CN109331852A - A kind of photocatalyst catalyst material and its preparation method and application - Google Patents
A kind of photocatalyst catalyst material and its preparation method and application Download PDFInfo
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- CN109331852A CN109331852A CN201811027363.9A CN201811027363A CN109331852A CN 109331852 A CN109331852 A CN 109331852A CN 201811027363 A CN201811027363 A CN 201811027363A CN 109331852 A CN109331852 A CN 109331852A
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- photocatalyst
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- 239000011941 photocatalyst Substances 0.000 title claims abstract description 76
- 239000000463 material Substances 0.000 title claims abstract description 37
- 239000003054 catalyst Substances 0.000 title claims abstract description 36
- 238000002360 preparation method Methods 0.000 title claims abstract description 21
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 claims abstract description 63
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 37
- 239000001257 hydrogen Substances 0.000 claims abstract description 24
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 24
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 23
- 238000000354 decomposition reaction Methods 0.000 claims abstract description 17
- 238000004519 manufacturing process Methods 0.000 claims abstract description 16
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 15
- 230000015556 catabolic process Effects 0.000 claims abstract description 13
- 238000006731 degradation reaction Methods 0.000 claims abstract description 13
- 229910052751 metal Inorganic materials 0.000 claims abstract description 6
- 239000002184 metal Substances 0.000 claims abstract description 6
- 239000000843 powder Substances 0.000 claims description 36
- 239000000243 solution Substances 0.000 claims description 32
- WFDIJRYMOXRFFG-UHFFFAOYSA-N acetic acid anhydride Natural products CC(=O)OC(C)=O WFDIJRYMOXRFFG-UHFFFAOYSA-N 0.000 claims description 22
- 238000001354 calcination Methods 0.000 claims description 18
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 16
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 14
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 14
- 239000008367 deionised water Substances 0.000 claims description 14
- 229910021641 deionized water Inorganic materials 0.000 claims description 14
- 229910000428 cobalt oxide Inorganic materials 0.000 claims description 12
- 239000007921 spray Substances 0.000 claims description 12
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 claims description 11
- 238000000034 method Methods 0.000 claims description 10
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 9
- 229910052697 platinum Inorganic materials 0.000 claims description 8
- 229910021529 ammonia Inorganic materials 0.000 claims description 7
- 239000011521 glass Substances 0.000 claims description 7
- 238000002156 mixing Methods 0.000 claims description 7
- 230000000694 effects Effects 0.000 claims description 6
- 239000011259 mixed solution Substances 0.000 claims description 6
- 239000002244 precipitate Substances 0.000 claims description 6
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims description 6
- 239000000725 suspension Substances 0.000 claims description 6
- ZHJGWYRLJUCMRT-UHFFFAOYSA-N 5-[6-[(4-methylpiperazin-1-yl)methyl]benzimidazol-1-yl]-3-[1-[2-(trifluoromethyl)phenyl]ethoxy]thiophene-2-carboxamide Chemical compound C=1C=CC=C(C(F)(F)F)C=1C(C)OC(=C(S1)C(N)=O)C=C1N(C1=C2)C=NC1=CC=C2CN1CCN(C)CC1 ZHJGWYRLJUCMRT-UHFFFAOYSA-N 0.000 claims description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 5
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 5
- 239000011575 calcium Substances 0.000 claims description 5
- 239000002131 composite material Substances 0.000 claims description 5
- 229960000935 dehydrated alcohol Drugs 0.000 claims description 5
- GJKFIJKSBFYMQK-UHFFFAOYSA-N lanthanum(3+);trinitrate;hexahydrate Chemical compound O.O.O.O.O.O.[La+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O GJKFIJKSBFYMQK-UHFFFAOYSA-N 0.000 claims description 5
- 239000002105 nanoparticle Substances 0.000 claims description 5
- 108010029541 Laccase Proteins 0.000 claims description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- 239000003426 co-catalyst Substances 0.000 claims description 4
- 239000001301 oxygen Substances 0.000 claims description 4
- 229910052760 oxygen Inorganic materials 0.000 claims description 4
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 4
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 4
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 3
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 3
- 238000001816 cooling Methods 0.000 claims description 3
- 239000003792 electrolyte Substances 0.000 claims description 3
