High-entropy Prussian blue analogue as well as preparation method and application thereof

Abstract

The invention discloses a high-entropy Prussian blue analogue and a preparation method and application thereof, and relates to the technical field of solid propellants, the high-entropy Prussian blue analogue comprises at least five of Fe, Co, Zn, Ni, Cu and Mn, and the high-entropy Prussian blue analogue is a solid cubic particle. The high-entropy Prussian blue analogue prepared by the preparation method disclosed by the invention is richer in catalytic active center, has the characteristics of stable catalytic process and catalysis sustainability, can enable the decomposition peak of AP to tend to be gentle, enables the decomposition behavior to be close to constant-speed decomposition, and improves the catalytic efficiency of AP.

Description

Technical Field

[0001] The invention belongs to the technical field of solid propellants, and in particular relates to a high-entropy Prussian blue analogue and a preparation method and application thereof. Background Art

[0002] Composite solid propellant is an energetic polymer composite material composed of multiple components such as adhesives, oxidants, reductants, plasticizers, burning rate regulators, etc. Its combustion behavior greatly affects the actual combat capability of missiles and the carrying capacity of launch vehicles.

[0003] AP (ammonium perchlorate) is the most common oxidant in composite solid propellants at this stage, and its thermal decomposition behavior determines the overall effect of the final composite solid propellant. In order to improve the burning rate and stability of the propellant and reduce the pressure index during the combustion process, the most commonly used method is to add a burning rate catalyst to the propellant to adjust the thermal decomposition behavior of AP. The commonly used burning rate catalyst is a single nano-metal oxide or some inorganic salts, which are non-energy components in the propellant. Adding it to the propellant reduces the relative content of the energy component, resulting in a decrease in the energy of the composite solid propellant.

[0004] PBAs (Prussian blue analogs) are one of the earliest burning rate catalysts used in composite solid propellants. They are inexpensive and highly efficient burning rate catalysts, and their catalytic efficiency is comparable to that of ferrocenes. More importantly, PBAs have positive heat generation, and even if they are added in larger amounts, they will not reduce the energy of composite solid propellants. Existing public literature (Chen Jianfa, Preparation and catalytic performance of nano Prussian blue compounds, master's thesis of Nanjing University of Science and Technology, 2010) studied the catalytic performance of PBAs on the thermal decomposition of AP. The results showed that nano PBAs have better catalytic performance than micron PBAs. However, nano PBAS, which is a catalyst for the thermal decomposition of AP, is composed of 2 to 3 metal elements. Although it can reduce the peak temperature of AP's high-temperature decomposition, AP decomposes quickly, and the thermal decomposition rate of AP cannot be regulated, and the purpose of AP uniform decomposition cannot be achieved.

[0005] High entropy materials were first proposed in 2004. Compared with traditional alloys, high entropy alloys have excellent mechanical properties, thermodynamic stability, electromagnetic properties, etc. In recent years, there have been endless reports on the application of high entropy materials as electrochemical energy storage materials, but there are no reports on the research of high entropy PBAs catalyzing the thermal decomposition of AP. Summary of the invention

[0006] The purpose of the present invention is to overcome the deficiencies in the prior art and provide a high-entropy Prussian blue analogue and a preparation method and application thereof. The prepared high-entropy Prussian blue analogue has richer catalytic active centers, has the characteristics of stable catalytic process and catalytic sustainability, can make the decomposition peak of AP tend to be gentle, the decomposition behavior is close to uniform decomposition, and the catalytic efficiency of AP is improved.

[0007] The present invention provides the following technical solutions: In a first aspect, a high entropy Prussian blue analogue is provided, wherein the high entropy Prussian blue analogue comprises at least five of Fe, Co, Zn, Ni, Cu, and Mn, and the high entropy Prussian blue analogue is a solid cubic particle.

[0008] Furthermore, the particle size of the high entropy Prussian blue analogue is 100-200 nm. If the particle size is too large, the catalytic effect will be reduced, and if the particle size is too small, agglomeration will occur due to the higher surface energy, thereby reducing the catalytic performance.

