CN109453798A - A kind of preparation method and application of silicon carbide-based photochemical catalyst - Google Patents
A kind of preparation method and application of silicon carbide-based photochemical catalyst Download PDFInfo
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- 229910010271 silicon carbide Inorganic materials 0.000 title claims abstract description 75
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 title claims abstract description 74
- 239000003054 catalyst Substances 0.000 title claims abstract description 30
- 238000002360 preparation method Methods 0.000 title claims abstract description 20
- 229910052982 molybdenum disulfide Inorganic materials 0.000 claims abstract description 41
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 21
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 20
- 239000000725 suspension Substances 0.000 claims abstract description 20
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 19
- 230000001699 photocatalysis Effects 0.000 claims abstract description 13
- 238000005406 washing Methods 0.000 claims abstract description 12
- 239000002608 ionic liquid Substances 0.000 claims abstract description 9
- 125000004108 n-butyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 claims abstract description 8
- 238000001291 vacuum drying Methods 0.000 claims abstract description 8
- 238000013019 agitation Methods 0.000 claims abstract description 7
- 229910052961 molybdenite Inorganic materials 0.000 claims description 35
- 239000000463 material Substances 0.000 claims description 27
- 229910052799 carbon Inorganic materials 0.000 claims description 19
- 238000006555 catalytic reaction Methods 0.000 claims description 19
- 239000008367 deionised water Substances 0.000 claims description 15
- 229910021641 deionized water Inorganic materials 0.000 claims description 15
- 238000000034 method Methods 0.000 claims description 13
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 10
- 229910052681 coesite Inorganic materials 0.000 claims description 8
- 229910052906 cristobalite Inorganic materials 0.000 claims description 8
- -1 hexafluorophosphate Chemical compound 0.000 claims description 8
- 239000000843 powder Substances 0.000 claims description 8
- 238000007789 sealing Methods 0.000 claims description 8
- 239000000377 silicon dioxide Substances 0.000 claims description 8
- 229910052682 stishovite Inorganic materials 0.000 claims description 8
- 229910052905 tridymite Inorganic materials 0.000 claims description 8
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 7
- 238000007654 immersion Methods 0.000 claims description 7
- 229910052750 molybdenum Inorganic materials 0.000 claims description 4
- 239000011733 molybdenum Substances 0.000 claims description 4
- 238000001354 calcination Methods 0.000 claims description 3
- 239000012535 impurity Substances 0.000 claims description 3
- 230000035484 reaction time Effects 0.000 claims description 2
- XRTWBRAUXVBGOO-UHFFFAOYSA-N 2-methyl-1h-imidazol-1-ium;bromide Chemical compound Br.CC1=NC=CN1 XRTWBRAUXVBGOO-UHFFFAOYSA-N 0.000 claims 1
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 41
- 239000001257 hydrogen Substances 0.000 abstract description 41
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 40
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical compound S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 abstract description 12
- 238000007146 photocatalysis Methods 0.000 abstract description 8
- 238000004519 manufacturing process Methods 0.000 abstract description 7
- 239000003426 co-catalyst Substances 0.000 abstract description 6
- PNGLEYLFMHGIQO-UHFFFAOYSA-M sodium;3-(n-ethyl-3-methoxyanilino)-2-hydroxypropane-1-sulfonate;dihydrate Chemical compound O.O.[Na+].[O-]S(=O)(=O)CC(O)CN(CC)C1=CC=CC(OC)=C1 PNGLEYLFMHGIQO-UHFFFAOYSA-M 0.000 abstract description 4
- 238000000354 decomposition reaction Methods 0.000 abstract description 2
- 229910021389 graphene Inorganic materials 0.000 abstract 1
- 238000002203 pretreatment Methods 0.000 abstract 1
- 239000002994 raw material Substances 0.000 abstract 1
- 230000002195 synergetic effect Effects 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 15
- 230000000052 comparative effect Effects 0.000 description 7
- 230000008859 change Effects 0.000 description 5