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 3
- 229910001961 silver nitrate Inorganic materials 0.000 claims description 3
- 238000005507 spraying Methods 0.000 claims description 3
- 238000002604 ultrasonography Methods 0.000 claims description 3
- NGNBDVOYPDDBFK-UHFFFAOYSA-N 2-[2,4-di(pentan-2-yl)phenoxy]acetyl chloride Chemical compound CCCC(C)C1=CC=C(OCC(Cl)=O)C(C(C)CCC)=C1 NGNBDVOYPDDBFK-UHFFFAOYSA-N 0.000 claims description 2
- 150000001805 chlorine compounds Chemical class 0.000 claims description 2
- 238000009833 condensation Methods 0.000 claims 1
- 230000005494 condensation Effects 0.000 claims 1
- 239000007788 liquid Substances 0.000 claims 1
- 230000001376 precipitating effect Effects 0.000 claims 1
- PANBYUAFMMOFOV-UHFFFAOYSA-N sodium;sulfuric acid Chemical compound [Na].OS(O)(=O)=O PANBYUAFMMOFOV-UHFFFAOYSA-N 0.000 claims 1
- 230000031700 light absorption Effects 0.000 abstract description 2
- 238000000746 purification Methods 0.000 abstract description 2
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000011161 development Methods 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 230000001699 photocatalysis Effects 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 230000007613 environmental effect Effects 0.000 description 3
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 3
- 230000005855 radiation Effects 0.000 description 3
- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical compound NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- NIPNSKYNPDTRPC-UHFFFAOYSA-N N-[2-oxo-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 NIPNSKYNPDTRPC-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 230000033228 biological regulation Effects 0.000 description 2
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000000227 grinding Methods 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 238000007146 photocatalysis Methods 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 238000004176 ammonification Methods 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 125000004429 atom Chemical group 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 239000011258 core-shell material Substances 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 230000002147 killing effect Effects 0.000 description 1
- FYDKNKUEBJQCCN-UHFFFAOYSA-N lanthanum(3+);trinitrate Chemical compound [La+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O FYDKNKUEBJQCCN-UHFFFAOYSA-N 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- XRRQZKOZJFDXON-UHFFFAOYSA-N nitric acid;silver Chemical compound [Ag].O[N+]([O-])=O XRRQZKOZJFDXON-UHFFFAOYSA-N 0.000 description 1
- 230000020477 pH reduction Effects 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
Classifications
-
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
-
- 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
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/003—Catalysts comprising hydrides, coordination complexes or organic compounds containing enzymes
-
- 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
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/26—Catalysts comprising hydrides, coordination complexes or organic compounds containing in addition, inorganic metal compounds not provided for in groups B01J31/02 - B01J31/24
- B01J31/28—Catalysts comprising hydrides, coordination complexes or organic compounds containing in addition, inorganic metal compounds not provided for in groups B01J31/02 - B01J31/24 of the platinum group metals, iron group metals or copper
-
- 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
-
- 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
-
- 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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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Electrochemistry (AREA)
- Inorganic Chemistry (AREA)
- Metallurgy (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
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Abstract
The present invention relates to a kind of photocatalyst catalyst material and its preparation method and application, which is perovskite type metal nitrogen oxides, has spherical porous microscopic appearance, and partial size is 100-500 nanometers, molecular formula La1‑xCaxTaO1+yN2‑y, wherein 0≤x, y≤1, the photocatalyst catalyst material can be used for preparing water decomposition hydrogen manufacturing type photocatalyst and degradation of formaldehyde type photocatalyst, have the characteristics that visible light-responded, light absorption is continuously adjusted the application, it can be achieved that solar hydrogen making and solar energy purification environment (formaldehyde).
Description
Technical field
The invention belongs to catalysis material technical fields, and in particular to a kind of photocatalyst catalyst material and preparation method thereof
And application.