[0009] In a second aspect, a method for preparing the high entropy Prussian blue analogue described in the first aspect is provided, comprising the following steps: dissolving a metal salt and a citrate in deionized water to obtain a metal precursor solution; adding the metal precursor solution to the hexacyano salt aqueous solution to obtain a turbid solution; The turbid liquid is allowed to stand and age, and the solid obtained after the aging is washed, impurity-removed and dried to obtain a high-entropy Prussian blue analogue.

[0010] Furthermore, the metal salt includes any one or more combinations of nitrate, perchlorate, hydrochloride, acetate, and sulfate, and the citrate includes any one or a combination of two of sodium citrate and potassium citrate.

[0011] Furthermore, the molar ratio of the metal salt to the citrate is 1:1, and the ratio of the metal salt to deionized water is 1mmol: 2~200mL. Too high a concentration of the metal salt will cause the product particle size to become smaller, while a lower concentration will cause the particle size to increase, thereby affecting the catalytic effect.

[0012] Furthermore, the hexacyanoferrate includes any one or more combinations of potassium hexacyanoferrate, sodium hexacyanoferrate, potassium hexacyanoferrate, and sodium hexacyanoferrate.

[0013] Furthermore, the molar ratio of the metal salt to the hexacyanodite is 1:1, the volume ratio of the hexacyanodite aqueous solution to the metal precursor solution is 1:1, and the metal precursor solution is added to the hexacyanodite aqueous solution and stirred for 5 to 60 minutes to obtain a turbid solution.

[0014] Furthermore, the aging time of the turbid solution is 1 to 96 hours. If the aging time is too short, it will affect the crystal growth, resulting in crystal defects or smaller particle size. If the aging time is too long, it will reduce the preparation efficiency.

[0015] In a third aspect, an application of a high entropy Prussian blue analogue is provided, specifically: the high entropy Prussian blue analogue described in the first aspect or the high entropy Prussian blue analogue prepared by the method described in the second aspect is added to a solid propellant as a catalyst for the decomposition of ammonium perchlorate.

[0016] Furthermore, the amount of the high entropy Prussian blue analogue is 5wt% or less of the total mass of the ammonium perchlorate and the high entropy Prussian blue analogue.

[0017] Compared with the prior art, the present invention has the following beneficial effects: (1) The high entropy Prussian blue analogue prepared by the present invention has the morphology of solid cubic particles, including at least five of Fe, Co, Zn, Ni, Cu, and Mn, and has a high metal content. The high configuration entropy brought by multi-element co-doping makes the catalytic active centers of the Prussian blue analogue richer, and has the characteristics of stable catalytic process and catalytic sustainability, which can make the decomposition peak of AP tend to be gentle, and the decomposition behavior is close to uniform decomposition. Moreover, the synergistic catalytic system of multiple transition metal elements also reduces the high-temperature decomposition temperature of AP to about 300°C, which coincides with the low-temperature decomposition temperature region of AP, making the decomposition heat of AP more concentrated, thereby improving the performance of the composite solid propellant; (2) The method provided by the present invention makes the morphology and particle size of the prepared high-entropy Prussian blue analogue controllable, the raw material cost is low, the process conditions are simple, the production process is green, environmentally friendly and pollution-free, and has good application prospects. BRIEF DESCRIPTION OF THE DRAWINGS

[0018] Figure 1 is the XRD pattern of CoMnNiCuZnFe-PBA prepared in Example 3 of the present invention; Figure 2 is a SEM image of the high entropy Prussian blue analogues prepared in Examples 4 and 5 of the present invention; Figure 3 is a DSC graph of pure AP in an embodiment of the present invention; Figure 4 is a DSC graph of CoMnNiCuZnFe-PBA prepared in Example 3 of the present invention; Figure 5 It is the DSC graph of Co-HSs prepared in Comparative Example 2 of the present invention. DETAILED DESCRIPTION

[0019] The present invention will be further described below in conjunction with the accompanying drawings. The following embodiments are only used to more clearly illustrate the technical solution of the present invention, and cannot be used to limit the protection scope of the present invention.

[0020] Example 1

[0021] This embodiment provides a method for preparing a high entropy Prussian blue analogue, the steps are as follows: S1. Preparation of metal precursor solution: Dissolve 0.5 mmol manganese nitrate, 0.5 mmol copper acetate, 0.5 mmol nickel acetate, 0.5 mmol zinc nitrate and 2 mmol sodium citrate in 40 mL deionized water and stir until a uniform and transparent metal precursor solution is formed.