- 238000002604 ultrasonography Methods 0.000 description 5
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 239000013078 crystal Substances 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 230000007547 defect Effects 0.000 description 3
- 239000011941 photocatalyst Substances 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- 101001106045 Homo sapiens Regulator of nonsense transcripts 2 Proteins 0.000 description 2
- 102100021087 Regulator of nonsense transcripts 2 Human genes 0.000 description 2
- 150000001336 alkenes Chemical class 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 239000004020 conductor Substances 0.000 description 2
- 238000002425 crystallisation Methods 0.000 description 2
- 230000008025 crystallization Effects 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000000985 reflectance spectrum Methods 0.000 description 2
- 235000012239 silicon dioxide Nutrition 0.000 description 2
- OIWSIWZBQPTDKI-UHFFFAOYSA-N 1-butyl-3-methyl-2h-imidazole;hydrobromide Chemical compound [Br-].CCCC[NH+]1CN(C)C=C1 OIWSIWZBQPTDKI-UHFFFAOYSA-N 0.000 description 1
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 description 1
- 101000579423 Homo sapiens Regulator of nonsense transcripts 1 Proteins 0.000 description 1
- 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 1
- 102100028287 Regulator of nonsense transcripts 1 Human genes 0.000 description 1
- 102100029938 Serine/threonine-protein kinase SMG1 Human genes 0.000 description 1
- 101710085356 Serine/threonine-protein kinase SMG1 Proteins 0.000 description 1
- 229910003978 SiClx Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 238000003760 magnetic stirring Methods 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 229940085991 phosphate ion Drugs 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 125000004434 sulfur atom Chemical group 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 238000010189 synthetic method Methods 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
Classifications
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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
- B01J27/20—Carbon compounds
- B01J27/22—Carbides
- B01J27/224—Silicon carbide
-
- 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
- B01J35/33—Electric or magnetic properties
-
- 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
- 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
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/61—Surface area
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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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- Chemical Kinetics & Catalysis (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
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- Carbon And Carbon Compounds (AREA)
Abstract
The invention discloses a kind of silicon carbide-based double midwifery hydrogen photochemical catalysts and preparation method thereof, comprising the following steps: a carries out pre-treatment to silicon carbide；B prepares entire hydro-thermal reaction system 8wt% molybdenum disulfide suspension using molybdenum disulfide as raw material；C takes 100mL 8wt% molybdenum disulfide suspension to be placed in a beaker, sequentially add silicon carbide (SiC), graphene oxide (GO) and 2 drop 1- butyl -3- methyl miaow diindyl hexafluorophosphoric acid ionic liquids, ultrasonic agitation is uniformly mixed it, d is transferred them in pyroreaction kettle, 20h is reacted at 220 DEG C, it is then centrifuged for washing to pH=7, places it in vacuum oven, it is spare after vacuum drying.Hydrothermal synthesis obtains silicon carbide-based double midwifery hydrogen photochemical catalysts.The present invention utilizes GO and molybdenum disulfide (MoS2) double co-catalysts synergistic effect, silicon carbide-based double midwifery hydrogen photochemical catalysts of preparation improve the performance of visible light photocatalysis hydrogen production by water decomposition, can establish certain basis for the application of its subsequent efficient visible light catalyst.
Description
Technical field
The present invention relates to a kind of preparation methods of visible-light photocatalyst, and in particular to a kind of silicon carbide-based double midwifery hydrogen light
Catalyst and preparation method thereof.