Background technique
With the continuous development of human society, existing energy resource structure has been increasingly difficult to meet the ever-increasing energy of the mankind
Source demand.Three big main fossil energy deposits (petroleum, natural gas and coal) will in this century with existing energy consumption speed
Depleted, Looking For Substitutions Of Oil is extremely urgent as early as possible.On the other hand, the exploitation of fossil fuel, use and discharge and induce
Serious environmental problem, such as climate warming, Ocean acidification, air pollution are unfavorable for the sustainable development of society.Therefore, it opens
Sending out or find the new sustainable energy utilization patterns of one kind is the key that solve the above problems.
Relative to the variety of problems of fossil energy, the development and utilization of solar energy has a variety of advantages.Firstly, solar energy stores up
It measures huge, in the positive value middle age in service life of the sun, will also burn away 5,000,000,000 years.It is estimated that arriving within one hour the sun of earth surface
1 year energy requirement of the mankind can be met；Secondly, solar radiation is widely distributed and easy acquisition.In addition to south poles will appear
Outside polar night phenomenon, there is considerable solar radiation in the place of human living；Again, the development and utilization of solar energy is cleaned without dirt
Dye, not will cause continued damage to environment.Existing Solar use mode mainly includes solar energy-electric energy conversion, solar energy
Can convert and solar energy conversion.Wherein solar energy chemical conversion is ideal energy development approach.For example, will interval
Property, the solar radiation of easily collecting and storage is not converted into the chemical energy (such as Hydrogen Energy) of easily collecting and storage, both can be effective
Existing fossil energy is matched using framework, is unlikely to overturn fossil energy economy completely, and can effectively avoid fossil energy and open
Hair utilizes brought environmental problem.
1) it is hydrogen and oxygen by water decomposition in photocatalyst surface using solar energy that the conversion of solar energy chemical energy is specifically included that
Gas (i.e. solar hydrogen making)；2) solar energy and photocatalyst decomposing organic pollutant such as formaldehyde (solar energy purification environment) are utilized.This
Two kinds of Solar use modes all rely on efficient photocatalyst, and photocatalyst is that one kind can be absorbed, conversion solar energy and be urged
Change the catalyst of chemical reaction, traditional photocatalyst such as TiO2(Energy&Environmental Science,5(2012)
6506-6512), the faces such as CdS (The Journal of Physical Chemistry C, 115 (2011) 11466-11473)
Face the problems such as sunshine absorptivity is low, stability is poor, solar hydrogen making efficiency and degradable organic pollutant (such as formaldehyde) is caused to be imitated
Rate is not high.
Summary of the invention
The purpose of the present invention is to solve the above-mentioned problems and provides a kind of light good with high catalytic activity, stability
Catalyst catalyst material and its preparation method and application.
The purpose of the present invention is achieved through the following technical solutions:
A kind of photocatalyst catalyst material, the catalyst material are perovskite type metal nitrogen oxides, are had spherical porous
Microscopic appearance, partial size are 100-500 nanometers, molecular formula La1-xCaxTaO1+yN2-y, wherein 0≤x, y≤1.
A kind of preparation method of photocatalyst catalyst material, comprising the following steps:
(1) under conditions of temperature is 263K-283K, acetic acid and acetic anhydride is mixed, clear solution S1 is obtained, in temperature
Under conditions of 273K-283K, tantalic chloride and dehydrated alcohol are mixed, clear solution S2 is made, is 273K-283K in temperature
Under conditions of, solution S 1 is mixed, and be vigorously stirred with solution S 2, obtains mixed solution S3；
(2) under conditions of temperature is 273K-283K, by calcium nitrate tetrahydrate, mixed solution is added in lanthanum nitrate hexahydrate
S3, and be vigorously stirred, until solution is clarified, it is labeled as solution S 4；
(3) solution S 4 is placed in baking oven, keeps the temperature 2-72 hours under the conditions of 303K-373K, obtains white precipitate P1,
White precipitate P1 is filtered under the conditions of 323K-373K and is kept the temperature 12-72 hours, later under the conditions of inert atmosphere protection
Obtain powder P2 within 523K-623K calcination 3-8 hours, inert gas flow velocity should be 50-100 ml/min；
(4) by powder P2 in oxygen protection under at 873K-973K calcination 5-24 hours, obtain white powder P3, white powder
For last P3 under ammonia atmosphere protection, ammonia flow velocity should be 100-300 ml/min, at 1023K-1423K calcination 5-25 hours, obtain
Photocatalyst catalyst material is obtained after deionized water rinse to powder P4, powder P4.
