CN115744841A - Nickel-based nitride nano combustion catalyst and preparation method thereof - Google Patents
Nickel-based nitride nano combustion catalyst and preparation method thereof Download PDFInfo
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- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 title claims abstract description 136
- 238000002485 combustion reaction Methods 0.000 title claims abstract description 67
- 239000003054 catalyst Substances 0.000 title claims abstract description 66
- 150000004767 nitrides Chemical class 0.000 title claims abstract description 40
- 229910052759 nickel Inorganic materials 0.000 title claims abstract description 38
- 238000002360 preparation method Methods 0.000 title claims abstract description 24
- 239000002243 precursor Substances 0.000 claims abstract description 38
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 21
- 238000000137 annealing Methods 0.000 claims abstract description 15
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 14
- 150000003624 transition metals Chemical class 0.000 claims abstract description 14
- 238000000034 method Methods 0.000 claims abstract description 13
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims abstract description 6
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 6
- 239000011651 chromium Substances 0.000 claims abstract description 6
- 239000011733 molybdenum Substances 0.000 claims abstract description 6
- 229910052750 molybdenum Inorganic materials 0.000 claims abstract description 6
- 229910052720 vanadium Inorganic materials 0.000 claims abstract description 6
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims abstract description 6
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 27
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 20
- 238000005121 nitriding Methods 0.000 claims description 18
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 13
- 239000004202 carbamide Substances 0.000 claims description 13
- 150000002815 nickel Chemical class 0.000 claims description 13
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 12
- 229910052786 argon Inorganic materials 0.000 claims description 10
- 229910021529 ammonia Inorganic materials 0.000 claims description 9
- 239000000843 powder Substances 0.000 claims description 9
- 239000002994 raw material Substances 0.000 claims description 9
- 239000012300 argon atmosphere Substances 0.000 claims description 6
- 239000012298 atmosphere Substances 0.000 claims description 6
- 239000008367 deionised water Substances 0.000 claims description 6
- 229910021641 deionized water Inorganic materials 0.000 claims description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 6
- 239000007789 gas Substances 0.000 claims description 5
- 238000001816 cooling Methods 0.000 claims description 4
- 238000001035 drying Methods 0.000 claims description 4
- 239000002244 precipitate Substances 0.000 claims description 4
- 239000000047 product Substances 0.000 claims description 4
- 238000005406 washing Methods 0.000 claims description 4
- 229910017855 NH 4 F Inorganic materials 0.000 claims description 3
- MQRWBMAEBQOWAF-UHFFFAOYSA-N acetic acid;nickel Chemical compound [Ni].CC(O)=O.CC(O)=O MQRWBMAEBQOWAF-UHFFFAOYSA-N 0.000 claims description 3
- ZCDOYSPFYFSLEW-UHFFFAOYSA-N chromate(2-) Chemical compound [O-][Cr]([O-])(=O)=O ZCDOYSPFYFSLEW-UHFFFAOYSA-N 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- MEFBJEMVZONFCJ-UHFFFAOYSA-N molybdate Chemical compound [O-][Mo]([O-])(=O)=O MEFBJEMVZONFCJ-UHFFFAOYSA-N 0.000 claims description 3
- 229940078494 nickel acetate Drugs 0.000 claims description 3
- BMGNSKKZFQMGDH-FDGPNNRMSA-L nickel(2+);(z)-4-oxopent-2-en-2-olate Chemical compound [Ni+2].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O BMGNSKKZFQMGDH-FDGPNNRMSA-L 0.000 claims description 3
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 claims description 3
- 238000000926 separation method Methods 0.000 claims description 3
- LSGOVYNHVSXFFJ-UHFFFAOYSA-N vanadate(3-) Chemical compound [O-][V]([O-])([O-])=O LSGOVYNHVSXFFJ-UHFFFAOYSA-N 0.000 claims description 3
- 239000002135 nanosheet Substances 0.000 abstract description 28
- 230000000694 effects Effects 0.000 abstract description 5
- 229910000480 nickel oxide Inorganic materials 0.000 abstract description 5
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 abstract description 5
- OLBVUFHMDRJKTK-UHFFFAOYSA-N [N].[O] Chemical compound [N].[O] OLBVUFHMDRJKTK-UHFFFAOYSA-N 0.000 abstract description 3
- 238000003421 catalytic decomposition reaction Methods 0.000 abstract description 3
- 230000009286 beneficial effect Effects 0.000 abstract 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 8
- 239000003380 propellant Substances 0.000 description 7
- 238000002441 X-ray diffraction Methods 0.000 description 6
- 230000003197 catalytic effect Effects 0.000 description 6
- 238000000635 electron micrograph Methods 0.000 description 5
