate a pressure gradient, which is detrimental to sample synthesis. Therefore, the pressurization rate should be controlled between 0.5 and 2 GPa / min.

[0082] Specifically, in S8 above, the method for unloading pressure is manual unloading.

[0083] Specifically, the density of the obtained polymeric CON energetic material is 4.1 g / cm³. 3 above.

[0084] Example 1-1

[0085] This embodiment provides a method for preparing a polymeric CON energetic material, including:

[0086] S1. Complete the preparation work for the high-pressure device; the high-pressure chamber of the high-pressure device contains a catalyst;

[0087] S2. Assemble the anvil of the high-pressure device into the low-temperature thermostat;

[0088] S3. Introduce CO and N2 into the low-temperature thermostat;

[0089] S4. Cool the low-temperature thermostat and its internal gas to a temperature between the melting and boiling points of CO and N2, so that the gaseous raw materials are liquefied and fill the high-pressure chamber of the high-pressure device.

[0090] S5. Pressurize the liquid raw material using the high-pressure anvil of the high-pressure device to encapsulate the liquid raw material inside the high-pressure chamber;

[0091] S6. Increase the temperature to vaporize the excess liquid raw material and complete the final processing, while sealing the high-pressure chamber;

[0092] S7. Under room temperature conditions, apply the pressure at the sample in the high-pressure chamber to the target pressure (without increasing the temperature); and maintain the temperature and pressure.

[0093] S8. Unload the pressure to obtain the polymeric CON energetic material.

[0094] Specifically, the high-pressure device in this embodiment uses a Paris-Edinburgh type compressor.

[0095] Specifically, in S1 above, the preparation work for the high-voltage device is carried out through the following steps:

[0096] S01. Clean the surface of the anvil of the high-pressure device and use the anvil surface to pre-press the gasket so that an indentation appears in the center of the gasket.

[0097] S02. Then, a hole with a diameter of 6 mm is punched at the center of the indentation of the gasket. This hole serves as a high-pressure chamber for sample encapsulation and reaction.

[0098] S03. Deposit the catalyst onto the upper and lower anvils of the high-pressure device, and the thickness of the deposited catalyst film is 30 nm;

[0099] S04. To manufacture a metal sealing ring suitable for sealing raw materials in high-pressure equipment, serving as a container after gas liquefaction;

[0100] S05. Secure the gasket and metal sealing ring to the indentation position on the anvil surface under the high-pressure device;

[0101] S06. Fix the relative positions of the upper anvil, sealing gasket, metal sealing ring and lower anvil, wherein a certain distance is maintained between the upper anvil and the lower anvil, for the encapsulation of N2 and CO gaseous raw materials.

[0102] Specifically, in S01 above, the gasket material is T301 stainless steel.

[0103] Specifically, in S02 above, the drilling is performed by laser drilling.

[0104] Specifically, in S05 above, the distance between the upper and lower pressing anvils is 5 mm.

[0105] Specifically, in the aforementioned SO3, the catalyst is Pd deposited onto the surface of a high-pressure anvil by magnetron sputtering, existing in the form of a thin film.

[0106] Specifically, in S3 above, the molar ratio of CO to N2 is 2:1.

[0107] Specifically, in S4 above, the cryogenic medium used for cooling is a liquid nitrogen solvent bath.

[0108] Specifically, in S5 above, the pressure required for encapsulating the liquid raw material is 0.2 GPa.

[0109] Specifically, in S6 above, the excess carbon monoxide and nitrogen are post-processed by being compressed and stored in spare cylinders under high pressure.

[0110] Specifically, in S7 above, the target pressure is 15 GPa, and the heat preservation and pressure holding time is 3 hours.

[0111] Specifically, in S7 above, the boost rate is 2 GPa / min.

[0112] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.6 g / cm³. 3 .

[0113] Examples 1-2

[0114] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiment 1-1, except that:

[0115] S7. Under room temperature conditions, apply the pressure at the sample in the high-pressure chamber to the target pressure; apply the temperature at the sample in the high-pressure chamber to the target temperature, and maintain the temperature and pressure; then stop heating and cool the high-pressure chamber and sample to room temperature.

