Polynitrogen fused ring compound and preparation method thereof

Abstract

The invention relates to a polynitrogen fused ring compound and a preparation method thereof, and belongs to the field of organic synthesis and energetic materials. According to the synthesis method of the novel multi-nitrogen fused ring energetic compound, the novel multi-nitrogen fused ring energetic compound of triazole or tetrazolo [1, 2, 4] [1, 5-d] tetrazole is simply and efficiently synthesized by taking a nitro-substituted triazole azo compound as a substrate. The compound has good performance in the aspect of energetic materials and has good application prospects in the future. The compound has very good performance in the aspect of energetic materials, the method is simple and efficient, and a novel triazolo tetrazole skeleton is successfully prepared. The target novel compound is synthesized from basic raw materials, the adopted synthesis method is simple, and reaction conditions are mild. And the compound has the characteristics of high density, high formation enthalpy, high detonation velocity, high detonation pressure, high thermal decomposition temperature, low mechanical sensitivity and the like, so that the compound has very high potential application value in the field of energetic materials.

Description

Technical Field

[0001] The invention relates to a polynitrogen condensed ring compound and a preparation method thereof, belonging to the field of energetic materials. Background Art

[0002] Energetic materials are compounds or mixtures that contain explosive groups or contain oxidants and combustibles, and can independently undergo chemical reactions and output energy. At the same time, energetic materials are also an important component of military explosives, propellants, and rocket propellant formulas. They are widely used in both military and civilian applications, especially in weapons and equipment and national defense construction. Therefore, the performance of energetic materials often plays a decisive role in their application. From the perspective of the design and construction of energetic compounds, the condensed ring skeleton is a very important parent ring skeleton. Since the detonation velocity and detonation pressure of condensed ring energetic compounds have a good linear relationship with the number of N atoms, polynitrogen condensed ring energetic compounds generally have higher energy and are easy to achieve a balance between energy and sensitivity. At the same time, there are more substitution sites on condensed ring compounds to introduce substituents to modify and improve the performance of energetic compounds. At present, most energetic compounds with condensed rings as parent rings are prepared by connecting two to three five-membered rings or six-membered rings in parallel to form condensed ring compounds. In terms of synthesis, the synthesis steps of these reported condensed ring energetic compounds are long and the experimental operation is difficult. In terms of performance, they cannot achieve a high balance between energy density and sensitivity. At the same time, triazolotetrazole condensed ring skeletons contain high nitrogen content, multiple substitution sites, simple synthesis routes, and easy post-experimental treatment, but they have not been reported yet. Therefore, related research in the application field of energetic materials deserves further exploration. Summary of the invention

[0003] The technical problem solved by the present invention is to overcome the deficiencies of the prior art and provide a polynitrogen condensed ring compound and a preparation method thereof.

[0004] The technical solution of the present invention is:

[0005] A polynitrogen fused ring compound, the polynitrogen fused ring compound is 2-(1-amino-1H-1,2,3,4-tetrazolyl-5-yl)-3,5-dihydro-tetrazolyl[1,2,3,4][1,5-d]tetrazolyl, and its structural formula is:

[0006]

[0007] The polynitrogen fused ring compound has very good comprehensive properties in terms of energetic materials, with a density of up to 1.95 g cm –3 , the formation enthalpy is as high as 3.06 kJ g –1 , the explosion speed is as high as 9740m s –1 And dull mechanical sensitivity (IS=40J,FS>360N).

[0008] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0009] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate; its structural formula is:

[0010]

[0011] The second step is to mix the nitrotriazole-substituted hydrazine intermediate prepared in the first step, a base and an organic solvent, react at 40 to 100° C. for 0.5 to 2 hours, then return to room temperature, add an amination reagent, react at room temperature for 0.5 to 12 hours, and remove the organic solvent by distillation under reduced pressure to obtain the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound;

[0012] The molar ratio of the nitrotriazole-substituted hydrazine intermediate to the base is 1:2-6;

[0013] The organic solvent is at least one of acetonitrile, ethanol and tetrahydrofuran;

[0014] The molar mass and volume ratio of the nitrotriazole-substituted hydrazine intermediate and the organic solvent is 1:3 to 10;

[0015] The ratio of the nitrotriazole-substituted hydrazine intermediate to the amination reagent is 1:2-4;

