CN116174000A - Preparation method and application of low-defect perovskite type tantalum-based oxynitride photocatalyst - Google Patents
Preparation method and application of low-defect perovskite type tantalum-based oxynitride photocatalyst Download PDFInfo
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- 229910052715 tantalum Inorganic materials 0.000 title claims abstract description 43
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 title claims abstract description 43
- 239000011941 photocatalyst Substances 0.000 title claims abstract description 18
- 238000002360 preparation method Methods 0.000 title abstract description 13
- 239000000843 powder Substances 0.000 claims abstract description 33
- 238000005121 nitriding Methods 0.000 claims abstract description 32
- 230000001699 photocatalysis Effects 0.000 claims abstract description 30
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 29
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 26
- 238000001816 cooling Methods 0.000 claims abstract description 15
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000003054 catalyst Substances 0.000 claims abstract description 10
- 239000001257 hydrogen Substances 0.000 claims abstract description 10
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 10
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 10
- 150000003624 transition metals Chemical class 0.000 claims abstract description 10
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 9
- 238000002156 mixing Methods 0.000 claims abstract description 9
- 239000001301 oxygen Substances 0.000 claims abstract description 9
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 9
- 238000005406 washing Methods 0.000 claims abstract description 9
- 238000001035 drying Methods 0.000 claims abstract description 8
- 238000000034 method Methods 0.000 claims description 21
- 239000002243 precursor Substances 0.000 claims description 15
- 230000007547 defect Effects 0.000 claims description 10
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 9
- 238000006243 chemical reaction Methods 0.000 claims description 9
- 239000012298 atmosphere Substances 0.000 claims description 8
- 238000004519 manufacturing process Methods 0.000 claims description 8
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 6
- 229910052772 Samarium Inorganic materials 0.000 claims description 6
- 238000001132 ultrasonic dispersion Methods 0.000 claims description 6
- 239000003153 chemical reaction reagent Substances 0.000 claims description 5
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 claims description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 claims description 4
- GEHJYWRUCIMESM-UHFFFAOYSA-L sodium sulfite Chemical compound [Na+].[Na+].[O-]S([O-])=O GEHJYWRUCIMESM-UHFFFAOYSA-L 0.000 claims description 4
- 230000015556 catabolic process Effects 0.000 claims description 3
- 238000006731 degradation reaction Methods 0.000 claims description 3
- 238000011068 loading method Methods 0.000 claims description 3
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 claims description 2
- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 claims description 2
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 239000011668 ascorbic acid Substances 0.000 claims description 2
- 235000010323 ascorbic acid Nutrition 0.000 claims description 2
- 229960005070 ascorbic acid Drugs 0.000 claims description 2
- 239000003795 chemical substances by application Substances 0.000 claims description 2
- 229910052804 chromium Inorganic materials 0.000 claims description 2
- 238000001704 evaporation Methods 0.000 claims description 2
- 235000019253 formic acid Nutrition 0.000 claims description 2
- 229940013688 formic acid Drugs 0.000 claims description 2
- 238000002844 melting Methods 0.000 claims description 2
- 230000008018 melting Effects 0.000 claims description 2
- 229940087646 methanolamine Drugs 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 239000005416 organic matter Substances 0.000 claims description 2
- 235000010265 sodium sulphite Nutrition 0.000 claims description 2
- 229960004418 trolamine Drugs 0.000 claims description 2
- 238000010304 firing Methods 0.000 claims 2
- 239000000463 material Substances 0.000 abstract description 13
- 238000007146 photocatalysis Methods 0.000 abstract description 10
- 230000031700 light absorption Effects 0.000 abstract description 3
- 230000003197 catalytic effect Effects 0.000 abstract description 2
- 238000013329 compounding Methods 0.000 abstract description 2
- 229910017464 nitrogen compound Inorganic materials 0.000 abstract description 2
- 230000003595 spectral effect Effects 0.000 abstract description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 abstract 1
- OLBVUFHMDRJKTK-UHFFFAOYSA-N [N].[O] Chemical compound [N].[O] OLBVUFHMDRJKTK-UHFFFAOYSA-N 0.000 abstract 1
- 239000003513 alkali Substances 0.000 abstract 1
- 239000010453 quartz Substances 0.000 description 18
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 18
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 16
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 15
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 12
- 230000015572 biosynthetic process Effects 0.000 description 12
- 238000010438 heat treatment Methods 0.000 description 12
- 238000003786 synthesis reaction Methods 0.000 description 10
- 150000002602 lanthanoids Chemical class 0.000 description 9
- 229910052747 lanthanoid Inorganic materials 0.000 description 8