Preferably, the weight part ratio of acetic acid described in step (1) and acetic anhydride is 100:5-10, dehydrated alcohol and phosphoric
Tantalum weight part ratio is 100:10-30, and solution S 1 and 2 weight ratio of solution S are 1:0.5-1.5.
Preferably, relative to 100 parts by weight tantalic chlorides in step (2), the dosage of calcium nitrate tetrahydrate is 70-90 weight
Part, the dosage of lanthanum nitrate hexahydrate is 10-30 parts by weight.
A kind of photocatalyst preparation, comprising above-mentioned photocatalyst catalyst material, and supported co-catalyst, the co-catalyst
Selected from one of cobalt oxide, Platinum Nanoparticles or nano silver or a variety of.
Further, the step of photocatalyst catalyst material supports cobalt oxide are as follows: by photocatalyst catalyst material, cobalt nitrate
It is mixed with deionized water, ultrasound obtains suspension M1, and suspension M1 is dried under the conditions of 353K-403K, obtains powder P6, powder
P6 under the conditions of 1023K-1123K, calcination 1-3 hours, obtains powder P7, powder P7 is in 423K-473K under ammonia atmosphere protection
Under the conditions of calcination 1-3 hours to get to the photocatalyst catalyst material for supporting cobalt oxide.
Further, the photocatalyst catalyst material for supporting cobalt oxide is mixed with platinum acid chloride solution, in 400K-500K item
Calcination 1-3 hours under part, water decomposition hydrogen manufacturing type photocatalyst is obtained.
Further, the photocatalyst catalyst material, silver nitrate and ethylene glycol that support cobalt oxide are mixed, in 393K-
Heated 10-30 minutes under the conditions of 463K, through cooling, filter, be dried to obtain composite material C1, by composite material C1, laccase, go from
Sub- water mixing, is dried to obtain degradation of formaldehyde type photocatalyst.
The photocatalyst preparation be used for water decomposition hydrogen manufacturing or degradation of formaldehyde, wherein water decomposition hydrogen manufacturing type photocatalyst it is specific
Application method are as follows:
(1) mix water decomposition hydrogen manufacturing type photocatalyst, polyvinylpyrrolidone, deionized water according to weight ratio 20:1:10,
Grinding is scratched to FTO electro-conductive glass；
(2) the FTO electro-conductive glass and platinized platinum for supporting water decomposition hydrogen manufacturing type photocatalyst respectively as working electrode and to electrode,
Aqueous sodium persulfate solution constitutes photoelectrolytic cell as electrolyte；
(3) working electrode is as anode, and to electrode as cathode, both ends apply voltage, irradiates working electrode in sunlight
Under the conditions of decompose water, cathode collects hydrogen；
The specifically used method of degradation of formaldehyde type photocatalyst are as follows:
(1) degradation of formaldehyde type photocatalyst, deionized water are mixed according to 1:20 weight ratio, ultrasonic disperse；
(2) object will be sprayed-on to clean out, the object of spraying will be avoided to be covered with film；
(3) the good spray gun of selection atomizing effect, spray gun and is kept 5-15cm distance between spray object；
(4) to be spontaneously dried by spray object.
Compared with prior art, the invention has the following advantages:
1, the present invention regulates and controls the hydrolysis rate of tantalic chloride, can be made has by the ratio of control acetic anhydride and acetic acid
The spherical nanoparticle of porous structure, the spherical nanoparticle have biggish specific surface, be conducive to catalysis reaction progress and
The transmission (such as Fig. 1) of substance.
2, the present invention obtains the powder of similar unformed shape, is conducive to nitrogen in ammonifying process by low-temperature treatment predecessor
The doping of atom and substance at phase.
3, the present invention, can suction with Effective Regulation photocatalyst to sunlight by the metering ratio of regulation calcium nitrate and lanthanum nitrate
Receipts ability, absorbing sunlight photon range continuously can regulate and control (such as Fig. 2) in 500-700 nanometers.