[0022] S2. Synthesis of high entropy Prussian blue analogs: Add the metal precursor solution into 40 mL of an aqueous solution containing 2 mmol of potassium hexacyanoferrate and stir for 10 min to obtain a turbid solution.

[0023] S3. Growth of high entropy Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 10 h.

[0024] S4. Purification of high entropy Prussian blue analogue: After the reaction, the Prussian blue analogue is washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue is placed in a 90° C. drying oven for 12 hours to obtain a manganese, nickel, copper, zinc, and iron co-doped high entropy Prussian blue analogue, recorded as MnNiCuZnFe-PBA.

[0025] Example 2

[0026] This embodiment provides a method for preparing a high entropy Prussian blue analogue, the steps are as follows: S1. Preparation of metal precursor solution: Dissolve 1 mmol of cobalt nitrate, 1 mmol of nickel sulfate, 1 mmol of copper acetate, 1 mmol of zinc sulfate and 4 mmol of sodium citrate in 80 mL of deionized water and stir until a uniform and transparent metal precursor solution is formed.

[0027] S2. Synthesis of high entropy Prussian blue analogs: Add the metal precursor solution into 80 mL of a solution containing 4 mmol of sodium hexacyanoferrate and stir for 5 min to obtain a turbid solution.

[0028] S3. Growth of high entropy Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 1 h.

[0029] S4. Purification of high entropy Prussian blue analogue: After the reaction, the Prussian blue analogue was washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue was placed in a 90° C. drying oven for 12 hours to obtain a cobalt-nickel-copper-zinc-iron co-doped high entropy Prussian blue analogue, recorded as CoNiCuZnFe-PBA.

[0030] Example 3

[0031] This embodiment provides a method for preparing a high entropy Prussian blue analogue, the steps are as follows: S1. Preparation of metal precursor solution: dissolve 1 mmol of cobalt nitrate, 1 mmol of copper nitrate, 1 mmol of nickel perchlorate, 1 mmol of manganese chloride, 1 mmol of zinc acetate and 5 mmol of sodium citrate in 100 mL of deionized water and stir until a uniform and transparent metal precursor solution is formed.

[0032] S2. Synthesis of high entropy Prussian blue analogs: Add the metal precursor solution into 100 mL of a solution containing 5 mmol of potassium hexacyanoferrate and stir for 30 min to obtain a turbid solution.

[0033] S3. Growth of high entropy Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 48 hours.

[0034] S4. Purification of high entropy Prussian blue analogue: After the reaction, the Prussian blue analogue is washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue is placed in a 90°C drying oven for 12 hours to obtain a high entropy Prussian blue analogue co-doped with cobalt, manganese, nickel, copper, zinc and iron, recorded as CoMnNiCuZnFe-PBA.

[0035] Example 4

[0036] This embodiment provides a method for preparing a high entropy Prussian blue analogue, the steps are as follows: S1. Preparation of metal precursor solution: 1.5 mmol cobalt nitrate, 1.5 mmol manganese acetate, 1.5 mmol copper sulfate, 1.5 mmol zinc acetate and 6 mmol sodium citrate were dissolved in 120 mL deionized water and stirred until a uniform and transparent metal precursor solution was formed.

[0037] S2. Synthesis of high entropy Prussian blue analogs: Add the metal precursor solution into 120 mL of a solution containing 6 mmol of sodium hexacyanoferrate and stir for 60 min to obtain a turbid solution.

[0038] S3. Growth of high entropy Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 12 h.

[0039] S4. Purification of high entropy Prussian blue analogue: After the reaction, the Prussian blue analogue was washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue was placed in a 90°C drying oven for 12 hours to obtain a cobalt-manganese-copper-zinc-iron co-doped high entropy Prussian blue analogue, recorded as CoMnCuZnFe-PBA.

[0040] Example 5

[0041] This embodiment provides a method for preparing a high entropy Prussian blue analogue, the steps are as follows: S1. Preparation of metal precursor solution: Dissolve 0.5 mmol manganese nitrate, 0.5 mmol cobalt acetate, 0.5 mmol nickel acetate, 0.5 mmol zinc nitrate and 2 mmol potassium citrate in 40 mL deionized water and stir until a uniform and transparent metal precursor solution is formed.