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 8
- FGDZQCVHDSGLHJ-UHFFFAOYSA-M rubidium chloride Chemical compound [Cl-].[Rb+] FGDZQCVHDSGLHJ-UHFFFAOYSA-M 0.000 description 8
- 239000011780 sodium chloride Substances 0.000 description 8
- 150000003839 salts Chemical class 0.000 description 7
- 239000012153 distilled water Substances 0.000 description 6
- 239000007789 gas Substances 0.000 description 6
- 239000007787 solid Substances 0.000 description 6
- 238000000862 absorption spectrum Methods 0.000 description 5
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- 238000010926 purge Methods 0.000 description 5
- 238000000926 separation method Methods 0.000 description 5
- 238000001228 spectrum Methods 0.000 description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- 238000010521 absorption reaction Methods 0.000 description 4
- 239000002253 acid Substances 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 4
- 229910052697 platinum Inorganic materials 0.000 description 4
- 238000006722 reduction reaction Methods 0.000 description 4
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 3
- MKYBYDHXWVHEJW-UHFFFAOYSA-N N-[1-oxo-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propan-2-yl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(C(C)NC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 MKYBYDHXWVHEJW-UHFFFAOYSA-N 0.000 description 3
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 229910017052 cobalt Inorganic materials 0.000 description 3
- 239000010941 cobalt Substances 0.000 description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 description 3
- 238000013032 photocatalytic reaction Methods 0.000 description 3
- 238000005215 recombination Methods 0.000 description 3
- 230000006798 recombination Effects 0.000 description 3
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 description 3
- 230000002194 synthesizing effect Effects 0.000 description 3
- OHVLMTFVQDZYHP-UHFFFAOYSA-N 1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-2-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound N1N=NC=2CN(CCC=21)C(CN1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)=O OHVLMTFVQDZYHP-UHFFFAOYSA-N 0.000 description 2
- RZVAJINKPMORJF-UHFFFAOYSA-N Acetaminophen Chemical compound CC(=O)NC1=CC=C(O)C=C1 RZVAJINKPMORJF-UHFFFAOYSA-N 0.000 description 2
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 description 2
- 229910001981 cobalt nitrate Inorganic materials 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 238000003384 imaging method Methods 0.000 description 2
- 229910000311 lanthanide oxide Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000001000 micrograph Methods 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 238000001144 powder X-ray diffraction data Methods 0.000 description 2
- 239000005297 pyrex Substances 0.000 description 2
- 238000004626 scanning electron microscopy Methods 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 238000010532 solid phase synthesis reaction Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052724 xenon Inorganic materials 0.000 description 2
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 2
- 101710134784 Agnoprotein Proteins 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 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 description 1
- ALWUDBGJBKUAME-UHFFFAOYSA-N palladium;sodium;hydrochloride Chemical compound [Na].Cl.[Pd] ALWUDBGJBKUAME-UHFFFAOYSA-N 0.000 description 1
- 230000000737 periodic effect Effects 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 238000006303 photolysis reaction Methods 0.000 description 1
- 230000015843 photosynthesis, light reaction Effects 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 238000005086 pumping Methods 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- GTCKPGDAPXUISX-UHFFFAOYSA-N ruthenium(3+);trinitrate Chemical compound [Ru+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O GTCKPGDAPXUISX-UHFFFAOYSA-N 0.000 description 1
- 229940001482 sodium sulfite Drugs 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 229910001936 tantalum oxide Inorganic materials 0.000 description 1
- 230000007704 transition Effects 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
- C01B13/02—Preparation of oxygen
- C01B13/0203—Preparation of oxygen from inorganic compounds
- C01B13/0207—Water
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/042—Decomposition of water
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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
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Abstract
The invention relates to a preparation method of low-defect perovskite structure tantalum-based oxynitride and application thereof in the field of photocatalysis, and belongs to the technical field of catalytic materials. R is R 2 O 3 、Ta 2 O 5 After mixing with alkali chloride (MCl), RTaO is synthesized 4 Cooling, washing with water to remove MCl, drying, and nitriding RTaO in a reactor with ammonia gas flow 4 Obtaining low-defect perovskite type oxynitride RTaON 2 ，RTaON 2 The powder carries transition metal as a cocatalyst, thereby preparing the photocatalyst. RTaON prepared by the invention 2 Is a low-defect oxygen-nitrogen compound material, has wide spectral light absorption and low current carryingSub-compounding, easy large-scale preparation, etc. The catalyst has obvious photocatalytic activity when applied to photocatalytic water splitting to produce hydrogen and photocatalytic water splitting to produce oxygen.