- 229910052757 nitrogen Inorganic materials 0.000 description 5
- 230000001105 regulatory effect Effects 0.000 description 4
- 239000004449 solid propellant Substances 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- 239000002086 nanomaterial Substances 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 2
- 230000001276 controlling effect Effects 0.000 description 2
- 238000001938 differential scanning calorimetry curve Methods 0.000 description 2
- XTFIVUDBNACUBN-UHFFFAOYSA-N 1,3,5-trinitro-1,3,5-triazinane Chemical compound [O-][N+](=O)N1CN([N+]([O-])=O)CN([N+]([O-])=O)C1 XTFIVUDBNACUBN-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 239000000028 HMX Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000007806 chemical reaction intermediate Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- -1 cobalt nitride Chemical class 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 229910001882 dioxygen Inorganic materials 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000002737 fuel gas Substances 0.000 description 1
- 239000000543 intermediate Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- DOTMOQHOJINYBL-UHFFFAOYSA-N molecular nitrogen;molecular oxygen Chemical compound N#N.O=O DOTMOQHOJINYBL-UHFFFAOYSA-N 0.000 description 1
- UZGLIIJVICEWHF-UHFFFAOYSA-N octogen Chemical compound [O-][N+](=O)N1CN([N+]([O-])=O)CN([N+]([O-])=O)CN([N+]([O-])=O)C1 UZGLIIJVICEWHF-UHFFFAOYSA-N 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 230000027756 respiratory electron transport chain Effects 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
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Abstract
The invention discloses a nickel-based nitride nano combustion catalyst and a preparation method thereof, wherein the nickel-based nitride nano combustion catalyst comprises Ni 3 N-nano combustion catalyst, O-doped Ni 3 N nano combustion catalyst and molybdenum, vanadium or chromium doped Ni 3 A N nano combustion catalyst; the nickel-based nitride nano combustion catalyst is prepared by adopting a precursor of a high-temperature nitridation NiO nano sheet, the NiO nano sheet is prepared by combining hydrothermal synthesis with a high-temperature annealing method, the adjustment of the oxygen-nitrogen ratio is realized by changing the nitridation temperature, and the bimetallic structure is realized by introducing other transition metal precursors into a hydrothermal reaction solution. Compared with the traditional nickel oxide, the invention is beneficial to improving the activity of the catalyst, can better match the HATO energy level structure and realizes high-efficiency catalytic decomposition.
Description
Technical Field
The invention belongs to the field of solid propellants, relates to a combustion catalyst, and particularly relates to a nickel-based nitride nano combustion catalyst and a preparation method thereof.
Background
Increased safety is a necessary requirement for the development of solid propellant technology. 5,5 '-bistetrazole-1, 1' -dioxygen dihydroxylamine salt (HATO) is adopted to replace hexogen or octogen, and is an effective way for improving the safety of the propellant. However, the introduction of HATO significantly improves the safety performance of the propellant and also causes the combustion performance of the propellant to be deteriorated, the burning rate and pressure index to be greatly increased, and then disintegration and explosion occur in the working process of the engine. This has become a key bottleneck problem that restricts the practical application of such solid propellants.
The combustion catalyst is the most common method for adjusting and improving the combustion performance of the propellant, and the burning rate pressure index of the propellant can be controllably adjusted within a wider pressure intensity range. However, as the solid rocket propellant is further developed towards high energy, clean fuel gas and controllable combustion, the catalytic efficiency of the existing combustion catalyst is difficult to meet the requirement of the high-performance solid propellant, and a new combustion catalytic material system with high activity and high selectivity needs to be developed urgently.
Generally, the catalytic activity of a combustion catalyst is related to its geometry and electronic structure, which involves activation of energetic molecules and adsorption of reaction intermediates that participate in the catalytic reaction. For transition metals, the adsorption strength of the intermediate species catalytically decomposed by the energetic molecule depends on the d-band center of the transition metal. Ni has a variable valence state, which allows Ni to regulate its electronic structure by coordinating with different electronegative elements such as carbon, nitrogen, oxygen, etc. Therefore, if the d band center of Ni is adjusted to a reasonable position, ni can be adjusted to a highly active combustion catalyst active site.