[0116] Specifically, the target pressure is 10 GPa, the target temperature is 1000℃, and the heat and pressure holding time is 3 hours.

[0117] In the above S7, the boost rate is 1.2 GPa / min.

[0118] The X-ray diffraction pattern of the polymeric CON energetic material prepared in this embodiment is as follows: Figure 1 As shown. The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.6 g / cm³. 3 .

[0119] Comparative Example 1-1

[0120] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Example 1-1, except that:

[0121] The high-pressure device in this comparative example uses a diamond anvil double-sided press.

[0122] In S02, a hole with a diameter of 300μm is punched at the center of the indentation of the gasket.

[0123] In S05, the distance between the upper and lower anvils is 2 mm.

[0124] The high-pressure unit in S1 does not contain a catalyst, i.e., it does not include SO3.

[0125] In S7, the target pressure is 50 GPa, and the heat and pressure holding time is 3 hours.

[0126] The polymeric CON energetic material prepared in this comparative example is a black solid with a density of approximately 4.6 g / cm³. 3 .

[0127] Comparative Examples 1-2

[0128] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Examples 1-2, except that:

[0129] The high-pressure device in this comparative example uses a diamond anvil double-sided press.

[0130] In S02, a hole with a diameter of 300μm is punched at the center of the indentation of the gasket.

[0131] In S05, the distance between the upper and lower anvils is 2 mm.

[0132] The high-pressure unit in S1 does not contain a catalyst, i.e., it does not include SO3.

[0133] In S7, the target pressure is 30 GPa, and the heat and pressure holding time is 3 hours.

[0134] The polymeric CON energetic material prepared in this comparative example is a black solid with a density of approximately 4.6 g / cm³. 3 .

[0135] By comparing Examples 1-1, 1-2, 1-1, and 1-2 above, it can be seen that the addition of a catalyst in the preparation method of the present invention can reduce the synthesis pressure of the polymeric CON energetic material from 50 GPa to 15 GPa, a reduction of 35 GPa; through the synergistic effect of the catalyst and high temperature, the synthesis pressure is reduced from 50 GPa to 10 GPa, a reduction of 40 GPa; thus reducing the preparation difficulty of the polymeric energetic material and providing technical support for its mass production.

[0136] Example 2-1

[0137] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiment 1-1, except that:

[0138] In S3 above, the molar ratio of CO to N2 is 1:1.

[0139] In the above S7, the target pressure is 20 GPa, and the heat preservation and pressure holding time is 3 hours.

[0140] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.1 g / cm³. 3 .

[0141] Example 2-2

[0142] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiments 1-2, except that:

[0143] In S3 above, the molar ratio of CO to N2 is 1:1.

[0144] In the above S7, the target pressure is 15 GPa, the target temperature is 1000℃, and the heat and pressure holding time is 0.5h.

[0145] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.1 g / cm³. 3 .

[0146] Comparative Example 2-1

[0147] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Comparative Example 1-1, except that:

[0148] In S3 above, the molar ratio of CO to N2 is 1:1.

[0149] In the above S7, the target pressure is 50 GPa, and the heat preservation and pressure holding time is 3 hours.

[0150] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.1 g / cm³. 3 .

[0151] Comparative Example 2-2

[0152] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Comparative Examples 1-2, except that:

[0153] In S3 above, the molar ratio of CO to N2 is 1:1.

[0154] In the above S7, the target pressure is 30 GPa, and the heat preservation and pressure holding time is 3 hours.

[0155] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.1 g / cm³. 3 .

[0156] By comparing Examples 2-1, 2-2, 2-1, and 2-2 above, it can be seen that the preparation method of the present invention can reduce the synthesis pressure of the polymeric CON energetic material by adding a catalyst, from 50 GPa to 20 GPa, a reduction of 30 GPa; through the synergistic effect of the catalyst and high temperature, the synthesis pressure is reduced from 50 GPa to 15 GPa, a reduction of 35 GPa; thus reducing the preparation difficulty of the polymeric energetic material and providing technical support for its mass production.

[0157] Example 3-1

[0158] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiment 1-1, except that:

[0159] In the SO3 mentioned above, the catalyst is Pt.

