CN109331861B - Platinum alloy-based tantalum compound electrocatalyst and preparation method and application thereof - Google Patents
Platinum alloy-based tantalum compound electrocatalyst and preparation method and application thereof Download PDFInfo
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- CN109331861B CN109331861B CN201811446655.6A CN201811446655A CN109331861B CN 109331861 B CN109331861 B CN 109331861B CN 201811446655 A CN201811446655 A CN 201811446655A CN 109331861 B CN109331861 B CN 109331861B
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- 150000003482 tantalum compounds Chemical class 0.000 title claims abstract description 53
- 229910001260 Pt alloy Inorganic materials 0.000 title claims abstract description 34
- 239000010411 electrocatalyst Substances 0.000 title claims abstract description 30
- 238000002360 preparation method Methods 0.000 title claims abstract description 18
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 47
- 239000001257 hydrogen Substances 0.000 claims abstract description 41
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 39
- 238000006243 chemical reaction Methods 0.000 claims abstract description 39
- 229910000510 noble metal Inorganic materials 0.000 claims abstract description 19
- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 claims abstract description 17
- 229910052715 tantalum Inorganic materials 0.000 claims abstract description 16
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims abstract description 15
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000000956 alloy Substances 0.000 claims abstract description 9
- 229910045601 alloy Inorganic materials 0.000 claims abstract description 8
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910001936 tantalum oxide Inorganic materials 0.000 claims abstract description 4
- 229910017052 cobalt Inorganic materials 0.000 claims abstract description 3
- 239000010941 cobalt Substances 0.000 claims abstract description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims abstract description 3
- 229910052751 metal Inorganic materials 0.000 claims abstract description 3
- 239000002184 metal Substances 0.000 claims abstract description 3
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 45
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 39
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims description 31
- 229910052700 potassium Inorganic materials 0.000 claims description 31
- 239000011591 potassium Substances 0.000 claims description 31
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical group [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 claims description 26
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 22
- 238000012360 testing method Methods 0.000 claims description 22
- 239000003792 electrolyte Substances 0.000 claims description 17
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 16
- 229910052799 carbon Inorganic materials 0.000 claims description 16
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims description 15
- 239000007864 aqueous solution Substances 0.000 claims description 13
- 238000001035 drying Methods 0.000 claims description 13
- 239000001103 potassium chloride Substances 0.000 claims description 13
- 235000011164 potassium chloride Nutrition 0.000 claims description 13
- 239000002243 precursor Substances 0.000 claims description 13
- 239000008367 deionised water Substances 0.000 claims description 12
- 229910021641 deionized water Inorganic materials 0.000 claims description 12
- NROKBHXJSPEDAR-UHFFFAOYSA-M potassium fluoride Chemical group [F-].[K+] NROKBHXJSPEDAR-UHFFFAOYSA-M 0.000 claims description 12
- 238000005406 washing Methods 0.000 claims description 12
- 229910021529 ammonia Inorganic materials 0.000 claims description 10
- 239000012153 distilled water Substances 0.000 claims description 10
- 238000001291 vacuum drying Methods 0.000 claims description 10
- 238000000227 grinding Methods 0.000 claims description 8
- 150000007529 inorganic bases Chemical class 0.000 claims description 8
- 239000004570 mortar (masonry) Substances 0.000 claims description 8
- 239000012299 nitrogen atmosphere Substances 0.000 claims description 8
- KLFRPGNCEJNEKU-FDGPNNRMSA-L (z)-4-oxopent-2-en-2-olate;platinum(2+) Chemical group [Pt+2].C\C([O-])=C\C(C)=O.C\C([O-])=C\C(C)=O KLFRPGNCEJNEKU-FDGPNNRMSA-L 0.000 claims description 7
- 239000012298 atmosphere Substances 0.000 claims description 7
- 238000001354 calcination Methods 0.000 claims description 7
- 150000001450 anions Chemical class 0.000 claims description 6
- 229910001510 metal chloride Inorganic materials 0.000 claims description 6
- 229910001512 metal fluoride Inorganic materials 0.000 claims description 6
- 239000011259 mixed solution Substances 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 6
- 239000011698 potassium fluoride Substances 0.000 claims description 6
- 235000003270 potassium fluoride Nutrition 0.000 claims description 6
- 239000000243 solution Substances 0.000 claims description 6
- FJDJVBXSSLDNJB-LNTINUHCSA-N cobalt;(z)-4-hydroxypent-3-en-2-one Chemical compound [Co].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O FJDJVBXSSLDNJB-LNTINUHCSA-N 0.000 claims description 5
- 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 5
- 150000003839 salts Chemical class 0.000 claims description 5
- 150000003057 platinum Chemical class 0.000 claims description 4
- CLSUSRZJUQMOHH-UHFFFAOYSA-L platinum dichloride Chemical compound Cl[Pt]Cl CLSUSRZJUQMOHH-UHFFFAOYSA-L 0.000 claims description 4
- 238000001914 filtration Methods 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 2
- 239000003513 alkali Substances 0.000 claims description 2
- 229940011182 cobalt acetate Drugs 0.000 claims description 2
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 2
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 2
- 229910000361 cobalt sulfate Inorganic materials 0.000 claims description 2
- 229940044175 cobalt sulfate Drugs 0.000 claims description 2