Background technique
Currently, well known production hydrogen photochemical catalyst is with TiO mostly2Based on be modified and make it more meet visible light light to urge
Change the requirement for producing hydrogen, promotes hydrogen generation efficiency.The catalyst has certain catalytic action, but the semiconductor material of low energy gap width
Material more meets the requirement that ultraviolet light photocatalysis produces hydrogen.In view of SiC to the good response and its conduction band of visible light, the position of valence band
The requirement of photocatalytic water is fully met, and is used to photocatalytic hydrogen production by water decomposition.But itself there are some defects to make it in light
There are certain difficulty in terms of Xie Shui, it is mainly manifested in the following aspects: first is that SiC has certain hydrophobicity, leading to it
It is more difficult to contact with hydrone；Second is that electron hole be easy it is compound so that hydrogen generation efficiency is low.Based on above some disadvantages, in order to change
Kind SiC Photocatalyzed Hydrogen Production efficiency, being modified using co-catalyst is common resolving ideas.And currently, Yuan Wenxia seminar
Modification is doped to SiC using CdS and Pt, production hydrogen rate is 259 μm of olh-1g-1.But Cd is heavy metal, and there are certain two
Secondary pollution risk, and Pt is noble metal, large-scale industrial application is subject to certain restrictions.Applicant utilizes MoS2And graphite oxide
The coordinative role of alkene (GO) double co-catalysts is doped SiC, utilizes MoS2And the advantages of GO, constructs SiC base visible light catalytic
Hydrogen material is produced, to make up the deficiency of SiC base visible light catalyst.
Summary of the invention
The purpose of the present invention is to provide a kind of preparation method of silicon carbide-based double midwifery hydrogen photochemical catalysts, this method is made
The catalyst obtained introduces GO and MoS2As double co-catalysts, is acted synergistically using double co-catalysts and be modified SiC, to improve its light
It is catalyzed hydrogen generation efficiency.
The adopted technical solution is that:
A kind of preparation method of silicon carbide-based photochemical catalyst, specifically includes the following steps:
(1) pure SiC preparation: SiC powder is roasted at high temperature, is down to room temperature naturally, to remove carbon impurity；Then in quality point
Number is that sealing is protected from light immersion in 2%HF solution, removes SiO2With other oxides；Finally washing is centrifuged repeatedly extremely with deionized water
PH=7 are placed in vacuum oven, obtain pure SiC；
(2) MoS2Suspension: by MoS2It is placed in deionized water, is uniformly mixed, obtains MoS2Suspension；
(3) it mixes: toward MoS2In suspension, pure SiC, GO and ionic liquid are sequentially added, ultrasonic agitation is uniformly mixed it；
(4) hydro-thermal reaction prepares silicon carbide-based pair and helps photochemical catalyst: the solution that step (3) obtains is transferred to pyroreaction kettle
In, a period of time is reacted at 220 DEG C, is then centrifuged for washing to pH=7, vacuum drying obtains catalysis material.
Further, in the step (1) maturing temperature be 600-800 DEG C, preferably 700 DEG C, calcining time 2-6h,
Preferably 5h, vacuum drying temperature are 60 DEG C.
Further, in step (3) hydrothermal system, MoS is calculated with molybdenum element2Mass percent be 2-10%, it is excellent
It is selected as 8%；The mass percent of the GO in terms of carbon is 0.5-3%, preferably 2.5%.
Further, the ultrasonic agitation time is 10h in the step (3), and the hydro-thermal reaction time is in the step (4)
20h, vacuum drying temperature are 60 DEG C.
Further, the ionic liquid in the step (3) includes but is not limited to 1- butyl -3- methyl miaow diindyl hexafluorophosphoric acid
Salt, 1- butyl -3-- methyl imidazolium tetrafluoroborate, 1- butyl -3- methylimidazole bromide and 1- ethyl-3-methylimidazole-tetrafluoro
One of borate.
The photocatalyst applications of the method preparation produce hydrogen rate in 55 μm of olh in photocatalytic water-1·g-1More than.
The method have the benefit that:
MoS in modifying process2As a kind of layered transition metal sulfide, active S atom is located at the edge of exposure, can be with
Increase the active site of Photocatalyzed Hydrogen Production, GO has biggish surface area and good electron transmission ability, light can be improved and urge
Change activity, more importantly MoS2It acts synergistically with GO, makes silicon carbide-based double midwifery hydrogen photochemical catalysts compared to silicon carbide
Itself and silicon carbide-based single midwifery hydrogen photochemical catalyst have higher Photocatalyzed Hydrogen Production efficiency, and its synthetic method is simpler
It is single, easy to operate, one-step synthesis.