Description
Technical Field
The invention relates to a preparation method of low-defect perovskite structure tantalum-based oxynitride and application thereof in the field of photocatalysis, and belongs to the technical field of catalytic materials.
Background
The photocatalysis reaction by using a semiconductor can be mainly divided into three steps, 1) light absorption, and electrons on a valence band absorb photons with energy larger than energy of a band gap, and transition from the valence band to a guide band to form photogenerated electrons and holes; 2) Charge separation and transfer, photogenerated electrons and holes transfer from the bulk phase to the surface; 3) The surface catalytic reaction, the photo-generated electrons participate in the reduction reaction on the surface, and the photo-generated holes participate in the oxidation reaction on the surface. In order to fully utilize the energy contained in sunlight, a semiconductor with a broad spectral response is first required to absorb photons effectively. It was found that tantalum-based nitrides or oxynitrides have a smaller band gap (BaTaO 2 N 1.8eV；Ta 3 N 5 2.1eV; taON 2.4 eV) can effectively utilize the visible light portion occupying most of the solar spectrum. At the same time, the surface catalytic reaction requires a suitable energy band structure to meet thermodynamic and kinetic requirements. Tantalum-based oxynitride materials have received considerable attention as ideal materials for a class of band structures with conduction bands around-0.3V. Tantalum-based nitrogen oxides are widely studied in the fields of photocatalytic decomposition of water, reduction of carbon dioxide, preparation of hydrogen peroxide by reduction of oxygen, degradation of organic pollutants, and the like.
The separation and transfer of charge is a central problem in photocatalysis. The separation and transfer time scale of the photo-generated electrons and the holes in the photo-catalytic reaction is nanosecond level, but the recombination of the photo-generated electrons and the holes occurs in picosecond level, so that a large number of carriers are easy to recombine in the separation and transfer process, and the photo-catalytic efficiency cannot be effectively improved. The recombination of the photo-generated electrons and holes often uses low-cost metal as a recombination site, so that one method for effectively improving the photocatalytic efficiency is to construct a low-defect photocatalytic material.
ABO 3 Perovskite-type materials are a class of materials with excellent physicochemical properties that are of interest in many contexts. The excellent properties of tantalum-based oxy-nitrogen compounds of perovskite structure in photocatalysis are also of great interest, including CaTaO 2 N，SrTaO 2 N，BaTaO 2 N，LaTaON 2 Etc. However, the formation of low-cost tantalum defects during synthesis inevitably prevents efficient separation of photogenerated charges, resulting in lower photocatalytic performance. How to build low-defect perovskite-structured tantalum-based oxynitride compounds is a difficult problem.
Lanthanoids are elements of the periodic table of elements numbered 57-71, which have similar atomic radii and exhibit similar chemical properties. The lanthanide atom can be used as an A-site framework atom for constructing a perovskite structure RTaON 2 . The 4f orbital energy of the lanthanide decreases progressively with increasing atomic number. Meanwhile, perovskite type RTaON 2 There are synthetic challenges. Oxynitride is obtained by nitriding an oxide precursor at a high temperature. Typical precursors can be obtained by direct solid phase methods and polymer composite methods. Direct solid phase method for synthesizing lanthanide tantalum-based oxide precursor, because tantalum oxide and lanthanide oxide are in solid phase contact, mass transfer is uneven due to limited contact area, pure phase of lanthanide tantalum-based oxide can not be obtained, and multiphase coexistence (RTaO) is possible 4 ，R 3 TaO 7 ，Ta 2 O 5 ，R 2 O 3 Etc.). The oxide precursor is obtained by using a polymerization compounding method, and organic reagents including citric acid, ethylene glycol, methanol and the like are required to be used, so that the method is not beneficial to environmental protection. On the other hand, multiphase oxynitrides including perovskite RTaON are also formed during nitridation of lanthanide oxides 2 R of pyrochlore phase 2 Ta 2 O 5 N 2 . These factors limit the synthesis of lanthanide oxynitrides and their use in the field of photocatalysis.