- KTVIXTQDYHMGHF-UHFFFAOYSA-L cobalt(2+) sulfate Chemical compound [Co+2].[O-]S([O-])(=O)=O KTVIXTQDYHMGHF-UHFFFAOYSA-L 0.000 claims description 2
- QAHREYKOYSIQPH-UHFFFAOYSA-L cobalt(II) acetate Chemical compound [Co+2].CC([O-])=O.CC([O-])=O QAHREYKOYSIQPH-UHFFFAOYSA-L 0.000 claims description 2
- 229940078494 nickel acetate Drugs 0.000 claims description 2
- LGQLOGILCSXPEA-UHFFFAOYSA-L nickel sulfate Chemical compound [Ni+2].[O-]S([O-])(=O)=O LGQLOGILCSXPEA-UHFFFAOYSA-L 0.000 claims description 2
- 229910000363 nickel(II) sulfate Inorganic materials 0.000 claims description 2
- 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 2
- 238000003756 stirring Methods 0.000 claims description 2
- 230000003197 catalytic effect Effects 0.000 abstract description 12
- 238000000034 method Methods 0.000 abstract description 12
- 239000013078 crystal Substances 0.000 abstract description 11
- 239000002105 nanoparticle Substances 0.000 abstract description 4
- 230000002195 synergetic effect Effects 0.000 abstract description 3
- 239000003054 catalyst Substances 0.000 description 52
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 25
- 229910002837 PtCo Inorganic materials 0.000 description 24
- 229910002844 PtNi Inorganic materials 0.000 description 23
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 20
- 229910003071 TaON Inorganic materials 0.000 description 15
- 238000005868 electrolysis reaction Methods 0.000 description 13
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 12
- 239000006185 dispersion Substances 0.000 description 12
- 229920000557 Nafion® Polymers 0.000 description 8
- 238000011056 performance test Methods 0.000 description 8
- 229910021607 Silver chloride Inorganic materials 0.000 description 7
- 239000004744 fabric Substances 0.000 description 7
- 238000004519 manufacturing process Methods 0.000 description 7
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 7
- 235000019441 ethanol Nutrition 0.000 description 6
- 239000000463 material Substances 0.000 description 6
- 229910052757 nitrogen Inorganic materials 0.000 description 6
- 238000003786 synthesis reaction Methods 0.000 description 6
- 238000001075 voltammogram Methods 0.000 description 6
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 5
- 238000009210 therapy by ultrasound Methods 0.000 description 5
- 238000004832 voltammetry Methods 0.000 description 5
- 229910000990 Ni alloy Inorganic materials 0.000 description 4
- 239000007809 chemical reaction catalyst Substances 0.000 description 4
- 239000002073 nanorod Substances 0.000 description 4
- PCLURTMBFDTLSK-UHFFFAOYSA-N nickel platinum Chemical compound [Ni].[Pt] PCLURTMBFDTLSK-UHFFFAOYSA-N 0.000 description 4
- 229910052697 platinum Inorganic materials 0.000 description 4
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- CLBRCZAHAHECKY-UHFFFAOYSA-N [Co].[Pt] Chemical compound [Co].[Pt] CLBRCZAHAHECKY-UHFFFAOYSA-N 0.000 description 3
- 230000004913 activation Effects 0.000 description 3
- 239000012670 alkaline solution Substances 0.000 description 3
- 238000012512 characterization method Methods 0.000 description 3
- 239000000460 chlorine Substances 0.000 description 3
- 229910052801 chlorine Inorganic materials 0.000 description 3
- -1 chlorine anions Chemical class 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 229910052731 fluorine Inorganic materials 0.000 description 3
- 239000011737 fluorine Substances 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 229910000531 Co alloy Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 239000002803 fossil fuel Substances 0.000 description 2
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 2
- 230000010287 polarization Effects 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 230000027756 respiratory electron transport chain Effects 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 238000004627 transmission electron microscopy Methods 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- 229910001362 Ta alloys Inorganic materials 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 238000004502 linear sweep voltammetry Methods 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- MBUJACWWYFPMDK-UHFFFAOYSA-N pentane-2,4-dione;platinum Chemical group [Pt].CC(=O)CC(C)=O MBUJACWWYFPMDK-UHFFFAOYSA-N 0.000 description 1
- 238000005381 potential energy Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000012088 reference solution Substances 0.000 description 1
- 238000004626 scanning electron microscopy Methods 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
- B01J23/8933—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/898—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals also combined with metals, or metal oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with vanadium, tantalum, niobium or polonium
-
- B01J35/33—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
- C25B11/097—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds comprising two or more noble metals or noble metal alloys
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Abstract
The invention discloses a platinum alloy-based tantalum compound electrocatalyst and a preparation method and application thereof, wherein the platinum alloy-based tantalum compound electrocatalyst is composed of a tantalum compound and a platinum-non-noble metal alloy loaded on the tantalum compound, and the mass ratio of the platinum-non-noble metal alloy to the tantalum compound is (0.5-1.5): 10, the tantalum compound is tantalum oxide, tantalum oxynitride or tantalum nitride, and the non-noble metal is at least one metal element of cobalt and nickel. The novel platinum alloy loaded tantalum compound is synthesized by a simple and low-cost method, the platinum alloy loaded tantalum compound exposes the special crystal face of the tantalum compound, the special crystal face of the tantalum compound and the platinum alloy nanoparticles generate a synergistic effect, the catalytic activity and stability of the hydrogen evolution reaction are obviously improved, and the current density is superior to PtC.