[0160] In S3 above, the molar ratio of CO to N2 is 1:2.

[0161] In the above S7, the target pressure is 22 GPa, and the heat preservation and pressure holding time is 3 hours.

[0162] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.3 g / cm³. 3 .

[0163] Example 3-2

[0164] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiments 1-2, except that:

[0165] In the SO3 mentioned above, the catalyst is Pt.

[0166] In S3 above, the molar ratio of CO to N2 is 1:2.

[0167] In the above S7, the target pressure is 18 GPa, the target temperature is 900℃, and the heat and pressure holding time is 0.5h.

[0168] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.3 g / cm³. 3 .

[0169] Comparative Example 3-1

[0170] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Comparative Example 1-1, except that:

[0171] In S3 above, the molar ratio of CO to N2 is 1:2.

[0172] In the above S7, the target pressure is 45 GPa, and the heat preservation and pressure holding time is 3 hours.

[0173] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.3 g / cm³. 3 .

[0174] Comparative Example 3-2

[0175] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Comparative Examples 1-2, except that:

[0176] In the above S3, the molar ratio of CO to N2 is 1:2;

[0177] In the above S7, the target pressure is 28 GPa, and the heat preservation and pressure holding time is 3 hours.

[0178] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.3 g / cm³. 3 .

[0179] By comparing the above Examples 3-1, 3-2, 3-1, and 3-2, it can be seen that the synthesis pressure of the polymeric CON energetic material can be reduced from 45 GPa to 22 GPa by adding a catalyst in the preparation method of the present invention, which is a reduction of 23 GPa; through the synergistic effect of the catalyst and high temperature, the synthesis pressure is reduced from 45 GPa to 18 GPa, which is a reduction of 27 GPa; the preparation difficulty of the polymeric energetic material is reduced, providing technical support for its mass production.

[0180] Example 4-1

[0181] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiment 1-1, except that:

[0182] In the SO3 mentioned above, the catalyst is Pt@CeO2.

[0183] In the above S3, the molar ratio of CO to N2 is 1:5;

[0184] In the above S7, the target pressure is 20 GPa, and the heat preservation and pressure holding time is 3 hours.

[0185] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.2 g / cm³. 3 .

[0186] Example 4-2

[0187] This embodiment provides a method for preparing a polymeric CON energetic material. The preparation method in this embodiment is basically the same as that in Embodiments 1-2, except that:

[0188] In the SO3 mentioned above, the catalyst is Pt@CeO2.

[0189] In the above S3, the molar ratio of CO to N2 is 1:5;

[0190] In the above S7, the target pressure is 13 GPa, the target temperature is 800℃, and the heat and pressure holding time is 0.5h.

[0191] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.2 g / cm³. 3 .

[0192] Comparative Example 4-1

[0193] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Comparative Example 1-1, except that:

[0194] In the above S3, the molar ratio of CO to N2 is 1:5.

[0195] In the above S7, the target pressure is 46 GPa, and the heat preservation and pressure holding time is 3 hours.

[0196] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.2 g / cm³. 3 .

[0197] Comparative Example 4-2

[0198] This comparative example provides a method for preparing a polymeric CON energetic material. The preparation method of this comparative example is basically the same as that of Comparative Examples 1-2, except that:

[0199] In the above S3, the molar ratio of CO to N2 is 1:5.

[0200] In the above S7, the target pressure is 32 GPa, and the heat preservation and pressure holding time is 3 hours.

[0201] The polymeric CON energetic material prepared in this embodiment is a black solid with a density of approximately 4.2 g / cm³. 3 .

[0202] By comparing Examples 4-1, 4-2, 4-1, and 4-2 above, it can be seen that the synthesis pressure of the polymeric CON energetic material can be reduced from 46 GPa to 20 GPa by adding a catalyst in the preparation method of the present invention, which is a reduction of 26 GPa; through the synergistic effect of the catalyst and high temperature, the synthesis pressure is reduced from 46 GPa to 13 GPa, which is a reduction of 33 GPa; the preparation difficulty of the polymeric energetic material is reduced, providing technical support for its mass production.