Changing the coordination environment of the metal is an effective method for regulating and controlling the electronic structure of the center of the active metal. For energetic molecules, nitrogen is often present in the structure. Therefore, the nitrogen element is introduced into the catalyst, so that the adsorption capacity of the catalytic active center on energetic molecules can be improved. On the basis, the d-band central position of Ni can be effectively regulated and controlled by regulating the oxygen nitrogen ratio in the coordination atoms, so that the catalytic activity of the Ni is improved.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a nickel-based nitride nano combustion catalyst and a preparation method thereof, wherein the catalyst utilizes the energy difference between d energy bands of different transition metals and Ni and the influence of coordination environment on the d band structure of Ni, and moves the valence band structure of nickel-based nitride by adjusting nitrogen-oxygen ratio and interface polarization effect, so that the performance of the metal nitride for combustion catalysis is regulated and controlled, and the efficient catalytic decomposition of typical energetic molecules such as HATO and the like is realized.
In order to solve the technical problems, the invention adopts the following technical scheme:
a preparation method of a nickel-based nitride nano combustion catalyst comprises the following steps:
step 1, raw materials of nickel salt, urea and NH 4 F, mixing and carrying out hydrothermal reaction at the temperature of 120 ℃ for 9h; cooling to room temperature, performing centrifugal separation, washing the centrifugal precipitate with deionized water and ethanol for three times, and drying in a vacuum oven at 60 deg.C for more than 12 hr to obtain green powder product;
and 3, nitriding the precursor prepared in the step 2 in an ammonia atmosphere to obtain the nickel-based nitride nano combustion catalyst.
The invention also comprises the following technical characteristics:
specifically, the nickel salt in step 1 is one of nickel nitrate, nickel acetate and nickel acetylacetonate.
Specifically, the nickel salt, urea and NH 4 The molar ratio of F is 1: (2-5): (1-3).
Specifically, the annealing temperature in the step 2 is 300-650 ℃, and the flow rate of argon gas is 100-300 mL/min.
Specifically, the nitriding temperature in the step 3 is 350-600 ℃, the nitriding time is 2 hours, the ammonia gas flow rate is 80-180 mL/min, and the prepared nickel-based nitride nano-combustion catalyst is Ni 3 N nanometer combustion catalyst.
Specifically, the nitridation temperature in the step 3 is 350 ℃, the nitridation time is 1.5h, the ammonia gas flow rate is 80-180 mL/min, and the prepared nickel-based nitride nano-combustion catalyst is O-doped Ni 3 N nanometer combustion catalyst.
Specifically, in the step 1, the raw material for the hydrothermal reaction further includes a transition metal precursor, the transition metal precursor is one of molybdate, vanadate and chromate, and the nickel-based nitride nano-combustion catalyst prepared according to the step of claim 2 is Ni-doped with molybdenum, vanadium or chromium 3 N nanometer combustion catalyst.
Specifically, in the raw materials of the hydrothermal reaction in the step 1, nickel salt, a transition metal precursor, urea and NH 4 The molar ratio of F is 1:0.1: (2-5): (1-3).
Specifically, the annealing temperature in the step 2 is 300-650 ℃, and the flow rate of argon gas is 100-300 mL/min; the nitriding temperature in the step 3 is 350-600 ℃, the nitriding time is 2h, and the ammonia gas flow rate is 80-180 mL/min.
The nickel-based nitride nanometer combustion catalyst is prepared by adopting the preparation method of the nickel-based nitride nanometer combustion catalyst.
Compared with the prior art, the invention has the following technical effects:
(1) According to the invention, the cobalt nitride is obtained by performing high-temperature nitridation treatment on the nickel oxide, and compared with the traditional nickel oxide, the nitrogen has more unpaired electrons which can provide more unoccupied d orbitals, so that the catalyst activity is improved.
(2) The invention passes through the pair of Ni 3 The N is doped to realize effective regulation and control of d-orbit energy, the HATO energy level structure can be better matched, and efficient catalytic decomposition is realized.
(3) The nickel-based nitride preparation method provided by the invention is simple, raw materials are easy to obtain, the preparation is easy to amplify, and the engineering application is favorably realized.