4, method of the present invention by being restored after first ammonification, photocatalyst surface support the nanometer cobalt with core-shell structure/
Cobalt oxide layer, the structure have the ability of quick separating charge.
5, the present invention is by mixing photocatalyst with silver nitrate solution, directly in photocatalyst surface in-situ deposition nano silver,
Nano silver is even closer in conjunction with photocatalyst, more obvious to the killing effect of bacterium.
6, the present invention can significantly increase the binding ability of photocatalyst and wood materials, be conducive to light by supporting laccase
The fixation on wooden utensil of catalyst.
7, the present invention mainly effectively converts indoor organic pollution using itself high efficiency photocatalysis activity of photocatalyst activity material
Object formaldehyde, active material used have very excellent visible light absorption capacity, can efficiently use sunlight and carry out photocatalysis
Reaction, remove formaldehyde products (active carbon etc.) from market mainstream has essence different by Adsorption formaldehyde, the invention patent
Advantage is effectively to convert formaldehyde pollutants, and reducing concentration of formaldehyde not by adsorption effect, (later period is easy
Secondary release formaldehyde).
Detailed description of the invention
Fig. 1 is perovskite type metal nitrogen oxides La0.9Ca0.1TaO1+yN2-yStereoscan photograph；
Fig. 2 is perovskite type metal nitrogen oxides La1-xCaxTaO1+yN2-yThe pass of (wherein, 0≤x, y≤1) absorptance and x
System.
Specific embodiment
The present invention is described in detail combined with specific embodiments below.
A kind of photocatalyst catalyst material, is made by the steps to obtain:
One, the preparation of metallic oxide precursor object:
(1) under conditions of temperature is 263K-283K, acetic acid and acetic anhydride is mixed, clear solution S1 is obtained；
(2) under conditions of temperature is 273K-283K, tantalic chloride and dehydrated alcohol are mixed, clear solution S2 is made；
(3) under conditions of temperature is 273K-283K, solution S 1 is mixed, and be vigorously stirred with solution S 2, is mixed
Solution S 3；
(4) under conditions of temperature is 273K-283K, by calcium nitrate tetrahydrate, mixed solution is added in lanthanum nitrate hexahydrate
S3, and be vigorously stirred, until solution is clarified, it is labeled as solution S 4；
(5) solution S 4 is placed in baking oven, keeps the temperature 2-72 hours under the conditions of 303K-373K, obtains white precipitate P1；
(6) white precipitate P1 is filtered under the conditions of 323K-373K and is kept the temperature 12-72 hours；
(7) white precipitate P1 is under inert atmosphere (nitrogen or argon gas) protective condition in 3-8 hour of 523K-623K calcination
Obtain white powder P2；
(8) white powder P2 obtains white powder P3 in 5-24 hour of 873K-973K calcination under oxygen protection；
Two, metal oxynitride La1-xCaxTaO1+yN2-yThe preparation step of (wherein, 0≤x, y≤1):
(1) white powder P3 is placed in alumina crucible, under ammonia atmosphere protection, in 1223K-1323K calcination 5-25
A hour obtains powder P4；
(2) powder P4 passes through deionized water rinse 5-10 times, obtains powder P5, as photocatalyst catalyst material.
The photocatalyst catalyst material supports nanometer cobalt/cobalt oxide layer specific steps are as follows:
(1) powder P5, cobalt nitrate, deionized water mixing, ultrasound obtain suspension M1；
(2) suspension M1 is dried under the conditions of 353K-403K, obtains powder P6；
(3) powder P6 under the conditions of 1023K-1123K, calcination 1-3 hours, obtains powder P7 under ammonia atmosphere protection；
(4) powder P7 obtains powder P8 calcination 1-3 hours under the conditions of 423K-473K；
The photocatalyst catalyst material supports the step of Platinum Nanoparticles obtain water decomposition hydrogen manufacturing type photocatalyst are as follows: powder P8 and chlorine
Platinic acid solution mixing, under the conditions of 400K-500K calcination 1-3 hour to get to water decomposition hydrogen manufacturing type photocatalyst.