Description
Technical Field
The invention belongs to the technical field of electrocatalysis, and particularly relates to a tantalum compound electrocatalyst based on a platinum alloy and a preparation method and application thereof.
Background
The energy source which is one of three major pillars of the modern society plays an important role in the development of the society. However, with the development of economy, the use of fossil fuels in large quantities by humans has not only led to the gradual decrease of non-renewable energy sources until the consumption is exhausted. In addition, during the combustion of fossil fuel, a great deal of pollution gas such as NOx, COx, SOx and the like is generated to form acid rain and cause greenhouse effect to harm the environment. People are therefore increasingly aware of the importance of finding clean energy sources. The clean energy sources discovered in recent years mainly include solar energy, hydrogen energy, wind energy, ocean energy, geothermal energy and the like. Among them, hydrogen energy is considered as the most potential energy source for the development of the 21 st century because of its high combustion efficiency, abundant resources, zero pollution and relatively low cost.
The preparation of high-purity hydrogen by electrolyzing water is an important means for industrial hydrogen production, wherein the research on hydrogen production by electrolysis in alkaline solution is more mature and the application is wider. The principle of hydrogen production by electrolysis in an alkaline solution is that sodium hydroxide is used as a conductive salt, water molecules in the alkaline solution are reduced at a cathode to generate hydrogen atoms and hydroxyl, the hydroxyl is oxidized at an anode to generate water molecules and oxygen atoms, the hydrogen atoms generated by reduction at the cathode are continuously combined with each other and are finally released in the form of hydrogen. Therefore, in the process of hydrogen production by electrolysis, the selection of the cathode hydrogen evolution reaction catalyst is crucial, which not only influences the reaction activation energy of hydrogen atoms and hydroxyl radicals generated by the reduction of water molecules, but also can determine the kinetic parameters of hydrogen atoms combined with each other to evolve hydrogen. The good cathode hydrogen evolution reaction catalyst can reduce the reaction activation energy of hydrogen atoms and hydroxyl radicals generated by the reduction of water molecules, namely, the electrochemical reversibility of the charge transfer step is improved, and the electrochemical polarization of the hydrogen evolution process is reduced. Therefore, the selection of a proper cathode hydrogen evolution reaction catalyst can improve the efficiency of energy conversion in the hydrogen production process by electrolysis, and avoid the release of heat energy converted from electric energy, thereby reducing the energy consumption in the hydrogen evolution process.
However, the most effective and reliable material in the current hydrogen evolution reaction catalyst is noble metal platinum, and although the noble metal platinum can reduce the activation energy of the electrolytic hydrogen evolution so as to save the cost of electric energy, the expensive price makes the production enterprises unable to purchase the noble metal platinum. Therefore, the selection of the hydrogen separation catalyst which is beneficial to reducing the electrochemical polarization of the hydrogen separation process so as to reduce the energy consumption becomes the choice which must be faced in the field of hydrogen production by electrolysis.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a tantalum compound electrocatalyst based on a platinum alloy and a preparation method and application thereof, and aims to improve the water decomposition catalytic activity and stability of a noble metal catalyst in an alkaline electrolyte.
A platinum alloy-based tantalum compound electrocatalyst is characterized by comprising a tantalum compound and a platinum-non-noble metal alloy loaded on the tantalum compound, wherein the mass ratio of the platinum-non-noble metal alloy to the tantalum compound is (0.5-1.5): 10, the tantalum compound is tantalum oxide, tantalum oxynitride or tantalum nitride, and the non-noble metal is at least one metal element of cobalt and nickel.
The preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized by comprising the following steps of:
1) adding soluble inorganic base and tantalum pentoxide into distilled water, fully stirring, transferring the uniformly stirred mixed solution into a high-pressure reaction kettle, placing the high-pressure reaction kettle in an oven at the temperature of 150-170 ℃ for constant-temperature reaction for 10-14 h, filtering the reaction solution in the high-pressure reaction kettle after the reaction is finished, washing filter residues with deionized water, and then placing the filter residues in a vacuum drying oven for drying to obtain potassium tantalate;
2) fully mixing the potassium tantalate obtained in the step 1) with metal chloride and metal fluoride, and then calcining the mixture in a muffle furnace at the temperature of 450-650 ℃ for 2-5 h to obtain a potassium tantalate precursor doped with anions (namely the potassium tantalate precursor doped with fluorine and chlorine anions, wherein the doping of the fluorine and chlorine anions can inhibit the growth of certain crystal faces of the catalyst in the subsequent treatment step so as to form nano-rod-shaped tantalum nitride or granular tantalum oxynitride);
3) placing the anion-doped potassium tantalate precursor obtained in the step 2) into a tubular furnace, roasting in an ammonia atmosphere, washing a roasted product with deionized water, and drying to obtain a tantalum compound;
4) and (3) placing the tantalum compound, the platinum salt and the non-noble metal salt obtained in the step 3) into a mortar for full grinding, then placing into a tubular furnace, and roasting in a nitrogen atmosphere to obtain the platinum alloy-based tantalum compound electrocatalyst.
The preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized in that in the step 1), the soluble inorganic alkali is potassium hydroxide; when the soluble inorganic base and the tantalum pentoxide are added into the distilled water, the molar ratio of the soluble inorganic base to the tantalum pentoxide is 30-10:1, and the concentration of the soluble inorganic base in the distilled water is 0.1-1 mol/L.
The preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized in that in the step 2), the metal chloride is potassium chloride, and the metal fluoride is potassium fluoride; the molar ratio of the potassium tantalate to the metal chloride to the metal fluoride is 1-2: 1.5-3: 0-1.5.
The preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized in that in the step 3), the calcination temperature is 850-.
The preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized in that in the step 4), platinum salt is acetylacetone platinum, potassium hexachloroplatinate, potassium chloroplatinate, platinum chloride or platinous chloride; the non-noble metal salt is one or more of cobalt acetylacetonate, cobalt acetate, cobalt nitrate, cobalt sulfate, nickel acetylacetonate, nickel acetate, nickel nitrate and nickel sulfate.
The preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized in that in the step 4), the roasting temperature is 300-600 ℃, and the roasting time is 2-5 hours.
The platinum alloy-based tantalum compound electrocatalyst is applied to an electrolytic water hydrogen evolution reaction.
The application of the platinum alloy-based tantalum compound electrocatalyst in the hydrogen evolution reaction by electrolysis is characterized in that a two-electrode system testing device is adopted, a carbon rod is used as a counter electrode, the platinum alloy-based tantalum compound electrocatalyst is used as a working electrode, and inorganic alkaline water solution is used as electrolyte to perform the water electrolysis reaction to generate hydrogen.
By adopting the technology, compared with the prior art, the invention has the following beneficial effects:
the novel platinum alloy loaded tantalum compound is synthesized by a simple and low-cost method, the composite material exposes the special crystal face of the tantalum compound, so that the special crystal face of the tantalum compound and platinum alloy nanoparticles generate a synergistic effect, the catalytic activity and stability of hydrogen evolution reaction are obviously improved, and the current density is superior to PtC; the preparation method is simple, low in cost and easy to regulate and control; provides basic application research for the material in the field of electrocatalysis, and has wide application prospect.
Drawings
FIG. 1a shows PtCo/Ta obtained in example 13N5Scanning electron microscope observation at 1 μm;
FIG. 1b shows PtCo/Ta obtained in example 13N5Scanning electron microscopy at 250 nm;
FIG. 2a shows PtCo/Ta obtained in example 13N5Transmission electron microscopy at 50 nm;
FIG. 2b shows PtCo/Ta obtained in example 13N5Transmission electron microscopy at 5 nm;
FIG. 3 shows PtCo/Ta obtained in example 13N5PtNi/Ta obtained in example 23N5And a linear scanning voltammogram of hydrogen produced by electrolysis of water with Pt/C;
FIG. 4 is a linear sweep voltammogram of hydrogen gas produced by electrolyzing water with PtCo/TaON obtained in example 3, PtNi/TaON obtained in example 4, and Pt/C;
FIG. 5 shows PtCo/Ta obtained in example 52O5PtNi/Ta obtained in example 62O5And electrolysis of water at Pt/C produces a linear sweep voltammogram of hydrogen.
Detailed Description
The present invention is further illustrated by the following examples, which should not be construed as limiting the scope of the invention.
Example 1: PtCo/Ta3N5Synthesis of (2)
1) Adding 30mL of 1mol/L potassium hydroxide aqueous solution and 0.4 g of tantalum pentoxide into 30mL of distilled water, carrying out ultrasonic treatment for 10 minutes, transferring the mixed solution into a high-pressure reaction kettle, placing the high-pressure reaction kettle in a 160 ℃ drying oven for carrying out constant-temperature reaction for 12 hours, filtering the reaction solution in the high-pressure reaction kettle after the reaction is finished, washing filter residues with deionized water, and drying in a 80 ℃ vacuum drying oven for 12 hours to obtain potassium tantalate;
2) fully mixing the potassium tantalate, the potassium chloride and the potassium fluoride obtained in the step 1) according to a molar ratio of 1.5:2:1, and then placing the mixture in a muffle furnace at 550 ℃ to calcine for 2 hours to obtain a potassium tantalate precursor material doped with anions;
3) placing the anion-doped potassium tantalate precursor obtained in the step 2) into a tubular furnace, roasting in an ammonia atmosphere at the roasting temperature of 950 ℃ for 2 hours at the ammonia flow of 200 mL/min, washing the roasted product with deionized water for 4 times, and then drying in a vacuum drying oven at the temperature of 60 ℃ for 12 hours to obtain tantalum nitride;
4) putting the tantalum nitride, platinum acetylacetonate and cobalt acetylacetonate obtained in the step 3) into a mortar according to the molar ratio of 20:1:1 for full grinding, then putting into a tube furnace, roasting in nitrogen atmosphere at the roasting temperature of 300 ℃ for 3 hours at the nitrogen flow of 80 mL/min, and preparing the tantalum compound electrocatalyst (PtCo/Ta for short) based on the platinum alloy3N5）。
PtCo/Ta obtained in the present example3N5And respectively carrying out observation and characterization by a scanning electron microscope and a transmission electron microscope, wherein the characterization result of the scanning electron microscope is shown in figure 1a and figure 1b, and the characterization result of the transmission electron microscope is shown in figure 2a and figure 2 b. As can be seen from FIGS. 1a, 1b, 2a and 2b, PtCo/Ta obtained in the present example3N5The nano-rod structure can expose special crystal faces {010} and {001} of tantalum nitride, the combination of the two crystal faces and the platinum-non-noble metal alloy is more stable, and compared with the tantalum nitride without the special crystal faces, the tantalum nitride with the special crystal faces {010} and {001} and the platinum-non-noble metal alloy have special electron transfer effect, and PtCo/Ta alloy has special electron transfer effect3N5Under the action of the catalyst, the electrolytic water hydrogen evolution reaction is easier to carry out.