Disclosure of Invention
Aiming at the problems of difficult construction of tantalum-based nitrogen oxides with low-defect perovskite structures and application of tantalum-based nitrogen oxides in photocatalysis, the invention aims to develop a novel strategy for utilizing lanthanide sources with lower 4f orbitalsThe child is used as an A-site, and Ta is protected by using a 4f track with reduced energy 5+ Is not reduced in the high-temperature nitriding process, and suppresses the generation of low-valence metal defects in the nitriding process. The specific technical scheme is that RTaO is synthesized by adopting a molten salt method 4 (R is at least one of Sm, eu and Gd) as an oxide precursor, and nitriding at high temperature in ammonia atmosphere to realize low-defect perovskite oxynitride RTaON 2 And (5) synthesizing. By carrying the transition metal cocatalyst, the lanthanide tantalum-based nitrogen oxide can be subjected to catalytic reaction under the illumination condition, and the lanthanide tantalum-based nitrogen oxide can be applied to photolysis water hydrogen production half reaction, oxygen production half reaction and carbon dioxide reduction half reaction to obtain excellent photocatalytic activity. Multiphase photocatalysis experiments show that the perovskite type tantalum-based oxynitride has good application prospect in the field of photocatalysis.
In order to achieve the above object, the technical scheme of the present invention is as follows:
the first aspect of the invention provides a method for preparing a low-defect perovskite-type tantalum-based oxynitride photocatalyst, which comprises the following steps:
(1) R is R 2 O 3 、Ta 2 O 5 Mixing with MCl and roasting;
r is at least one of Sm, eu and Gd, and M is at least one of Li, na, K, rb, cs;
(2) Cooling the roasted product obtained in the step (1), washing with water to remove MCl, and then drying to obtain RTaO 4 ；
(3) The RTaO obtained in the step (2) is reacted with 4 Nitriding in a reactor with ammonia gas flow to obtain low-defect perovskite-type tantalum-based oxynitride RTaON 2 ；
(4) The RTaON obtained in the step (3) is processed 2 And carrying transition metal to obtain the low-defect perovskite type tantalum-based oxynitride photocatalyst.
In the above technical solution, further, the R 2 O 3 、Ta 2 O 5 And MCl in a molar ratio of 1:1: (2-1000).
In the above technical scheme, further, the roasting temperature in the step (1) is 10-1000 ℃ higher than the melting point of MCl, and the roasting time is 2-100 h.
In the above technical scheme, further, the flow rate of the ammonia gas flow in the step (3) is 100-5000 ml/min; the nitriding temperature is 800-1200 ℃, and the nitriding time is 1-30 h.
In the above technical solution, further, in the step (4), the transition metal includes at least one of Cr, mn, fe, co, ni, cu, mo, ru, rh, pd, ag, ir, pt, au; the loading of the transition metal is 0.01-5 wt%.
In the above technical solution, further, the loading method in the step (4) is:
(1) Will RTaON 2 Immersing the powder in a transition metal precursor solution, and evaporating the powder in a water bath after ultrasonic dispersion;
(2) Reducing for 0.1 to 5 hours at the temperature of between 100 and 500 ℃ under the hydrogen gas flow; or treating for 0.1 to 5 hours at 200 to 800 ℃ under the ammonia gas flow, and then roasting for 0.1 to 5 hours at 100 to 500 ℃ in the air atmosphere; or roasting for 0.1-5 h at 100-500 ℃ under nitrogen or argon inert atmosphere.
In a second aspect, the present invention provides a low-defect perovskite-type tantalum-based oxynitride photocatalyst prepared by the preparation method, wherein Ta is contained in the tantalum-based oxynitride 5+ The molar ratio of Ta/Ta is greater than 80%.
The third aspect of the invention provides an application of the low-defect perovskite-type tantalum-based oxynitride photocatalyst in photocatalytic organic matter degradation.
In a fourth aspect, the present invention provides an application of the low-defect perovskite-type tantalum-based oxynitride photocatalyst in a photocatalytic hydrogen-generating reaction, wherein one or more of sodium sulfite, ascorbic acid, formic acid, methanol and triethanolamine are used as a hole sacrificial reagent, and are dispersed in H together with catalyst powder 2 In O, the light is decomposed into H 2 O generates hydrogen.
In a fifth aspect, the present invention provides an application of the low-defect perovskite-type tantalum-based oxynitride photocatalyst in photocatalytic water splitting oxygen production reaction, wherein Ag is + ，Fe 3+ ，IO 3- ，Fe(SCN) 6 3- One or more of them serving asIs a hole sacrificial agent dispersed in H together with catalyst powder 2 In O, the light is decomposed into H 2 O generates oxygen.
The beneficial effects of the invention are as follows:
(1) the synthesis process is simple and easy to operate, and is easy to popularize and apply in a large area.
(2) The catalyst has high yield and the obtained functional material has stable chemical property.
(3) The synthesized catalyst has low defect density and broad spectrum light absorption, and has potential application value in a plurality of photocatalytic reactions.