[0016] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0017] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate, the structural formula of which is:

[0018]

[0019] The second step is to mix the nitrotriazole-substituted hydrazine intermediate prepared in the first step, a base and an organic solvent, react at 40 to 100° C. for 0.5 to 2 hours, then return to room temperature, add an amination reagent, react at room temperature for 0.5 to 12 hours, then add an oxidant, react for 1 to 12 hours, and then remove the organic solvent by reduced pressure distillation to obtain the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound; the molar ratio of the nitrotriazole-substituted hydrazine intermediate to the base is 1:2 to 6;

[0020] The organic solvent is at least one of acetonitrile, ethanol and tetrahydrofuran;

[0021] The molar mass and volume ratio of the nitrotriazole-substituted hydrazine intermediate and the organic solvent is 1:3 to 10;

[0022] The ratio of the nitrotriazole-substituted hydrazine intermediate to the amination reagent is 1:2-4;

[0023] The ratio of the nitrotriazole-substituted hydrazine intermediate to the oxidant is 1:1.8-4;

[0024] The oxidant is at least one of N-bromosuccinimide, tert-butyl hypochlorite, and dibromoisocyanuric acid;

[0025] The amination reagent is Hydroxylamine-O-sulfonic acid, At least one of

[0026] In the first step, the method for preparing the nitrotriazole-substituted hydrazine intermediate is:

[0027] A nitro-substituted triazole azo compound, a metal reducing agent and an organic solvent are mixed, and the reaction is carried out at 50 to 100° C. for 4 to 12 hours. After the reaction is completed, the mixture is filtered, and the liquid phase is extracted with an organic solvent to remove the organic solvent to obtain a nitrotriazole-substituted hydrazine intermediate.

[0028] The structural formula of the nitro-substituted triazole azo compound is:

[0029] The metal reducing agent is metal magnesium or zinc;

[0030] The ratio of the molar mass of the nitro-substituted triazole azo compound, the molar mass of the metal reducing agent and the volume of the organic solvent is 1:4-6:6-10;

[0031] In the first step, the method for preparing the nitrotriazole-substituted hydrazine intermediate is:

[0032] A nitro-substituted triazole azo compound, a metal hydride reducing agent and an organic solvent are mixed, and the reaction is carried out at 50 to 100° C. for 4 to 12 hours. After the reaction is completed, the mixture is filtered, and the liquid phase is extracted with an organic solvent to remove the organic solvent to obtain a nitrotriazole-substituted hydrazine intermediate.

[0033] The metal hydride reducing agent is borane, sodium borohydride or lithium aluminum hydride;

[0034] The ratio of the molar mass of the nitro-substituted triazole azo compound, the molar mass of the metal hydride reducing agent and the volume of the organic solvent is 1:4-6:6-10;

[0035] In the first step, the method for preparing the nitrotriazole-substituted hydrazine intermediate is:

[0036] A nitro-substituted triazole azo compound, a base, a hydrazine reducing agent and an organic solvent are mixed, and the reaction is carried out at 10 to 50° C. for 4 to 12 hours. After the reaction is completed, the mixture is filtered, and the liquid phase is extracted with an organic solvent to remove the organic solvent to obtain a nitrotriazole-substituted hydrazine intermediate;

[0037] The hydrazine reducing agent is hydrazine hydrate or hydrazine generated in situ;

[0038] The ratio of the molar mass of the nitro-substituted triazole azo compound, the molar mass of the base, the molar mass of the hydrazine reducing agent and the volume of the organic solvent is 1:2-4:4-6:6-10;

[0039] The obtained nitrotriazole-substituted hydrazine intermediate has similar energetic material properties and a density of 1.74 g cm –3 , the formation enthalpy is as high as 1.55 kJ g –1 , the detonation velocity is 8360m s –1 The explosion pressure is as high as 27.6GPa, with a thermal decomposition temperature of 261℃, a specific impulse of 227.6s and a dull mechanical sensitivity (IS>40J, FS>360N).

[0040] Beneficial Effects

[0041] 1. The novel polynitrogen fused ring energetic compound of the present invention has very good energetic material performance. The density of LX-11 is 1.95 g cm –3 The formation enthalpy is 3.06 kJ g –1 , explosion speed is 9740m s –1 And dull mechanical sensitivity (IS=40J,FS>360N).