The step of photocatalyst catalyst material nano silver loaded obtains degradation of formaldehyde type photocatalyst are as follows: powder P8, nitric acid
Silver and ethylene glycol mixing, heat 10-30 minutes under the conditions of 393K-463K, through cooling, filter, are dried to obtain composite material C1；
Composite material C1, laccase, deionized water mixing, drying, obtain degradation of formaldehyde type photocatalyst.
The application method of water decomposition hydrogen manufacturing type photocatalyst:
(1) choose 1 piece of clean FTO electro-conductive glass (10 10 centimetres of cm x), by water decomposition hydrogen manufacturing type photocatalyst,
Polyvinylpyrrolidone (PVP, molecular weight 1300000), deionized water are mixed according to weight ratio 20:1:10, grinding, are scratched extremely
On FTO electro-conductive glass；
(2) the FTO electro-conductive glass that supports water decomposition hydrogen manufacturing type photocatalyst, platinized platinum (1 1 centimetre of cm x) are respectively as work
Electrode and to electrode, aqueous sodium persulfate solution (0.1 mol/L concentration) is used as electrolyte, constitutes photoelectrolytic cell；
(3) working electrode is as anode, and to electrode as cathode, both ends apply 0.2 volt of voltage, irradiates work in sunlight
Make to decompose water under electrode conditions, cathode collects hydrogen.
The application method of degradation of formaldehyde type photocatalyst:
(1) degradation of formaldehyde type photocatalyst, deionized water are mixed according to 1:20 weight ratio, ultrasonic disperse；
(2) object will be sprayed-on to clean out, the object of spraying will be avoided to be covered with film；
(3) select the preferable spray gun of atomizing effect, spray gun and by between spray object keep 5-15 cm distance；
(4) it to be spontaneously dried by spray object, is not wiped before dry.
Photocatalyst preparation is prepared by the raw material proportioning in table 1 and the photocatalytic water performance and according to GB/ under the conditions of AM 1.5G
Formaldehyde performance test is gone in T16129 detection.
The raw material proportioning table of table 1 embodiment 1-4 and comparative example 1-3
Table 2 embodiment 1-4 and comparative example 1-3 under the conditions of AM 1.5G photocatalytic water performance and according to GB/T16129 detection go
Formaldehyde performance.
The above description of the embodiments is intended to facilitate ordinary skill in the art to understand and use the invention.
Person skilled in the art obviously easily can make various modifications to these embodiments, and described herein general
Principle is applied in other embodiments without having to go through creative labor.Therefore, the present invention is not limited to the above embodiments, ability
Field technique personnel announcement according to the present invention, improvement and modification made without departing from the scope of the present invention all should be of the invention
Within protection scope.
Claims (10)
1. a kind of photocatalyst catalyst material, which is characterized in that the catalyst material is perovskite type metal nitrogen oxides, is had
Spherical porous microscopic appearance, partial size are 100-500 nanometers, molecular formula La1-xCaxTaO1+yN2-y, wherein 0≤x, y≤1.
2. a kind of preparation method of photocatalyst catalyst material as described in claim 1, which is characterized in that including following step
It is rapid:
(1) under conditions of temperature is 263K-283K, acetic acid and acetic anhydride is mixed, clear solution S1 is obtained, is in temperature
Under conditions of 273K-283K, tantalic chloride and dehydrated alcohol are mixed, clear solution S2 is made, is 273K-283K's in temperature
Under the conditions of, solution S 1 is mixed, and be vigorously stirred with solution S 2, obtains mixed solution S3；
(2) under conditions of temperature is 273K-283K, by calcium nitrate tetrahydrate, mixed solution S3 is added in lanthanum nitrate hexahydrate, and
It is vigorously stirred, until solution is clarified, is labeled as solution S 4；
(3) solution S 4 is placed in baking oven, keeps the temperature 2-72 hours under the conditions of 303K-373K, obtains white precipitate P1, white
Precipitating P1 is filtered under the conditions of 323K-373K and is kept the temperature 12-72 hours, later in 523K- under the conditions of inert atmosphere protection
Obtain powder P2 within 623K calcination 3-8 hours；
(4) by powder P2 in oxygen protection under at 873K-973K calcination 5-24 hours, obtain white powder P3, white powder P3
Under ammonia atmosphere protection, at 1023K-1423K calcination 5-25 hours, powder P4 is obtained, powder P4 is obtained after deionized water rinse
To photocatalyst catalyst material.