Detailed description of the invention
Fig. 1 is MoS produced by the present invention2Silicon carbide-based double midwifery hydrogen photochemical catalyst XRD spectras of load capacity variation.
Fig. 2 is the XRD spectra of silicon carbide-based double midwifery hydrogen photochemical catalysts of GO load capacity produced by the present invention variation
Fig. 3 is self-control light-catalyzed reaction system.
Fig. 4 is MoS produced by the present invention2Silicon carbide-based double midwifery hydrogen photochemical catalysts, the pure silicon carbide, carbon of load capacity variation
SiClx base list midwifery hydrogen photochemical catalyst 4h hydrogen generation efficiency figure.
Fig. 5 is silicon carbide-based double midwifery hydrogen photochemical catalyst 4h hydrogen generation efficiency figures of GO load capacity produced by the present invention variation.
Fig. 6 is MoS produced by the present invention2The silicon carbide-based double midwifery hydrogen photochemical catalysts and pure silicon carbide of load capacity variation
Ultraviolet-visible diffuse reflectance spectrum figure.
Specific embodiment
Below by specific embodiment, the invention will be further described.
Embodiment 1
(1) it prepares pure SiC: SiC powder is placed in Muffle furnace, 5h is roasted at 700 DEG C, is down to room temperature naturally, to go to clean
Matter carbon；Sealing is protected from light immersion one the whole night in 2%HF solution, removes SiO2With other oxides；It is centrifuged repeatedly and is washed with deionized water
11 times are washed to pH=7, vacuum oven is placed in, is dried in vacuo at 60 DEG C；
(2) MoS2Suspension: at room temperature, by 0.1741gMoS2It is placed in 100mL deionized water, is uniformly mixed, obtains MoS2It suspends
Liquid；
(3) it mixes: at room temperature, toward MoS25.0g pure SiC, 0.05gGO and 2 drop 1- butyl -3- first are sequentially added in suspension
Base miaow diindyl hexafluorophosphoric acid ionic liquid, ultrasonic wave stirring 10h are uniformly mixed it；
(4) hydrothermal synthesis method prepares silicon carbide-based double midwifery hydrogen catalysis materials: the solution after above-mentioned ultrasound is placed in 300mL high
In warm reaction kettle, 20h is reacted at 220 DEG C, washing is then centrifuged for 5 times to pH=7, vacuum oven is placed it in, at 60 DEG C
It is dried in vacuo, obtains SGM-2 catalysis material.MoS2Mass percent in hydro-thermal reaction system is 2%(with molybdenum member
Element calculates).
Embodiment 2
The present embodiment removes step (2) MoS2For 0.4590gMoS2, other are same as Example 1, obtain SGM-5 photocatalysis material
Material；MoS2Mass percent in hydro-thermal reaction system is that 5%(is calculated with molybdenum element).
Embodiment 3
The present embodiment removes step (2) MoS2For 0.7769g MoS2, other are same as Example 1, obtain SGM-8 photocatalysis material
Material；MoS2Mass percent in hydro-thermal reaction system is that 8%(is calculated with molybdenum element).
Embodiment 4
The present embodiment removes step (2) MoS2For 1.01g MoS2, other are same as Example 1, obtain SGM-10 photocatalysis material
Material；MoS2Mass percent in hydro-thermal reaction system is that 10%(is calculated with molybdenum element).
Fig. 1 is MoS prepared by pure SiC and embodiment 1-42Silicon carbide-based double midwifery hydrogen photocatalysis materials of load capacity variation
Expect XRD spectra.As shown in Figure 1, compared to pure SiC, left avertence shifting occurs for other sample characteristic peaks, and wherein sample SGM-8 is deviated
Degree is maximum, and its characteristic peak enhanced strength degree is maximum.Thus illustrate, MoS2The change of load capacity has SiC crystal growth
Facilitation.Sample SGM-10 slightly dies down compared to the intensity of sample SGM-8 characteristic peak, illustrates that sample preparation procedure exists
MoS2Optimum load range.Sample SGM-8 crystal form is best, and good crystallization can reduce the defect of conductor photocatalysis, is conducive to light
Raw carrier transmits between lattice in lattice, to improve light-catalysed activity.