[0042] 2. The synthesis method of the novel polynitrogen fused ring energetic compound of the present invention uses a nitro-substituted triazole azo compound as a substrate to simply and efficiently synthesize a novel polynitrogen fused ring energetic compound of the triazole or tetrazolyl[1,2,4][1,5-d]tetrazolyl type. This compound has good performance in energetic materials and will have good application prospects in the future. The compound has very good performance in energetic materials, the method is simple and efficient, and a novel triazole tetrazolyl skeleton is successfully prepared.

[0043] The present invention relates to a type of polynitrogen fused ring compound and a preparation method thereof, and belongs to the field of organic synthesis and energetic materials. The present invention synthesizes a target novel compound from basic raw materials, and the synthesis method adopted is simple and the reaction conditions are mild. In addition, the compound has the characteristics of high density, high formation enthalpy, high detonation velocity and detonation pressure, high thermal decomposition temperature and low mechanical sensitivity, and thus has high potential application value in the field of energetic materials. BRIEF DESCRIPTION OF THE DRAWINGS

[0044] Figure 1 It is the H NMR spectrum of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl;

[0045] Figure 2 The NMR carbon spectrum of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl;

[0046] Figure 3 The NMR nitrogen spectrum of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl;

[0047] Figure 4 It is a high-resolution mass spectrum of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazole;

[0048] Figure 5 The infrared spectrum of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl;

[0049] Figure 6 Differential scanning calorimetry (DSC) (10℃min) of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl –1 );

[0050] Figure 7 This is a single crystal structure diagram of the polynitrogen fused ring compound 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazole. DETAILED DESCRIPTION

[0051] The present invention is further described below in conjunction with specific embodiments, wherein the methods are conventional methods unless otherwise specified, and the raw materials can be obtained from public commercial channels or prepared according to literature unless otherwise specified.

[0052] Example 1

[0053] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0054] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate: Synthesis of 1,2-bis(3-nitro-1H-1,2,4-triazole-5-yl)hydrazine: Dissolve the nitro-substituted triazole azo compound (178 mg, 0.7 mmol) in 7 mL of water, add sodium hydroxide (763 mg, 6.7 mmol), and then add a water (3 mL) solution of hydroxylamine-O-sulfonic acid (191 mg, 4.8 mmol), and react overnight at room temperature. After the reaction is completed, filter and remove the solvent under reduced pressure to obtain 154 mg of a light yellow hydrazine-linked product with a yield of 84%.

[0055]

[0056] The second step is the synthesis of polynitrogen fused ring energetic compounds. The specific steps are as follows:

[0057] The nitrotriazole-substituted hydrazine intermediate (178 mg, 0.7 mmol) prepared in the first step was dissolved in 8 mL of acetonitrile, sodium hydroxide (88 mg, 2.2 mmol) was added, and the mixture was reacted at 50°C for 10 minutes, then returned to room temperature, and MSH (409 mg, 1.9 mmol) was added, and the mixture was reacted at room temperature for 12 hours. After the reaction, the acetonitrile was removed by distillation under reduced pressure, and water and ethyl acetate were added for extraction. The solvent was removed by distillation under reduced pressure to obtain 30 mg of a light yellow solid with a yield of 15%, i.e., the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

[0058]

[0059] The H NMR spectrum data of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound are (400 MHz, DMSO-d 6 ):δ7.80(s,2H,NH)ppm, such as Figure 1 As shown;

[0060] The NMR carbon spectrum data of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound are (100 MHz, DMSO-d 6 ):δ16.1,158.3,156.2,141.0ppm, such as Figure 2 As shown;

[0061] The NMR nitrogen spectrum data of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound are (700MHz, DMSO-d 6 ):δ353.0,351.1,330.4,303.4,285.7,280.0,259.5,251.4,236.7,222.5,199.0,88.5ppm, such as Figure 3 As shown;

[0062] The high-resolution mass spectrum data of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound are C 4 H 3 N 12 O 4 [M–H] - :283.0406,found:283.0395,such as Figure 4 As shown;

[0063] The infrared spectrum data of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound are 3347(s), 3281(m), 1566(m), 1418(m), 1331(m), 1315(s), 11192(s), 1098(s)cm -1 ,like Figure 5 As shown;