PtCo/Ta prepared in this example3N5The nanorod structure is probably because the doping of fluorine and chlorine anions inhibits the growth of certain crystal faces of the catalyst during the preparation process of the catalyst, so that the nanorod-shaped tantalum nitride is formed.
The catalytic performance of the platinum-cobalt alloy supported tantalum nitride catalyst prepared in example 1 was tested by the following specific method:
electrocatalytic performance tests were performed at room temperature using CHI760E three-electrode cell system of Shanghai Chenghua, Ag/AgCl (internal reference solution was 3M KCl aqueous solution, reference electrode of the following examples was the same as example 1) electrode as reference electrode, carbon rod as counter electrode, PtCo/Ta prepared in example 13N5The catalyst is prepared into dispersion (the mass of the catalyst is 4mg, the ethanol is 900 mu L, and the Nafion is 100 mu L) and is uniformly dripped on carbon cloth of 1 multiplied by 1 cm, and the dispersion is dried at room temperature and directly used as a working electrode; using 1mol/L KOH aqueous solution as electrolyte to carry out an electrolytic water hydrogen evolution test, wherein the scanning rate of a linear scanning voltammetry is 5mV/s, and H is introduced before the test2For 30 minutes, make H in the electrolyte2Saturation was reached and the test results are shown in figure 3.
Example 2: PtNi/Ta3N5Synthesis of (2)
1) Adding 30mL of 1mol/L potassium hydroxide aqueous solution and 0.4 g of tantalum pentoxide into 30mL of distilled water, carrying out ultrasonic treatment for 10 minutes, transferring the mixed solution into a high-pressure reaction kettle, placing the high-pressure reaction kettle in a 160 ℃ oven for constant-temperature reaction for 12 hours, washing with deionized water, and drying in a 80 ℃ vacuum drying oven for 12 hours to obtain potassium tantalate;
2) fully mixing the potassium tantalate, the potassium chloride and the potassium fluoride obtained in the step 1) according to a molar ratio of 1.5:2:1, and then placing the mixture in a muffle furnace at 550 ℃ to calcine for 2 hours to obtain a potassium tantalate precursor material doped with anions;
3) placing the anion-doped potassium tantalate precursor obtained in the step 2) into a tubular furnace, roasting in an ammonia atmosphere at the roasting temperature of 950 ℃ for 2 hours at the ammonia flow of 200 mL/min, washing the roasted product with deionized water for 4 times, and then drying in a vacuum drying oven at the temperature of 60 ℃ for 12 hours to obtain tantalum nitride;
4) placing the tantalum nitride, the platinum acetylacetonate and the nickel acetylacetonate obtained in the step 3) into a mortar according to the molar ratio of 20:1:1 for full grinding, then placing into a tubular furnace, roasting in a nitrogen atmosphere, wherein the roasting temperature is 300 ℃, the roasting time is 3 hours, and the nitrogen flow is 80 mL/min, and preparing the tantalum compound electrocatalyst based on the platinum alloy(abbreviated as PtNi/Ta)3N5）。
The catalytic performance of the platinum-nickel alloy supported tantalum nitride nanorod catalyst prepared in example 2 was tested, and the specific method was as follows:
electrocatalytic performance tests were performed at room temperature using CHI760E three-electrode electrolytic cell system of Shanghai Chenghua, Ag/AgCl (3M KCl) electrode as reference electrode, carbon rod as counter electrode, PtNi/Ta prepared in example 23N5The catalyst is prepared into dispersion (the mass of the catalyst is 4mg, the ethanol is 900 mu L, and the Nafion is 100 mu L) and is uniformly dripped on carbon cloth of 1 multiplied by 1 cm, and the dispersion is dried at room temperature and directly used as a working electrode; using 1mol/L KOH aqueous solution as electrolyte to carry out an electrolytic water hydrogen evolution test, wherein the scanning rate of a linear scanning voltammetry is 5mV/s, and H is introduced before the test2For 30 minutes, make H in the electrolyte2Saturation was reached and the test results are shown in figure 3.