Drawings
FIG. 1 shows Ni 3 N electron micrographAnd XRD pattern;
FIG. 2 is O-doped Ni 3 N electron micrograph and XRD pattern;
FIG. 3 is Mo doped Ni 3 An electron micrograph and XRD pattern of N;
fig. 4 is a DSC curve of nickel-based nitrides and commercial nickel oxide mixed with HATO.
Detailed Description
The invention provides a nickel-based nitride nano combustion catalyst and a preparation method thereof, wherein the nickel-based nitride nano combustion catalyst comprises Ni 3 N nano combustion catalyst, O doped Ni 3 N nano combustion catalyst and molybdenum, vanadium or chromium doped Ni 3 A N nano combustion catalyst; the nickel-based nitride nanometer combustion catalyst is prepared by adopting a precursor of high-temperature nitridation NiO nano-sheets, the NiO nano-sheets are prepared by combining hydrothermal synthesis with a high-temperature annealing method, the adjustment of the oxygen-nitrogen ratio is realized by changing the nitridation temperature, and the bimetallic structure is realized by introducing other transition metal precursors into a hydrothermal reaction solution. Specifically, the preparation method comprises the following steps:
step 1, ni (OH) 2 Preparing a nanosheet precursor:
preparation of Ni (OH) by hydrothermal method 2 Nanosheet, and raw materials for hydrothermal method comprise nickel salt, urea and NH 4 F, controlling the hydrothermal reaction temperature to be 120 ℃ and the reaction time to be 9h; cooling to room temperature, centrifuging, washing the precipitate with deionized water and ethanol for three times, and drying in a vacuum oven at 60 deg.C for more than 12 hr to obtain powder Ni (OH) 2 A nanosheet; the nickel salt in the step 1 is one of nickel nitrate, nickel acetate and nickel acetylacetonate, and the content is 0.5-2 mmol;
mixing the Ni (OH) obtained in the step 1 2 Annealing the nanosheets in an argon atmosphere for 2 hours to obtain a NiO precursor;
step 3, high-temperature nitridation of the NiO nano sheet precursor:
and (3) nitriding the NiO precursor prepared in the step (2) in an ammonia atmosphere to obtain the nickel-based nitride nano combustion catalyst.
When preparing Ni 3 Nickel salt, urea and NH in step 1 when N is a nano combustion catalyst 4 The molar ratio of F is 1: (2-5): (1-3); the annealing temperature in the step 2 is 300-650 ℃, and the flow rate of argon is 100-300 mL/min; the nitriding temperature in the step 3 is 350-600 ℃, the nitriding time is 2h, the ammonia gas flow rate is 80-180 mL/min, and the prepared nickel-based nitride nano-combustion catalyst is Ni 3 N nanometer combustion catalyst.
When preparing O-doped Ni 3 Nickel salt, urea and NH in step 1 when N is a nano combustion catalyst 4 The molar ratio of F is 1: (2-5): (1-3); the annealing temperature in the step 2 is 300-650 ℃, and the flow rate of argon gas is 100-300 mL/min; the nitridation temperature in the step 3 is 350 ℃, the nitridation time is 1.5h, the ammonia gas flow rate is 80-180 mL/min, and the prepared nickel-based nitride nano combustion catalyst is O-doped Ni 3 N nanometer combustion catalyst.
When preparing Ni doped with molybdenum, vanadium or chromium 3 When the catalyst is an N nano combustion catalyst, in the step 1, the raw materials of the hydrothermal method further comprise a transition metal precursor, wherein the transition metal precursor is one of molybdate, vanadate and chromate, nickel salt, the transition metal precursor, urea and NH 4 The molar ratio of F is 1:0.1: (2-5): (1-3) Mo-doped Ni (OH) can be obtained by the above step 1 2 A nanosheet precursor; the annealing temperature in the step 2 is 300-650 ℃, the argon flow rate is 100-300 mL/min, and a Mo-doped NiO nano sheet precursor is obtained through the step 2; the nitridation temperature in the step 3 is 350-600 ℃, the nitridation time is 2h, the ammonia gas flow rate is 80-180 mL/min, and the prepared nickel-based nitride nano combustion catalyst is Ni doped with molybdenum, vanadium or chromium 3 N nanometer combustion catalyst.