3. a kind of preparation method of photocatalyst catalyst material according to claim 2, which is characterized in that in step (1)
The weight part ratio of the acetic acid and acetic anhydride is 100:5-10, and dehydrated alcohol and tantalic chloride weight part ratio are 100:10-30, molten
Liquid S1 and 2 weight ratio of solution S are 1:0.5-1.5.
4. a kind of preparation method of photocatalyst catalyst material according to claim 2, which is characterized in that in step (2)
Relative to 100 parts by weight tantalic chlorides, the dosage of calcium nitrate tetrahydrate is 70-90 parts by weight, and the dosage of lanthanum nitrate hexahydrate is
10-30 parts by weight.
5. a kind of photocatalyst preparation, which is characterized in that include photocatalyst catalyst material as described in claim 1, and support
Co-catalyst, the co-catalyst are selected from one of cobalt oxide, Platinum Nanoparticles or nano silver or a variety of.
6. a kind of photocatalyst preparation according to claim 5, which is characterized in that photocatalyst catalyst material supports cobalt oxide
The step of are as follows: photocatalyst catalyst material, cobalt nitrate are mixed with deionized water, ultrasound obtains suspension M1, and suspension M1 exists
It is dried under the conditions of 353K-403K, obtains powder P6, powder P6 is under ammonia atmosphere protection, under the conditions of 1023K-1123K, calcination
1-3 hours, powder P7 is obtained, powder P7 is touched for calcination 1-3 hours under the conditions of 423K-473K to get to the light for supporting cobalt oxide
Matchmaker's catalyst material.
7. a kind of photocatalyst preparation according to claim 6, which is characterized in that the photocatalyst catalyst of cobalt oxide will be supported
Material is mixed with platinum acid chloride solution, calcination 1-3 hours under the conditions of 400K-500K, obtains water decomposition hydrogen manufacturing type photocatalyst.
8. a kind of photocatalyst preparation according to claim 6, which is characterized in that the photocatalyst catalyst of cobalt oxide will be supported
Material, silver nitrate and ethylene glycol mixing, heat 10-30 minutes under the conditions of 393K-463K, through cooling, filter, be dried to obtain answer
Composite material C1, laccase, deionized water are mixed, are dried to obtain degradation of formaldehyde type photocatalyst by condensation material C1.
9. a kind of application of photocatalyst preparation as claimed in claim 5, which is characterized in that the photocatalyst preparation is used for moisture
Solve hydrogen manufacturing or degradation of formaldehyde.
10. a kind of application of photocatalyst preparation according to claim 9, which is characterized in that water decomposition hydrogen manufacturing type photocatalyst
Specifically used method are as follows:
(1) water decomposition hydrogen manufacturing type photocatalyst, polyvinylpyrrolidone, deionized water mixed according to weight ratio 20:1:10, ground
Mill is scratched to FTO electro-conductive glass；
(2) the FTO electro-conductive glass and platinized platinum for supporting water decomposition hydrogen manufacturing type photocatalyst are respectively as working electrode and to electrode, sulfuric acid
Sodium water solution constitutes photoelectrolytic cell as electrolyte；
(3) working electrode is as anode, and to electrode as cathode, both ends apply voltage, irradiates working electrode condition in sunlight
Lower decomposition water, cathode collect hydrogen；
The specifically used method of degradation of formaldehyde type photocatalyst are as follows:
(1) degradation of formaldehyde type photocatalyst, deionized water are mixed according to 1:20 weight ratio, ultrasonic disperse；
(2) object will be sprayed-on to clean out, the object of spraying will be avoided to be covered with film；
(3) the good spray gun of selection atomizing effect, spray gun and is kept 5-15cm distance between spray object；
(4) to be spontaneously dried by spray object.
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