Drawings
FIG. 1 is a representation of a sample of example 1, wherein (a) GdTaON 2 And GdTaO 4 Powder XRD pattern; (b) Perovskite structure GdTaON 2 A unit cell schematic; (c) GdTaON 2 Scanning electron microscope images;
FIG. 2 is a representation of a sample of example 4, wherein (a) SmTaON 2 And SmTaO 4 Powder XRD pattern; (b) SmTaON of perovskite structure 2 A unit cell schematic; (c) SmTaON 2 Scanning electron microscope images;
FIG. 3 is a graph showing the ultraviolet-visible absorption spectrum of a sample of the present invention, wherein (a) GdTaO prepared in example 1 4 And GdTaON 2 An ultraviolet visible absorption spectrum of the sample; (b) SmTaO prepared in example 4 4 And SmTaON 2 An ultraviolet visible absorption spectrum of the sample; (c) Example 1 preparation of GdTaON 2 Sample Ta 4f XPS peak spectrum; (d) EXAMPLE 4 preparation of SmTaON 2 Sample Ta 4f XPS peak spectrum;
FIG. 4 is a graph showing the activities of the photocatalyst prepared according to the present invention in various photocatalytic reactions, wherein (a) application example 1 GdTaON carrying 1wt% platinum 2 A photo-catalytic water decomposition hydrogen production activity diagram; (b) Application example 2 GdTaON with 2wt% cobalt content 2 Photocatalytic water splitting to produce oxygen activity diagram.
Detailed Description
The present invention will be described in further detail with reference to examples and drawings, but embodiments of the present invention are not limited thereto.
Example 1
(1) Synthesis of oxide precursor GdTaO 4 Gd is combined with 2 O 3 、Ta 2 O 5 RbCl is as per 1:1: charging materials according to the molar ratio of 30, uniformly mixing in a container, transferring into an alumina crucible, heating to 1000 ℃ at 5 ℃/min, keeping for 20 hours, naturally cooling, washing the obtained solid with secondary distilled water to remove molten salt RbCl, and drying the rest powder at 120 ℃ for 24 hours to obtain oxide gadolinium tantalate GdTaO 4 ；
(2) The nitriding pipeline is connected, and GdTaO is taken 4 Placing powder in an alumina magnetic boat, placing the magnetic boat in the center of a quartz tube, connecting an air inlet of the quartz tube with an air path containing ammonia gas, and connecting an air outlet of the quartz tube with a tail gas absorbing device;
(3) Nitriding to obtain GdTaON 2 Introducing ammonia gas into the pipeline at a flow rate of 500ml/min, purging at room temperature for 1h to remove air, heating from room temperature to 1000 ℃ at 5 ℃/min, preserving heat for 20h at 1000 ℃ for nitriding, and naturally cooling to room temperature to obtain low-defect perovskite tantalum-based oxynitride powder GdTaON 2 ；
(4) Supported cocatalyst, 1g GdTaON 2 The powder was immersed in a chloroplatinic acid solution having a platinum content of 1wt%, sonicated, evaporated to dryness in a water bath, and reduced at 200℃under a hydrogen gas stream for 3 hours.
Example 2
(1) Synthesis of oxide precursor GdTaO 4 Gd is combined with 2 O 3 ，Ta 2 O 5 NaCl was as follows 1:1: feeding the materials according to the molar ratio of 50, uniformly mixing in a container, transferring into an alumina crucible, heating to 1000 ℃ at 5 ℃/min, and naturally cooling after keeping for 20 hours; washing the obtained solid with distilled water to remove molten salt NaCl, and drying the rest powder at 120deg.C for 24 hr to obtain gadolinium tantalate GdTaO oxide 4 ；
(2) The nitriding pipeline is connected, and GdTaO is taken 4 Placing powder in an alumina magnetic boat, placing the magnetic boat in the center of a quartz tube, connecting an air inlet of the quartz tube with an air path containing ammonia gas, and connecting an air outlet of the quartz tube with a tail gas absorbing device;
(3) Nitriding to obtain GdTaON 2 Introducing ammonia gas into the pipeline at a flow rate of 500ml/min, purging at room temperature for 1h to remove air, heating from room temperature to 1000 ℃ at 5 ℃/min, preserving heat for 20h at 1000 ℃ for nitriding, and naturally cooling to room temperature to obtain low-defect perovskite tantalum-based oxynitride powder GdTaON 2 ；
(4) Supported cocatalyst, 1g GdTaON 2 The powder is immersed in a cobalt nitrate solution with the cobalt content of 2wt percent, is evaporated to dryness in a water bath after ultrasonic dispersion, is treated for 2 hours at the temperature of 650 ℃ under an ammonia gas flow, and is baked for 1 hour at the temperature of 200 ℃ under an air atmosphere.