Example 3: synthesis of PtCo/TaON
1) Adding 30mL of 1mol/L potassium hydroxide aqueous solution and 0.4 g of tantalum pentoxide into 30mL of distilled water, carrying out ultrasonic treatment for 10 minutes, transferring the mixed solution into a high-pressure reaction kettle, placing the high-pressure reaction kettle in a 160 ℃ oven for constant-temperature reaction for 12 hours, washing with deionized water, and drying in a 80 ℃ vacuum drying oven for 12 hours to obtain potassium tantalate;
2) fully mixing the potassium tantalate, the potassium chloride and the potassium fluoride obtained in the step 1) according to a molar ratio of 1.5:2:1, and then placing the mixture in a muffle furnace at 550 ℃ to calcine for 2 hours to obtain a potassium tantalate precursor material doped with anions;
3) placing the anion-doped potassium tantalate precursor obtained in the step 2) into a tubular furnace, roasting in an ammonia atmosphere at the roasting temperature of 850 ℃ for 2 hours at the ammonia flow of 50 mL/min, washing the roasted product with deionized water for 4 times, and then drying in a vacuum drying oven at the temperature of 60 ℃ for 12 hours to obtain tantalum oxynitride;
4) and 3) placing the tantalum oxynitride, platinum acetylacetonate and cobalt acetylacetonate obtained in the step 3) into a mortar according to the molar ratio of 20:1:1 for full grinding, then placing into a tube furnace, and roasting in a nitrogen atmosphere at the roasting temperature of 300 ℃ for 3 hours at the nitrogen flow rate of 80 mL/min to obtain the platinum alloy-based tantalum compound electrocatalyst (PtCo/TaON for short).
The catalytic performance of the platinum-cobalt alloy supported tantalum oxynitride catalyst prepared in example 3 was tested by the following specific method:
electrocatalysis performance tests are carried out at room temperature by utilizing a CHI760E three-electrode electrolytic cell system of Shanghai Chenghua, an Ag/AgCl (3M KCl) electrode is used as a reference electrode, a carbon rod is used as a counter electrode, the PtCo/TaON catalyst prepared in example 3 is prepared into a dispersion (the mass of the catalyst is 4mg, the ethanol is 900 mu L, and the Nafion is 100 mu L) and uniformly dripped on carbon cloth of 1 multiplied by 1 cm, and the dispersion is dried at room temperature and directly used as a working electrode; using 1mol/L KOH aqueous solution as electrolyte to carry out an electrolytic water hydrogen evolution test, wherein the scanning rate of a linear scanning voltammetry is 5mV/s, and H is introduced before the test2For 30 minutes, make H in the electrolyte2Saturation was reached and the test results are shown in figure 4.
Example 4: synthesis of PtNi/TaON
1) Adding 30mL of 1mol/L potassium hydroxide aqueous solution and 0.4 g of tantalum pentoxide into 30mL of distilled water, carrying out ultrasonic treatment for 10 minutes, transferring the mixed solution into a high-pressure reaction kettle, placing the high-pressure reaction kettle in a 160 ℃ oven for constant-temperature reaction for 12 hours, washing with deionized water, and drying in a 80 ℃ vacuum drying oven for 12 hours to obtain potassium tantalate;
2) fully mixing the potassium tantalate, the potassium chloride and the potassium fluoride obtained in the step 1) according to a molar ratio of 1.5:2:1, and then placing the mixture in a muffle furnace at 550 ℃ to calcine for 2 hours to obtain a potassium tantalate precursor material doped with anions;
3) placing the anion-doped potassium tantalate precursor obtained in the step 2) into a tubular furnace, roasting in an ammonia atmosphere at the roasting temperature of 850 ℃ for 2 hours at the ammonia flow of 50 mL/min, washing the roasted product with deionized water for 4 times, and then drying in a vacuum drying oven at the temperature of 60 ℃ for 12 hours to obtain tantalum oxynitride;
4) and (2) placing tantalum oxynitride, platinum acetylacetonate and nickel acetylacetonate in a molar ratio of 20:1:1 in a mortar for full grinding, then placing in a tubular furnace, and roasting in a nitrogen atmosphere at the roasting temperature of 300 ℃ for 3 hours at the nitrogen flow of 80 mL/min to obtain the PtNi/TaON catalyst.
The catalytic performance of the platinum-nickel alloy supported tantalum oxynitride catalyst prepared in example 4 was tested by the following specific method:
electrocatalysis performance tests are carried out at room temperature by utilizing a CHI760E three-electrode electrolytic cell system of Shanghai Chenghua, an Ag/AgCl (3M KCl) electrode is used as a reference electrode, a carbon rod is used as a counter electrode, the PtNi/TaON catalyst prepared in example 4 is prepared into a dispersion (the mass of the catalyst is 4mg, the ethanol is 900 mu L, and the Nafion is 100 mu L) and uniformly dripped on carbon cloth of 1 multiplied by 1 cm, and the dispersion is dried at room temperature and directly used as a working electrode; using 1mol/L KOH aqueous solution as electrolyte to carry out an electrolytic water hydrogen evolution test, wherein the scanning rate of a linear scanning voltammetry is 5mV/s, and H is introduced before the test2For 30 minutes, make H in the electrolyte2Saturation was reached and the test results are shown in figure 4.