[0042] S2. Synthesis of high entropy Prussian blue analogs: Add the metal precursor solution into 40 mL of a solution containing 2 mmol of sodium hexacyanoferrate and stir for 25 min to obtain a turbid solution.

[0043] S3. Growth of high entropy Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 96 h.

[0044] S4. Purification of high entropy Prussian blue analogue: After the reaction, the Prussian blue analogue is washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue is placed in a 90° C. drying oven for 12 hours to obtain a high entropy Prussian blue analogue co-doped with cobalt, manganese, nickel, zinc and iron, recorded as CoMnNiZnFe-PBA.

[0045] Example 6

[0046] This embodiment provides a method for preparing a high entropy Prussian blue analogue, the steps are as follows: S1. Preparation of metal precursor solution: Dissolve 0.25 mmol manganese nitrate, 0.25 mmol copper acetate, 0.25 mmol nickel acetate, 0.25 mmol cobalt chloride and 1 mmol sodium citrate in 20 mL deionized water and stir until a uniform and transparent metal precursor solution is formed.

[0047] S2. Synthesis of high entropy Prussian blue analogs: Add the metal precursor solution into 20 mL of a solution containing 1 mmol of potassium hexacyanoferrate and stir for 45 min to obtain a turbid solution.

[0048] S3. Growth of high entropy Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 30 h.

[0049] S4. Purification of high entropy Prussian blue analogue: After the reaction, the Prussian blue analogue is washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue is placed in a 90° C. drying oven for 12 hours to obtain a high entropy Prussian blue analogue co-doped with cobalt, manganese, nickel, copper and iron, recorded as CoMnNiCuFe-PBA.

[0050] Comparative Example 1 This comparative example provides a method for preparing a tetrametallic Prussian blue analogue, and the specific steps are as follows: S1. Preparation of metal precursor solution: Dissolve 0.1 mmol manganese nitrate, 0.1 mmol copper acetate, 0.1 mmol zinc acetate and 2 mmol potassium citrate in 40 mL deionized water and stir until a uniform and transparent metal precursor solution is formed.

[0051] S2. Synthesis of tetrametallic Prussian blue analogs: Add the metal precursor solution into 40 mL of a solution containing 2 mmol of sodium hexacyanoferrate and stir for 25 min to obtain a turbid solution.

[0052] S3. Growth of tetrametallic Prussian blue analog crystals: The obtained turbid solution was allowed to stand at room temperature for 12 h.

[0053] S4. Purification of tetrametallic Prussian blue analogue: After the reaction, the Prussian blue analogue was washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogue was placed in a drying oven at 90° C. for 12 hours to obtain a tetrametallic Prussian blue analogue, which was recorded as CuMnZnFe-PBA.

[0054] Comparative Example 2 This comparative example provides a method for preparing a multi-metal hollow Prussian blue analog, which specifically comprises the following steps: S1. Preparation of metal precursor solution: First, dissolve 7 mmol of cobalt nitrate in 40 mL of isopropanol and 8 mL of glycerol under stirring until a uniform and transparent solution is formed; S2. Synthesis of metal alkoxide: The metal precursor solution is heated to a certain temperature of 180° C. in a reactor, and the total heating time is controlled within 6 hours to obtain metal alkoxide by reaction.

[0055] S3. Preparation of Prussian blue analogs: 300 mg of the prepared metal alkoxide was dispersed in 140 ml of ethanol. After dispersion, the solution was added dropwise to 100 ml of potassium hexacyanoferrate solution containing 0.9 g of the metal alkoxide. The reaction was heated to 90° C. for 5 h.

[0056] S4. Purification of Prussian blue analogues: After the reaction, the Prussian blue analogues were washed with deionized water and ethanol for multiple times to remove impurities. The purified Prussian blue analogues were placed in a drying oven at 90° C. for 12 hours to obtain cobalt Prussian blue hollow spheres (Co-HSs) assembled from Prussian blue cubes formed by Co-Fe.

[0057] This comparative example is Example 4 in the invention patent application CN118145678A.