Example 3
(1) Synthesis of oxide precursor GdTaO 4 Gd is combined with 2 O 3 、Ta 2 O 5 NaCl, KCl according to 1:1:25:25, mixing uniformly in a container, transferring into an alumina crucible, heating to 1000 ℃ at 5 ℃/min, keeping for 20 hours, naturally cooling, washing the obtained solid with secondary distilled water to remove molten salt NaCl and KCl, and drying the rest powder at 120 ℃ for 24 hours to obtain oxide gadolinium tantalate GdTaO 4 ；
(2) The nitriding pipeline is connected, and GdTaO is taken 4 Placing powder in an alumina magnetic boat, placing the magnetic boat in the center of a quartz tube, connecting an air inlet of the quartz tube with an air path containing ammonia gas, and connecting an air outlet of the quartz tube with a tail gas absorbing device;
(3) Nitriding to obtain GdTaON 2 . Introducing ammonia gas into the pipeline, wherein the flow rate of the ammonia gas is 500ml/min, purging at room temperature for 1h to remove air, then heating from room temperature to 1000 ℃ at 5 ℃/min, preserving heat for 20h at 1000 ℃ for nitriding, and naturally cooling to room temperature to obtain low-defect perovskite structure tantalum-based oxynitride powder GdTaON 2 ；
(4) Supported cocatalyst, 1g GdTaON 2 The powder was immersed in 1wt% gold chloroauric acid solution, 1wt% palladium sodium chloride solution, 1wt% platinum chloroplatinic acid solution, 1wt% copper nitrate solution, and after ultrasonic dispersion, evaporated to dryness in a water bath, and reduced at 200 ℃ for 3 hours under a hydrogen atmosphere.
Example 4
(1) Synthesis of oxide precursor SmTaO 4 Will beSm 2 O 3 、Ta 2 O 5 RbCl is as per 1:1: and (3) feeding the materials according to the molar ratio of 50, uniformly mixing in a container, transferring into an alumina crucible, heating to 1000 ℃ at 5 ℃/min, naturally cooling after maintaining for 20 hours, and washing the obtained solid with secondary distilled water to remove molten salt RbCl. The rest powder is placed at 120 ℃ for 24 hours and dried to obtain the oxide samarium tantalate SmTaO 4 ；
(2) Nitriding pipeline connection, smTaO is taken 4 Placing powder in an alumina magnetic boat, placing the magnetic boat in the center of a quartz tube, connecting an air inlet of the quartz tube with an air path containing ammonia gas, and connecting an air outlet of the quartz tube with a tail gas absorbing device;
(3) Nitriding to obtain SmTaON 2 Introducing ammonia gas into the pipeline at a flow rate of 500ml/min, purging at room temperature for 1h to remove air, heating from room temperature to 1000 ℃ at 2 ℃/min, preserving heat for 20h at 1000 ℃ for nitriding, and naturally cooling to room temperature to obtain low-defect perovskite tantalum-based oxynitride powder SmTaON 2 ；
(4) Supported cocatalyst, 1g SmTaON 2 The powder was immersed in a chloroplatinic acid solution having a platinum content of 1wt%, sonicated, evaporated to dryness in a water bath, and reduced at 200℃under a hydrogen gas stream for 3 hours.
Example 5
(1) Synthesis of oxide precursor SmTaO 4 Sm is to 2 O 3 、Ta 2 O 5 NaCl according to 1:1:50, uniformly mixing in a container, transferring into an alumina crucible, heating to 1000 ℃ at 5 ℃/min, keeping for 20 hours, naturally cooling, washing the obtained solid with secondary distilled water to remove molten salt NaCl, and drying the rest powder at 120 ℃ for 24 hours to obtain the oxide samarium tantalate SmTaO 4 ；
(2) Nitriding pipeline connection, smTaO is taken 4 Placing powder in an alumina magnetic boat, placing the magnetic boat in the center of a quartz tube, connecting an air inlet of the quartz tube with an air path containing ammonia gas, and connecting an air outlet of the quartz tube with a tail gas absorbing device;
(3) Nitriding to obtain SmTaON 2 . Ammonia gas is introduced into the pipeline, the flow rate of the ammonia gas is 500ml/min, and the ammonia gas is purged at room temperature for 1h, exhausting air, then heating from room temperature to 1000 ℃ at 2 ℃/min, preserving heat for 20h at 1000 ℃ for nitriding, and naturally cooling to room temperature to obtain tantalum-based oxynitride powder SmTaON with low-defect perovskite structure 2 ；
(4) Supported cocatalyst, 1g SmTaON 2 The powder is immersed in a cobalt nitrate solution with the cobalt content of 2wt percent, is evaporated to dryness in a water bath after ultrasonic dispersion, is reduced for 2 hours at the temperature of 650 ℃ under an ammonia gas flow, and is baked for 1 hour at the temperature of 200 ℃ under an air atmosphere.