[0203] As can be seen from the embodiments and comparative examples of this invention, by adding a catalyst to the synthesis process of polymeric CON energetic materials, this invention effectively reduces the pressure required for the synthesis of polymeric CON energetic materials. By employing a synergistic approach of catalyst and high temperature to complete the preparation of energetic materials, the polymerization reaction of polymeric CON energetic materials is promoted, and the pressure required for the polymerization reaction of CO and N2 is reduced. By reducing the synthesis pressure, the preparation difficulty of polymeric CON energetic materials can be greatly reduced, providing technical support for the mass production of polymeric CON energetic materials.

[0204] The above description is only a preferred embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any changes or substitutions that can be easily conceived by those skilled in the art within the scope of the technology disclosed in the present invention should be included within the scope of protection of the present invention.

Claims

1. A method for preparing a polymeric CON energetic material, characterized in that, The preparation method includes the following steps: S1. Complete the preparation work for the high-pressure device; the high-pressure chamber of the high-pressure device contains a catalyst; S2. Assemble the anvil of the high-pressure device into the low-temperature thermostat; S3. Introduce CO and N2 into the low-temperature thermostat; S4. Cool the low-temperature thermostat and its internal gas to a temperature between the melting and boiling points of CO and N2, so that the gaseous raw materials are liquefied and fill the high-pressure chamber of the high-pressure device. S5. Pressurize the liquid raw material using the high-pressure anvil of the high-pressure device to encapsulate the liquid raw material inside the high-pressure chamber; S6. Increase the temperature to vaporize the excess liquid raw material and complete the final processing, while sealing the high-pressure chamber; S7. Under room temperature conditions, apply the pressure at the sample in the high-pressure chamber to the target pressure; And maintain heat and pressure; A polymeric CON energetic material was obtained.

2. The preparation method according to claim 1, characterized in that, In step S1, the preparation of the high-voltage device includes the following steps: S01. Clean the surface of the anvil of the high-pressure device and use the anvil surface to pre-press the gasket so that an indentation appears in the center of the gasket. S02. Drill a hole at the center of the indentation on the gasket; the hole serves as a high-pressure chamber for sample encapsulation and reaction. S03. Deposit the catalyst onto the upper and lower anvils of the high-pressure device; S04. To manufacture a metal sealing ring suitable for sealing raw materials in high-pressure equipment, serving as a container after gas liquefaction; S05. Secure the gasket and metal sealing ring to the indentation position on the anvil surface under the high-pressure device; S06. Fix the relative positions of the upper anvil, sealing gasket, metal sealing ring and lower anvil, wherein a certain distance is maintained between the upper anvil and the lower anvil, for the encapsulation of N2 and CO gaseous raw materials.

3. The preparation method according to claim 2, characterized in that, In S01, the sealing gasket material is T301 stainless steel, rhenium metal, or tungsten metal.

4. The preparation method according to claim 2, characterized in that, In the SO3, the catalyst is Pd, Pt, Au, Ru, Rh or Cu or metal-supported CeO2 or TiO2.

5. The preparation method according to claim 2, characterized in that, The catalyst is deposited onto the surface of a high-pressure anvil by magnetron sputtering and exists in the form of a thin film.

6. The preparation method according to claim 2, characterized in that, The thickness of the catalyst film is 15~30nm.

7. The preparation method according to claim 1, characterized in that, In S7, the target pressure is 9~23 GPa, and the heat preservation and pressure holding time is 0.5~4h.

8. The preparation method according to claim 1, characterized in that, In step S7, under room temperature conditions, the pressure at the sample in the high-pressure chamber is applied to the target pressure; the temperature at the sample in the high-pressure chamber is applied to the target temperature (above 700°C) through the heating system, and the temperature and pressure are maintained; then the heating is stopped, and the high-pressure chamber and the sample are cooled to room temperature to obtain the polymeric CON energetic material.

9. The preparation method according to claim 8, characterized in that, In S7, the target pressure is 9~19 GPa, the target temperature is 700~1250℃, and the heat and pressure holding time is 0.5~3h.

10. A polymeric CON energetic material, characterized in that, The polymeric CON energetic material is prepared using the preparation method described in any one of claims 1 to 9.

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