[0058] Comparative Example 3 This comparative example provides a method for preparing a high entropy multimetal alkoxide, and the specific steps are as follows: S1. Preparation of metal precursor solution: First, dissolve 1 mmol of cobalt nitrate, 1 mmol of nickel acetate, 1 mmol of copper chloride, 1 mmol of zinc sulfate, and 1 mmol of manganese nitrate in 40 mL of isopropanol and 8 mL of glycerol under stirring until a uniform and transparent solution is formed; S2. Synthesis of high entropy multi-metal alkoxides: The metal precursor solution is heated to a certain temperature of 180° C. in a reactor, and the total heating time is controlled within 6 hours to obtain metal alkoxides by reaction.

[0059] S3. Purification of high entropy polymetallic alkoxide: After the reaction, the high entropy polymetallic alkoxide is washed with deionized water and ethanol for multiple times to remove impurities. The purified high entropy polymetallic alkoxide is placed in a drying oven at 90°C for 12 hours to obtain high entropy polymetallic alkoxide, which is recorded as CoMnNiCuZn-SSs.

[0060] Performance Characterization Example 1. Perform XRD test on the high entropy Prussian blue analog (CoMnNiCuZnFe-PBA) powder prepared in Example 3. Figure 1 As shown in the figure, there are strong peaks at around 18°, 25° and 36°, which correspond to the (200), (220) and (400) crystal planes of the Prussian blue analogue, respectively. The peaks corresponding to these crystal planes are the characteristic peaks of the Prussian blue analogue.

[0061] 2. The products prepared in Examples 1 to 6 and Comparative Examples 1 to 3 were characterized by SEM. Figure 2 As shown, the high entropy Prussian blue analogs prepared in Example 4 and Example 5 all present similar nanocubic structures, and the particle size is between 100 and 200 nm. The product morphologies of other examples and comparative examples are shown in Table 1. It can be seen from Table 1 that the products in Examples 1 to 6, Comparative Example 1 and Comparative Example 3 all present solid cubic structures, and the Co-HSs in Comparative Example 2 presents hollow spheres.

[0062] 3. The high entropy Prussian blue analogue samples prepared in Examples 1 to 6 and the product samples prepared in Comparative Examples 1 to 3 were used as catalysts for thermal decomposition of AP. Specifically, each sample was mixed with AP, and the amount of each sample was 0.5 mg, which was 5% of the total mass of the sample + AP. Differential scanning calorimetry (DSC) was used to characterize the process of AP decomposition catalyzed by each sample. The heating rate was 10°C / min. The high temperature decomposition peak and curve trend of AP are shown in Table 1.

[0063] Table 1 Morphology and DSC characterization results of samples of Examples 1 to 6 and Comparative Examples 1 to 3

[0064] (1) Figure 3 The DSC curve of pure AP decomposition process. It can be seen from the figure that the decomposition process of pure AP is divided into two stages: low temperature decomposition stage (T L =293.5℃) and high temperature decomposition stage (T H =414.1℃).

[0065] Figure 4 The DSC curve of the AP decomposition process catalyzed by CoMnNiCuZnFe-PBA prepared in Example 3 shows that, under the condition of a heating rate of 10°C / min, the entire decomposition stage presents a continuous process with a peak value of 298.4°C. Figure 3 By comparison, the addition of CoMnNiCuZnFe-PBA significantly advances the high-temperature decomposition stage of pure AP to 298.4°C.

[0066] From Table 1, it can be seen that Examples 1-6 and Comparative Example 1 are all Prussian blue analogs, and their morphological structures are all solid cubes, and both can significantly reduce the decomposition temperature of AP. However, Examples 1-6 can decompose AP smoothly, while Comparative Example 1 makes the decomposition of AP quickly reach a peak value. The reason is that Examples 1-6 are high-entropy Prussian blue analogs (five or more metal elements are used), while Comparative Example 1 is a four-metal Prussian blue analog. The high-entropy Prussian blue analog has a higher atomic utilization rate and abundant active sites, thereby decomposing AP smoothly. This shows that the high entropy characteristics of Prussian blue analogs have a key influence on the catalytic decomposition effect of AP.

[0067] (2) Figure 5 The DSC test results of the AP decomposition process catalyzed by the multi-metal hollow Prussian blue analogue prepared in Comparative Example 2 are shown in the figure. As can be seen from the figure, at a heating rate of 10°C / min, the multi-metal hollow Prussian blue analogue in Comparative Example 2 can reduce the decomposition temperature of AP to 298.4°C, but it quickly reaches the peak value during decomposition. Figure 4 contrast, Figure 4The decomposition peak of AP in the medium tends to be gentle, and a flat-top peak appears, indicating that the decomposition behavior is close to uniform decomposition.