Example 6
Synthesis of oxide precursor SmTaO 4 Sm is to 2 O 3 、Ta 2 O 5 NaCl, KCl according to 1:1:25:25, uniformly mixing in a container, transferring into an alumina crucible, heating to 1000 ℃ at 5 ℃/min, keeping for 20 hours, naturally cooling, washing the obtained solid with secondary distilled water to remove molten salt NaCl and KCl, and drying the rest powder at 120 ℃ for 24 hours to obtain the oxide samarium tantalate SmTaO 4 ；
(2) Nitriding pipeline connection, smTaO is taken 4 Placing powder in an alumina magnetic boat, placing the magnetic boat in the center of a quartz tube, connecting an air inlet of the quartz tube with an air path containing ammonia gas, and connecting an air outlet of the quartz tube with a tail gas absorbing device;
(3) Nitriding to obtain SmTaON 2 Introducing ammonia gas into the pipeline at a flow rate of 500ml/min, purging at room temperature for 1h to remove air, heating from room temperature to 1000 ℃ at 2 ℃/min, preserving heat for 20h at 1000 ℃ for nitriding, and naturally cooling to room temperature to obtain low-defect perovskite tantalum-based oxynitride powder SmTaON 2 ；
(4) Supported cocatalyst, 1g SmTaON 2 The powder is immersed in a ruthenium nitrate solution with the ruthenium content of 1wt%, and is evaporated to dryness in a water bath after ultrasonic dispersion, and is baked for 2 hours at 350 ℃ in a nitrogen atmosphere.
FIG. 1 (a) shows a sample GdTaO of example 1 4 And GdTaON 2 Is demonstrated by nitriding a single phase oxide precursor GdTaO 4 GdTaON of perovskite structure is synthesized 2 The method comprises the steps of carrying out a first treatment on the surface of the FIG. 1 (b) shows a perovskite structure GdTaON of example 1 2 Is shown in the crystal structure of (a)Intent by the method of GdTaON 2 XRD data was refined and showed GdTaON 2 Coordination bonding relation of each atom; FIG. 1 (c) is a sample GdTaON of example 1 2 Scanning electron microscopy imaging shows the microscopic morphology as a stack of hundred nanometer sized particles.
FIG. 2 (a) is sample SmTaO of example 4 4 And SmTaON 2 Is demonstrated by nitriding a single phase oxide precursor SmTaO 4 Synthesis of perovskite Structure SmTaON 2 The method comprises the steps of carrying out a first treatment on the surface of the FIG. 2 (b) is a SmTaON of perovskite structure of example 4 2 By a schematic of the crystal structure of SmTaON 2 XRD data were refined and showed SmTaON 2 Coordination bonding relation of each atom; FIG. 2 (c) is sample SmTaON of example 4 2 Scanning electron microscopy imaging shows the microscopic morphology as a stack of hundred nanometer sized particles.
FIG. 3 is a graph of UV-visible absorption spectrum, (a) is a graph of GdTaO obtained in example 1 4 And GdTaON 2 (b) ultraviolet visible absorption of (a) SmTaO was used to prepare sample SmTaO in example 4 4 And SmTaON 2 The UV-visible absorption of (C) indicates that the absorption range of the material is widened by nitriding. By GdTaON in the ultraviolet visible absorption spectrum 2 And SmTaON 2 The low tail absorption also demonstrates their low defect nature, demonstrating the effectiveness of synthesizing low defect tantalum-based oxynitride compounds by design through reduced 4f orbitals.
FIG. 3 (c) is a chart showing the preparation of GdTaON in example 1 2 Sample Ta 4f XPS peak spectrum; FIG. 3 (d) is a schematic illustration of example 4 preparation of SmTaON 2 Sample Ta 4f XPS peak spectrum; the Ta 4f peak splitting results show that the higher tantalum occupies the main part and the lower tantalum occupies a small proportion, directly illustrating the effectiveness of suppressing lower tantalum formation with reduced 4f orbitals.