[0064] The differential scanning calorimetry (DSC) scanning result of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound showed that the decomposition temperature was 205.8°C, such as Figure 6 As shown;

[0065] The single crystal structure of the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound is shown in FIG. Figure 7 As shown;

[0066] Then the obtained 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound was tested and calculated for performance. First, the density was tested. Under normal temperature and vacuum, its density was 1.95 g cm–3 , the enthalpy of formation is calculated to be 3.06 kJ g –1 , the detonation velocity is calculated to be 9740 m s –1 The explosion pressure was calculated to be 41.8 GPa. The thermal decomposition temperature was tested and the initial decomposition temperature was 206°C. The mechanical sensitivity was tested and the impact sensitivity was 40 J and the friction sensitivity>360 N.

[0067] Example 2

[0068] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0069] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate: the synthesis method of 1,2-di(3-nitro-1H-1,2,4-triazole-5-yl)hydrazine: dissolve the nitro-substituted triazole azo compound (127 mg, 0.5 mmol) in 3 mL of water, add magnesium metal (63 mg, 2.6 mmol), heat at 100 ° C for 6 hours, and after the reaction is completed, filter to remove the solid, and extract the filtrate with ethyl acetate (50 mL × 3 times), and distill under reduced pressure to remove the solvent to obtain 57 mg of a light yellow product with a yield of 45%.

[0070]

[0071] The second step is the synthesis of polynitrogen fused ring energetic compounds. The specific steps are as follows:

[0072] The nitrotriazole-substituted hydrazine intermediate (178 mg, 0.7 mmol) prepared in the first step was dissolved in 8 mL of acetonitrile, sodium hydroxide (88 mg, 2.2 mmol) was added, and the mixture was reacted at 50°C for 10 minutes, then returned to room temperature, MSH (409 mg, 1.9 mmol) was added, and the mixture was reacted at room temperature for 20 minutes, and NBS (214 mg, 1.2 mmol) was added, and the mixture was reacted at room temperature for 1 hour. After the reaction, the acetonitrile was removed by distillation under reduced pressure, and water and ethyl acetate were added for extraction, and the solvent was removed by distillation under reduced pressure to obtain 33 mg of a light yellow solid with a yield of 17%, i.e., the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

[0073]

[0074] Example 3

[0075] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0076] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate: the synthesis method of 1,2-di(3-nitro-1H-1,2,4-triazole-5-yl)hydrazine: dissolve the nitro-substituted triazole azo compound (127 mg, 0.5 mmol) in 3 mL of ethanol, add metallic zinc (343 mg, 5.3 mmol), heat the reaction for 10 hours, and after the reaction is completed, filter to remove the solid, and extract the filtrate with ethyl acetate (50 mL×3 times), and distill under reduced pressure to remove the solvent to obtain 43 mg of a light yellow product with a yield of 34%.

[0077]

[0078] The second step is the synthesis of polynitrogen fused ring energetic compounds. The specific steps are as follows:

[0079] The nitrotriazole-substituted hydrazine intermediate (178 mg, 0.7 mmol) prepared in the first step was dissolved in 8 mL of acetonitrile, sodium hydroxide (88 mg, 2.2 mmol) was added, and the mixture was reacted at 50°C for 10 minutes, then returned to room temperature, MSH (409 mg, 1.9 mmol) was added, and the mixture was reacted at room temperature for 20 minutes, and NBS (214 mg, 1.2 mmol) was added, and the mixture was reacted at room temperature for 12 hours. After the reaction, the acetonitrile was removed by vacuum distillation, and water and ethyl acetate were added for extraction, and the solvent was removed by vacuum distillation again to obtain 40 mg of a light yellow solid with a yield of 20%, namely the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

[0080]

[0081] Example 4

[0082] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0083] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate: the synthesis method of 1,2-di(3-nitro-1H-1,2,4-triazol-5-yl)hydrazine: dissolve the nitro-substituted triazole azo compound (127 mg, 0.5 mmol) in 3 mL of tetrahydrofuran, add a tetrahydrofuran solution of borane (1 mol / L, 0.6 mL, 0.6 mmol), react at room temperature for 6 hours, and after the reaction is completed, filter and remove the solvent by vacuum distillation to obtain 96 mg of a light yellow product with a yield of 75%.