[0068] As shown in Table 1, Examples 1-6 and Comparative Example 2 are all Prussian blue analogs, but the morphology of Examples 1-6 is a solid cube, while the morphology of Comparative Example 2 is a hollow sphere. The results show that both Examples 1-6 and Comparative Example 2 can significantly reduce the decomposition temperature of AP, but Examples 1-6 can decompose AP steadily, while Comparative Example 2 can make the decomposition of AP quickly reach a peak value, which shows that the morphology of Prussian blue analogs has a key influence on the catalytic decomposition effect of AP.

[0069] (3) Examples 1-6 and Comparative Example 3 are all high entropy alloys, Examples 1-6 are high entropy Prussian blue analogs, and Comparative Example 3 is high entropy metal alkoxide. As shown in Table 1, Examples 1-6 and Comparative Example 3 can significantly reduce the decomposition temperature of AP, but Examples 1-6 can make AP decompose steadily, while Comparative Example 3 makes the decomposition of AP quickly reach a peak value, which shows that Prussian blue analogs, a class of compounds containing cyano and transition metal ions, have a key influence on the catalytic decomposition effect of AP.

[0070] The above is only a preferred embodiment of the present invention. It should be pointed out that for ordinary technicians in this technical field, several improvements and modifications can be made without departing from the technical principles of the present invention. These improvements and modifications should also be regarded as the scope of protection of the present invention.

Claims

1. A high entropy Prussian blue analogue, characterized in that The high entropy Prussian blue analogue includes at least five of Fe, Co, Zn, Ni, Cu, and Mn, and the high entropy Prussian blue analogue is a solid cubic particle.

2. The high entropy Prussian blue analogue according to claim 1, characterized in that The particle size of the high entropy Prussian blue analogue is 100-200 nm.

3. A method for preparing the high entropy Prussian blue analogue according to any one of claims 1 to 2, characterized in that: The following steps are involved: dissolving a metal salt and a citrate in deionized water to obtain a metal precursor solution; adding the metal precursor solution to the hexacyano salt aqueous solution to obtain a turbid solution; The turbid liquid is allowed to stand and age, and the solid obtained after the aging is washed, impurity-removed and dried to obtain a high-entropy Prussian blue analogue.

4. The method for preparing a high entropy Prussian blue analogue according to claim 3, characterized in that: The metal salt includes any one or more combinations of nitrate, perchlorate, hydrochloride, acetate, and sulfate, and the citrate includes any one or a combination of two of sodium citrate and potassium citrate.

5. The method for preparing a high entropy Prussian blue analogue according to claim 3, characterized in that: The molar ratio of the metal salt to the citrate is 1:1, and the ratio of the metal salt to deionized water is 1 mmol: 2-200 mL.

6. The method for preparing a high entropy Prussian blue analogue according to claim 3, characterized in that: The hexacyanoferrate includes any one or more combinations of potassium hexacyanoferrate, sodium hexacyanoferrate, potassium hexacyanoferrate, and sodium hexacyanoferrate.

7. The method for preparing a high entropy Prussian blue analogue according to claim 3, characterized in that: The molar ratio of the metal salt to the hexacyanodite is 1:1, the volume ratio of the hexacyanodite aqueous solution to the metal precursor solution is 1:1, and the metal precursor solution is added to the hexacyanodite aqueous solution and stirred for 5 to 60 minutes to obtain a turbid solution.

8. The method for preparing a high entropy Prussian blue analogue according to claim 3, characterized in that: The aging time of the turbid liquid is 1 to 96 hours.

9. An application of a high entropy Prussian blue analogue, characterized in that: Use of the high entropy Prussian blue analogue described in any one of claims 1 to 2 or the high entropy Prussian blue analogue prepared by the method described in any one of claims 3 to 8 as a catalyst for the decomposition of ammonium perchlorate added to a solid propellant.

10. The use of the high entropy Prussian blue analogue according to claim 9, characterized in that: The amount of the high entropy Prussian blue analogue is 5wt% or less of the total mass of the ammonium perchlorate and the high entropy Prussian blue analogue.

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