Example 5: PtCo/Ta2O5Synthesis of (2)
And (2) placing tantalum oxynitride, platinum acetylacetonate and cobalt acetylacetonate in a molar ratio of 20:1:1 in a mortar for full grinding, then placing in a tubular furnace, and roasting in a nitrogen atmosphere at the roasting temperature of 300 ℃ for 3 hours at the nitrogen flow of 80 mL/min to obtain the PtNi/TaON catalyst.
The catalytic performance of the platinum-nickel alloy supported tantalum oxynitride catalyst prepared in example 5 was tested by the following specific method:
electrocatalytic performance tests were performed at room temperature using CHI760E three-electrode cell system of Shanghai Chenghua, Ag/AgCl (3M KCl) electrode as reference electrode, carbon rod as counter electrode, PtCo/Ta prepared in example 52O5The catalyst is prepared into dispersion (the mass of the catalyst is 4mg, the ethanol is 900 mu L, and the Nafion is 100 mu L) and is uniformly dripped on carbon cloth of 1 multiplied by 1 cm, and the dispersion is dried at room temperature and directly used as a working electrode; using 1mol/L KOH aqueous solution as electrolyte, carrying out electrolytic water hydrogen evolution test experiment, and scanning by linear scanning voltammetryAt a rate of 5mV/s, H was switched on before the test was performed2For 30 minutes, make H in the electrolyte2Saturation was reached and the test results are shown in figure 5.
Example 6: PtNi/Ta2O5Synthesis of (2)
And (2) placing tantalum oxynitride, platinum acetylacetonate and nickel acetylacetonate in a molar ratio of 20:1:1 in a mortar for full grinding, then placing in a tubular furnace, and roasting in a nitrogen atmosphere at the roasting temperature of 300 ℃ for 3 hours at the nitrogen flow of 80 mL/min to obtain the PtNi/TaON catalyst.
The catalytic performance of the platinum-nickel alloy supported tantalum oxynitride catalyst prepared in example 6 was tested by the following specific method:
electrocatalytic performance tests were performed at room temperature using CHI760E three-electrode electrolytic cell system of Shanghai Chenghua, Ag/AgCl (3M KCl) electrode as reference electrode, carbon rod as counter electrode, PtNi/Ta prepared in example 62O5The catalyst is prepared into dispersion (the mass of the catalyst is 4mg, the ethanol is 900 mu L, and the Nafion is 100 mu L) and is uniformly dripped on carbon cloth of 1 multiplied by 1 cm, and the dispersion is dried at room temperature and directly used as a working electrode; using 1mol/L KOH aqueous solution as electrolyte to carry out an electrolytic water hydrogen evolution test, wherein the scanning rate of a linear scanning voltammetry is 5mV/s, and H is introduced before the test2For 30 minutes, make H in the electrolyte2Saturation was reached and the test results are shown in figure 5.
Example 7: preparation of Pt/C catalyst
The performance test method of the comparative sample with Pt/C (Pt loading 20%) as hydrogen evolution reaction is as follows: weighing 4mg of Pt/C, adding the Pt/C into a 4 mL centrifuge tube, sequentially weighing 100 mu L of Nafion solution and 900 mu L of absolute ethyl alcohol by using a pipette gun, adding the Nafion solution and the absolute ethyl alcohol into the centrifuge tube, and then placing the centrifuge tube in an ultrasonic instrument for ultrasonic treatment for 30 minutes to form uniformly dispersed Pt/C slurry. 1 mL of Pt/C slurry was uniformly coated on a carbon cloth of 1X 1 cm by a pipette, air-dried at room temperature, and used as a working electrode, Ag/AgCl (3M KCl) as a reference electrode, and a carbon rod as a counter electrode, and electrocatalytic performance tests were performed at room temperature using a CHI760E three-electrode electrolytic cell system of Shanghai Chenghua. To carry outThe electrolyte used in the Hydrogen Evolution Reaction (HER) test is 1mol/L KOH aqueous solution, and H is firstly introduced before the test2For 30 minutes, make H in the electrolyte2Saturation was reached and the sweep rate of linear sweep voltammetry was 5mV/s, with the results shown in FIG. 3, FIG. 4 and FIG. 5.
FIG. 3 is PtCo/Ta of example 13N5Catalyst, PtNi/Ta of example 23N5HER Linear sweep voltammograms for catalyst and Pt/C catalyst from example 7, PtNi/Ta can be seen in FIG. 33N5The catalyst has better overpotential (current density is 10 mA/cm) in hydrogen evolution reaction2HER overpotential was 23 mV), superior to commercial Pt/C. These excellent properties are attributed to the synergistic effect of the tantalum nitride nanorods and the platinum cobalt nanoparticle nanoparticles.
FIG. 4 is a HER linear sweep voltammogram of the PtCo/TaON catalyst of example 3, the PtNi/TaON catalyst of example 4, and the Pt/C catalyst of example 7. As can be seen from FIG. 4, the performance of the PtCo/TaON catalyst is similar to that of the Pt/C catalyst in catalyzing electrolysis of water to separate hydrogen, and the performance of the PtNi/TaON catalyst is superior to that of the Pt/C catalyst.