[0084]

[0085] The second step is the synthesis of polynitrogen fused ring energetic compounds. The specific steps are as follows:

[0086] The nitrotriazole-substituted hydrazine intermediate (178 mg, 0.7 mmol) prepared in the first step was dissolved in 8 mL of acetonitrile, sodium hydroxide (88 mg, 2.2 mmol) was added, and the mixture was reacted at 50°C for 10 minutes, then returned to room temperature, MSH (409 mg, 1.9 mmol) was added, and the mixture was reacted at room temperature for 20 minutes, and tert-butyl hypochlorite (214 mg, 1.2 mmol) was added, and the mixture was reacted at room temperature for 1 hour. After the reaction, the acetonitrile was removed by vacuum distillation, and water and ethyl acetate were added for extraction, and the solvent was removed by vacuum distillation again to obtain 124 mg of a light yellow solid with a yield of 63%, namely the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

[0087]

[0088] Example 5

[0089] A method for preparing a polynitrogen condensed ring compound, the method comprising the steps of:

[0090] The first step is to prepare a nitrotriazole-substituted hydrazine intermediate: the synthesis method of 1,2-di(3-nitro-1H-1,2,4-triazole-5-yl)hydrazine: the same as Example 1.

[0091] The second step is a method for synthesizing a novel polynitrogen fused ring energetic compound, the specific steps are as follows:

[0092] Under the protection of anhydrous and oxygen-free argon, the nitrotriazole-substituted hydrazine intermediate (178 mg, 0.7 mmol) prepared in the first step was dissolved in 8 mL of acetonitrile, sodium hydroxide (88 mg, 2.2 mmol) was added, and the mixture was reacted at 50°C for 10 minutes, then returned to room temperature, and MSH (409 mg, 1.9 mmol) was added, and the mixture was reacted at room temperature for 12 hours. After the reaction, the acetonitrile was removed by vacuum distillation, and water and ethyl acetate were added for extraction. The solvent was removed by vacuum distillation to obtain 42 mg of a light yellow solid with a yield of 22%, i.e., the 2-(1-amino-3-nitro-1H-1,2,4-triazol-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

[0093]

[0094] In summary, the above are only preferred embodiments of the present invention and are not intended to limit the protection scope of the present invention. Any modifications, equivalent substitutions, improvements, etc. made within the spirit and principles of the present invention should be included in the protection scope of the present invention.

Claims

1. A polynitrogen fused ring compound, characterized in that: The polynitrogen fused ring compound is 2-(1-amino-1H-1,2,3,4-tetrazolyl-5-yl)-3,5-dihydro-tetrazolyl[1,2,3,4][1,5-d]tetrazolyl, and its structural formula is:

2. A method for preparing the polynitrogen fused ring compound according to claim 1, characterized in that The steps of the method include: The first step is to prepare a nitrotriazole-substituted hydrazine intermediate; its structural formula is: In the second step, the nitrotriazole-substituted hydrazine intermediate prepared in the first step, a base and an organic solvent are mixed, reacted at 40-100° C. for 0.5-2 h, then restored to room temperature, an amination reagent is added, reacted at room temperature for 0.5-12 h, and the organic solvent is removed by distillation under reduced pressure to obtain the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

3. The method for preparing a polynitrogen fused ring compound according to claim 2, characterized in that: In the first step, the structural formula of the prepared nitrotriazole-substituted hydrazine intermediate is:

4. The method for preparing a polynitrogen fused ring compound according to claim 2, characterized in that: In the second step, the organic solvent is at least one of acetonitrile, ethanol and tetrahydrofuran; In the second step, the base is at least one of sodium hydroxide, sodium bicarbonate, and sodium carbonate; The amination reagent is Hydroxylamine-O-sulfonic acid, At least one of, wherein R = The molar ratio of the nitrotriazole-substituted hydrazine intermediate to the base is 1:2-6; The volume ratio of the molar mass of the nitrotriazole-substituted hydrazine intermediate to the organic solvent is 1:3 to 10; The ratio of the nitrotriazole-substituted hydrazine intermediate to the amination reagent is 1:2-4.