The following embodiments are given as examples of the present invention, and it should be noted that the present invention is not limited to the following embodiments, and all equivalent changes based on the technical solutions of the present invention are included in the protection scope of the present invention.
Example 1: ni 3 Preparation of N nano combustion catalyst
Step 1, ni (OH) 2 Preparing a nanosheet precursor:
preparation of Ni (OH) by hydrothermal method 2 The nano-sheets, the hydrothermal reaction solution comprises 1mmol Ni (NO) 3 ) 2 ·6H 2 O, 4.4mmol of Urea CO (NH) 2 ) 2 And 1.8mmol of NH 4 And (3) carrying out hydrothermal reaction at 120 ℃ for 9 hours, cooling to room temperature, carrying out centrifugal separation on the sample, washing the centrifugal precipitate with deionized water and ethanol for three times, and drying in a vacuum oven at 60 ℃ for more than 12 hours to obtain green powder Ni (OH) 2 。
The green powder Ni (OH) prepared in the step 1 is added 2 Further, annealing was carried out at 400 ℃ for 2 hours in an argon atmosphere (argon flow rate: 150 mL/min), thereby preparing a precursor of NiO.
Step 3, high-temperature nitridation of NiO nano sheet precursor
Nitriding the NiO precursor prepared in the step 2 in an ammonia atmosphere at 400 ℃ (ammonia flow rate is 120 mL/min.) for 2 hours to prepare Ni 3 And (3) N nano material.
Example 2: o doping with Ni 3 Preparation of N nano combustion catalyst
Step 1, ni (OH) 2 Preparation of nanosheet precursor
Preparation of Ni (OH) by hydrothermal method 2 The nano-sheets, the hydrothermal reaction solution comprises 1mmol Ni (NO) 3 ) 2 ·6H 2 O, 4.4mmol of Urea CO (NH) 2 ) 2 And 1.8mmol of NH 4 The solution F is reacted at the hydrothermal temperature of 120 ℃ for 9 hours, cooled to room temperature, centrifugally separated, washed with deionized water and ethanol for three times, and then dried in a vacuum oven at the temperature of 60 ℃ for more than 12 hours to obtain green powder Ni (OH) 2 。
The green powder Ni (OH) prepared in the step 1 is added 2 Further annealing at 400 ℃ in an argon atmosphere (argon flow rate of 150 mL/min) for 2 hours before NiO is preparedAnd (4) driving the body.
Step 3, high-temperature nitridation of NiO nano-sheet precursor
Nitriding the NiO precursor prepared in the step 2 in an ammonia atmosphere at 350 ℃ (the ammonia flow rate is 120 mL/min.) for 1.5 hours to prepare O-doped Ni 3 And (3) N nano materials.
Example 3: mo doped Ni 3 Preparation of N nano combustion catalyst
Step 1, mo doping with Ni (OH) 2 Preparing a nanosheet precursor:
preparation of Ni (OH) by hydrothermal method 2 The nano-sheets, the hydrothermal reaction solution comprises 1mmol Ni (NO) 3 ) 2 ·6H 2 O、0.1mmolNa 2 MoO 4 ·2H 2 O, 5mmol of Urea CO (NH) 2 ) 2 And 2.5mmol of NH 4 The solution F is reacted at the hydrothermal temperature of 120 ℃ for 9 hours, cooled to room temperature, centrifugally separated, washed with deionized water and ethanol for three times, and then dried in a vacuum oven at the temperature of 60 ℃ for more than 12 hours to obtain green powder Mo-doped Ni (OH) 2 。
the green powder Ni (OH) prepared in the step 1 is added 2 Further annealing for 2 hours at 450 ℃ in an argon atmosphere (the argon flow rate is 120 mL/min) to prepare a Mo-doped NiO precursor.
Step 3, high-temperature nitridation of the Mo-doped NiO nano sheet precursor:
nitriding the NiO precursor prepared in the step 2 in an ammonia atmosphere at 400 ℃ (ammonia flow rate is 100 mL/min.) for 2 hours to prepare Mo-doped Ni 3 And (3) N nano material.