FIG. 5 is PtCo/Ta of example 52O5Catalyst, PtNi/Ta of example 62O5HER Linear sweep voltammogram for catalyst and Pt/C catalyst from example 7, PtCo/Ta, as seen in FIG. 52O5Catalyst and PtNi/Ta2O5The performance of the catalyst was inferior to that of the Pt/C catalyst.
As can be seen by comparing FIGS. 3, 4 and 5, PtNi/Ta3N5Catalyst, PtNi/TaON catalyst and PtNi/Ta2O5The catalytic electrolysis hydro-evolution performance of the catalyst is reduced in sequence, which is probably because the nano-rod-shaped tantalum nitride with a special crystal face and the granular tantalum oxynitride with a regular shape are obtained by respectively roasting in the ammonia gas atmosphere in the preparation process of the catalysts in the embodiments 3 and 4, and the catalyst with the nano-rod-shaped tantalum nitride has better catalytic performance when being used for water electrolysis reaction; PtNi/Ta2O5During the preparation process of the catalyst, the catalyst is preparedThe raw materials are directly ground and calcined to form amorphous tantalum oxide, and the performance of hydrogen evolution by catalytic electrolysis water is poor.
The statements in this specification merely set forth a list of implementations of the inventive concept and the scope of the present invention should not be construed as limited to the particular forms set forth in the examples.
Claims (8)
1. A platinum alloy-based tantalum compound electrocatalyst is characterized by comprising a tantalum compound and a platinum-non-noble metal alloy loaded on the tantalum compound, wherein the mass ratio of the platinum-non-noble metal alloy to the tantalum compound is (0.5-1.5): 10, the tantalum compound is tantalum oxide, tantalum oxynitride or tantalum nitride, and the non-noble metal is at least one metal element of cobalt and nickel;
the preparation method of the platinum alloy-based tantalum compound electrocatalyst is characterized by comprising the following steps of:
1) adding soluble inorganic base and tantalum pentoxide into distilled water, fully stirring, transferring the uniformly stirred mixed solution into a high-pressure reaction kettle, placing the high-pressure reaction kettle in an oven at the temperature of 150-170 ℃ for constant-temperature reaction for 10-14 h, filtering the reaction solution in the high-pressure reaction kettle after the reaction is finished, washing filter residues with deionized water, and then placing the filter residues in a vacuum drying oven for drying to obtain potassium tantalate;
2) fully mixing the potassium tantalate obtained in the step 1) with metal chloride and metal fluoride, and then calcining the mixture in a muffle furnace at the temperature of 450-650 ℃ for 2-5 h to obtain a potassium tantalate precursor doped with anions;
3) placing the anion-doped potassium tantalate precursor obtained in the step 2) into a tubular furnace, roasting in an ammonia atmosphere, washing a roasted product with deionized water, and drying to obtain a tantalum compound;
4) placing the tantalum compound, the platinum salt and the non-noble metal salt obtained in the step 3) into a mortar for full grinding, then placing into a tubular furnace, and roasting in a nitrogen atmosphere to obtain the tantalum compound electrocatalyst based on the platinum alloy;
in the step 1), the soluble inorganic alkali is potassium hydroxide;
in the step 2), the metal chloride is potassium chloride, and the metal fluoride is potassium fluoride.
2. The platinum alloy-based tantalum compound electrocatalyst according to claim 1, wherein when the soluble inorganic base and the tantalum pentoxide are added to distilled water, the molar ratio of the soluble inorganic base to the tantalum pentoxide is 30-10:1, and the concentration of the soluble inorganic base in the distilled water is 0.1-1 mol/L.
3. The platinum alloy-based tantalum compound electrocatalyst according to claim 1 wherein the molar ratio of potassium tantalate to metal chloride to metal fluoride is 1-2: 1.5-3: 1-1.5.
4. The platinum alloy-based tantalum compound electrocatalyst according to claim 1, wherein in step 3), the calcination temperature is 850-950 ℃, the calcination time is 2-10 hours, and the ammonia gas flow is 100-400 mL/min.
5. The platinum alloy-based tantalum compound electrocatalyst according to claim 1, wherein in step 4), the platinum salt is platinum acetylacetonate, potassium hexachloroplatinate, potassium chloroplatinate, platinum chloride or platinous chloride; the non-noble metal salt is one or more of cobalt acetylacetonate, cobalt acetate, cobalt nitrate, cobalt sulfate, nickel acetylacetonate, nickel acetate, nickel nitrate and nickel sulfate.
6. The platinum alloy-based tantalum compound electrocatalyst according to claim 1, wherein in step 4), the calcination temperature is 300-600 ℃ and the calcination time is 2-5 hours.
7. Use of the platinum alloy based tantalum compound electrocatalyst according to claim 1 for electrolytic hydro-evolution of hydrogen.
8. The application of claim 7, wherein a two-electrode system testing device is adopted, a carbon rod is used as a counter electrode, the platinum alloy-based tantalum compound electrocatalyst is used as a working electrode, an inorganic alkaline aqueous solution is used as an electrolyte, and an electrolytic water reaction is carried out to generate hydrogen.
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