5. A method for preparing the polynitrogen fused ring compound according to claim 1, characterized in that The steps of the method include: The first step is to prepare a nitrotriazole-substituted hydrazine intermediate; In the second step, the nitrotriazole-substituted hydrazine intermediate prepared in the first step, a base and an organic solvent are mixed, reacted at 40-100° C. for 0.5-2 h, then restored to room temperature, an amination reagent is added, reacted at room temperature for 0.5-12 h, an oxidant is added, reacted for 1-12 h, and the organic solvent is removed by reduced pressure distillation to obtain the 2-(1-amino-3-nitro-1H-1,2,4-triazole-5-yl)-6-nitro-3,5-dihydro-triazolo[1,2,4][1,5-d]tetrazolyl compound.

6. The method for preparing a polynitrogen fused ring compound according to claim 5, characterized in that: In the first step, the structural formula of the prepared nitrotriazole-substituted hydrazine intermediate is:

7. The method for preparing a polynitrogen fused ring compound according to claim 5, characterized in that: In the second step, the organic solvent is at least one of acetonitrile, ethanol and tetrahydrofuran; In the second step, the base is at least one of sodium hydroxide, sodium bicarbonate, and sodium carbonate; The amination reagent is Hydroxylamine-O-sulfonic acid, At least one of, wherein R = The oxidant is at least one of N-bromosuccinimide, tert-butyl hypochlorite, and dibromoisocyanuric acid; The molar ratio of the nitrotriazole-substituted hydrazine intermediate to the base is 1:2-6; The volume ratio of the molar mass of the nitrotriazole-substituted hydrazine intermediate to the organic solvent is 1:3 to 10; The molar mass ratio of the nitrotriazole-substituted hydrazine intermediate to the amination reagent is 1:2-4; The molar mass ratio of the nitrotriazole-substituted hydrazine intermediate to the oxidant is 1:1.8-4.

8. The method for preparing a polynitrogen fused ring compound according to claim 2 or 5, characterized in that: In the first step, the method for preparing the nitrotriazole-substituted hydrazine intermediate is: A nitro-substituted triazole azo compound, a metal reducing agent and an organic solvent are mixed, and the reaction is carried out at 50 to 100° C. for 4 to 12 hours. After the reaction is completed, the mixture is filtered, and the liquid phase is extracted with an organic solvent to remove the organic solvent to obtain a nitrotriazole-substituted hydrazine intermediate. The structural formula of the nitro-substituted triazole azo compound is: The metal reducing agent is metal magnesium or zinc; The ratio of the molar mass of the nitro-substituted triazole azo compound, the molar mass of the metal reducing agent and the volume of the organic solvent is 1:4-6:6-10.

9. The method for preparing a polynitrogen fused ring compound according to claim 2 or 5, characterized in that: In the first step, the method for preparing the nitrotriazole-substituted hydrazine intermediate is: A nitro-substituted triazole azo compound, a metal hydride reducing agent and an organic solvent are mixed, and the reaction is carried out at 50 to 100° C. for 4 to 12 hours. After the reaction is completed, the mixture is filtered, and the liquid phase is extracted with an organic solvent to remove the organic solvent to obtain a nitrotriazole-substituted hydrazine intermediate. The metal hydride reducing agent is borane, sodium borohydride or lithium aluminum hydride; The organic solvent is at least one of acetonitrile, ethanol and tetrahydrofuran; The ratio of the molar mass of the nitro-substituted triazole azo compound, the molar mass of the metal hydride reducing agent and the volume of the organic solvent is 1:4-6:6-10.

10. The method for preparing a polynitrogen fused ring compound according to claim 2 or 5, characterized in that: In the first step, the method for preparing the nitrotriazole-substituted hydrazine intermediate is: A nitro-substituted triazole azo compound, a base, a hydrazine reducing agent and an organic solvent are mixed, and the reaction is carried out at 10 to 50° C. for 4 to 12 hours. After the reaction is completed, the mixture is filtered, and the liquid phase is extracted with an organic solvent to remove the organic solvent to obtain a nitrotriazole-substituted hydrazine intermediate; The hydrazine reducing agent is hydrazine hydrate or hydrazine generated in situ; The ratio of the molar mass of the nitro-substituted triazole azo compound, the molar mass of the base, the molar mass of the hydrazine reducing agent and the volume of the organic solvent is 1:2-4:4-6:6-10.

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