The preparation results of the above examples are characterized as follows:
FIG. 1 shows Ni 3 An electron micrograph and XRD pattern of N, ni is shown in FIG. 1 3 The shape of N is a two-dimensional ultrathin nanosheet. FIG. 2 is O-doped Ni 3 The electron micrograph and XRD pattern of N show that, as shown in FIG. 2, O is uniformly distributed in Ni 3 In the N nanosheet, the doping of O does not influence Ni 3 And the stability of the sample structure is ensured by the N lattice constant. FIG. 3 is Mo doped Ni 3 In the electron micrograph and XRD pattern of N, it can be seen from FIG. 3 that Mo is uniformly distributed in Ni 3 Forming MoO in N nano sheet on surface 2 And Ni 3 N heterojunction, mo doping does not affect Ni 3 The morphology of the N nanosheet. FIG. 4 is a DSC curve of nickel-based nitrides and commercial nickel oxides mixed with HATO, and it can be seen from FIG. 4 that Ni prepared in examples 1-3 was compared with NiO 3 The N sample can greatly reduce the decomposition temperature of HATO, shows good catalytic activity, and can greatly improve the heat release of HATO by doping Mo, because of MoO 2 And Ni 3 The heterojunction of N has improved electron transfer efficiency, and it is more thorough to decompose to be favorable to promoting the combustion efficiency of propellant.
Claims (10)
1. The preparation method of the nickel-based nitride nano-combustion catalyst is characterized by comprising the following steps of:
step 1, raw materials of nickel salt, urea and NH 4 F, mixing and carrying out hydrothermal reaction at the temperature of 120 ℃ for 9h; cooling to room temperature, performing centrifugal separation, washing the centrifugal precipitate with deionized water and ethanol for three times, and drying in a vacuum oven at 60 deg.C for more than 12 hr to obtain green powder product;
step 2, annealing the product obtained in the step 1 in an argon atmosphere for 2 hours to obtain a precursor;
and 3, nitriding the precursor prepared in the step 2 in an ammonia atmosphere to obtain the nickel-based nitride nano combustion catalyst.
2. The method for preparing the nickel-based nitride nano-combustion catalyst according to claim 1, wherein the nickel salt in the step 1 is one of nickel nitrate, nickel acetate and nickel acetylacetonate.
3. The method of preparing the nickel-based nitride nano-combustion catalyst according to claim 2, wherein the nickel salt, urea andNH 4 the molar ratio of F is 1: (2-5): (1-3).
4. The method for preparing the nickel-based nitride nano-combustion catalyst according to claim 3, wherein the annealing temperature in the step 2 is 300 to 650 ℃, and the flow rate of argon gas is 100 to 300mL/min.
5. The method for preparing the nickel-based nitride nano-combustion catalyst according to claim 4, wherein the nitriding temperature in the step 3 is 350 to 600 ℃, the nitriding time is 2 hours, the ammonia gas flow rate is 80 to 180mL/min, and the prepared nickel-based nitride nano-combustion catalyst is Ni 3 N nanometer combustion catalyst.
6. The method for preparing the nickel-based nitride nano-combustion catalyst according to claim 4, wherein the nitriding temperature in the step 3 is 350 ℃, the nitriding time is 1.5h, and the ammonia gas flow rate is 80-180 mL/min, and the prepared nickel-based nitride nano-combustion catalyst is O-doped Ni 3 N nanometer combustion catalyst.
7. The method of claim 2, wherein in the step 1, the hydrothermal reaction raw material further comprises a transition metal precursor, the transition metal precursor is one of molybdate, vanadate and chromate, and the Ni-based nitride nano-combustion catalyst prepared according to the step of claim 2 is Ni-doped with molybdenum, vanadium or chromium 3 N nanometer combustion catalyst.
8. The method for preparing the nickel-based nitride nano-combustion catalyst according to claim 7, wherein the raw materials of the hydrothermal reaction of the step 1 include nickel salt, a transition metal precursor, urea, and NH 4 The molar ratio of F is 1:0.1: (2-5): (1-3).
9. The method for preparing the nickel-based nitride nano-combustion catalyst according to claim 8, wherein the annealing temperature in the step 2 is 300 to 650 ℃, and the flow rate of argon gas is 100 to 300mL/min; the nitriding temperature in the step 3 is 350-600 ℃, the nitriding time is 2h, and the ammonia gas flow rate is 80-180 mL/min.
10. A nickel-based nitride nano-combustion catalyst, which is characterized by being prepared by the preparation method of the nickel-based nitride nano-combustion catalyst according to any one of claims 5 to 7.
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