Application example 1
Preparation of Hydrogen by photocatalytic Water decomposition reaction was carried out in a top-illuminated Pyrex glass reactor with a constant temperature water bath at 15℃and 50mg of the composite photocatalyst prepared in example 1 was ultrasonically dispersed in 100mL of solution (containing 20vol% CH) 3 OH as sacrificial reagent), in the reactorThe air in (2) is removed by vacuumizing, a xenon lamp is used as a light source, photons in the ultraviolet part are filtered through a filter (lambda is more than or equal to 420 nm), and the hydrogen production activity of the catalyst under visible light is tested.
Application example 2
Preparation of Hydrogen by photocatalytic Water decomposition reaction in a top-illuminated Pyrex glass reactor with a constant temperature Water bath at 15℃50mg of the composite photocatalyst prepared in example 2 was ultrasonically dispersed in 100mL of solution (containing 0.01M AgNO) 3 As a sacrificial reagent), air in the reactor was removed by vacuum pumping, a xenon lamp was used as a light source, light in the ultraviolet portion was filtered through a filter (lambda. Is not less than 420 nm), and the oxygen generating activity of the catalyst under visible light was tested.
FIG. 4 is a graph of the photocatalytic activity of application examples 1-2, illustrating the use of such catalysts in photocatalysis for a number of reactions.
Claims (10)
1. A method for preparing a low defect perovskite-type tantalum-based oxynitride photocatalyst, the method comprising the steps of:
(1) R is R 2 O 3 、Ta 2 O 5 Mixing with MCl and roasting;
r is at least one of Sm, eu and Gd, and M is at least one of Li, na, K, rb, cs;
(2) Cooling the roasted product obtained in the step (1), washing with water to remove MCl, and then drying to obtain RTaO 4 ；
(3) The RTaO obtained in the step (2) is reacted with 4 Nitriding in a reactor with ammonia gas flow to obtain low-defect perovskite-type tantalum-based oxynitride RTaON 2 ；
(4) The RTaON obtained in the step (3) is processed 2 And carrying transition metal to obtain the low-defect perovskite type tantalum-based oxynitride photocatalyst.
2. The method of claim 1, wherein R is 2 O 3 、Ta 2 O 5 And MCl in a molar ratio of 1:1: (2-1000).
3. The method according to claim 1, wherein the firing temperature in the step (1) is 10 to 1000 ℃ higher than the melting point of MCl, and the firing time is 2 to 100 hours.
4. The method according to claim 1, wherein the flow rate of the ammonia gas stream in the step (3) is 100 to 5000ml/min; the nitriding temperature is 800-1200 ℃, and the nitriding time is 1-30 h.
5. The method of claim 1, wherein the transition metal in step (4) comprises at least one of Cr, mn, fe, co, ni, cu, mo, ru, rh, pd, ag, ir, pt, au; the loading of the transition metal is 0.01-5 wt%.
6. The method according to claim 1, wherein the supporting method in the step (4) is:
(1) Will RTaON 2 Immersing the powder in a transition metal precursor solution, and evaporating the powder in a water bath after ultrasonic dispersion;
(2) Reducing for 0.1 to 5 hours at the temperature of between 100 and 500 ℃ under the hydrogen gas flow;
or treating for 0.1 to 5 hours at 200 to 800 ℃ under the ammonia gas flow, and then roasting for 0.1 to 5 hours at 100 to 500 ℃ in the air atmosphere;
or roasting for 0.1-5 h at 100-500 ℃ under nitrogen or argon inert atmosphere.
7. A low defect perovskite-type tantalum-based oxynitride photocatalyst produced by the production method as claimed in any one of claims 1 to 6, characterized in that Ta in said tantalum-based oxynitride 5+ The molar ratio of Ta/Ta is greater than 80%.
8. Use of a low defect perovskite-based tantalum-based oxynitride photocatalyst according to claim 7 for photocatalytic organic matter degradation.
9. A low defect perovskite tantalum according to claim 7The application of the base oxynitride photocatalyst in the photocatalytic hydrogen production reaction is characterized in that: sodium sulfite, one or more of ascorbic acid, formic acid, methanol and triethanolamine are used as hole sacrificial reagent, and dispersed in H together with catalyst powder 2 In O, the light is decomposed into H 2 O generates hydrogen.
10. Use of the low defect perovskite-based tantalum-based oxynitride photocatalyst according to claim 7 in photocatalytic water splitting oxygen production reactions, characterized in that: by Ag + ，Fe 3+ ，IO 3- ，Fe(SCN) 6 3- As hole sacrificial agent, dispersed in H together with the catalyst powder 2 In O, the light is decomposed into H 2 O generates oxygen.
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| CN116809105B (en) * | 2023-06-12 | 2024-05-28 | 中国科学院大连化学物理研究所 | Perovskite tantalum nitrogen co-doped strontium titanate and preparation method and application thereof |
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