Embodiment 5
(1) it prepares pure SiC: SiC powder is placed in Muffle furnace, 5h is roasted at 700 DEG C, is down to room temperature naturally, to go to clean
Matter carbon；Sealing is protected from light immersion one the whole night in 2%HF solution, removal SiO2 and other oxides；It is centrifuged repeatedly and is washed with deionized water
11 times are washed to pH=7, vacuum oven is placed in, is dried in vacuo at 60 DEG C；
(2) MoS2 suspension: at room temperature, being placed in 100mL deionized water for 0.7769gMoS2, is uniformly mixed, and obtains MoS2 suspension
Liquid；
(3) it mixes: at room temperature, toward MoS25.0g pure SiC, 0.0583gGO and 2 drop 1- butyl -3- are sequentially added in suspension
Methyl miaow diindyl hexafluorophosphoric acid ionic liquid, ultrasonic wave stirring 10h are uniformly mixed it；
(4) hydrothermal synthesis method prepares silicon carbide-based double midwifery hydrogen catalysis materials: the solution after above-mentioned ultrasound is placed in 300mL high
In warm reaction kettle, 20h is reacted at 220 DEG C, washing is then centrifuged for 5 times to pH=7, vacuum oven is placed it in, at 60 DEG C
It is dried in vacuo, obtains SMG-1 catalysis material.Mass percent of the GO in hydro-thermal reaction system is 1%(with carbon
It calculates).
Embodiment 6
The present embodiment is 0.0880gGO except step (3) GO, other are same as Example 5, obtain SMG-1.5 catalysis material；
Mass percent of the GO in hydro-thermal reaction system is that 1.5%(is calculated with carbon).
Embodiment 7
The present embodiment is 0.1178gGO except step (3) GO, other are same as Example 5, obtain SMG-2 catalysis material；GO
Mass percent in hydro-thermal reaction system is that 2%(is calculated with carbon).
Embodiment 8
The present embodiment is 0.1481gGO except step (3) GO, other are same as Example 5, obtain SMG-2.5 catalysis material；
Mass percent of the GO in hydro-thermal reaction system is that 2.5%(is calculated with carbon).
Embodiment 9
The present embodiment is 0.1787gGO except step (3) GO, other are same as Example 5, obtain SMG-3 catalysis material；Institute
Stating mass percent of the GO in step (3) in hydrothermal system is that 3%(is calculated with carbon).
Embodiment 10
(1) it prepares pure SiC: SiC powder is placed in Muffle furnace, 6h is roasted at 600 DEG C, is down to room temperature naturally, to go to clean
Matter carbon；Sealing is protected from light immersion one the whole night in 2%HF solution, removal SiO2 and other oxides；It is centrifuged repeatedly and is washed with deionized water
11 times are washed to pH=7, vacuum oven is placed in, is dried in vacuo at 60 DEG C；
(2) MoS2 suspension: at room temperature, being placed in 100mL deionized water for 0.8gMoS2, is uniformly mixed, obtains MoS2 suspension；
(3) it mixes: at room temperature, toward MoS25.0g pure SiC, 0.0583gGO and 2 drop 1- ethyl -3- are sequentially added in suspension
Methyl imidazolium tetrafluoroborate ionic liquid, ultrasonic wave stirring 10h are uniformly mixed it；
(4) hydrothermal synthesis method prepares silicon carbide-based double midwifery hydrogen catalysis materials: the solution after above-mentioned ultrasound is placed in 300mL high
In warm reaction kettle, 20h is reacted at 220 DEG C, washing is then centrifuged for 5 times to pH=7, vacuum oven is placed it in, at 60 DEG C
It is dried in vacuo, obtains catalysis material.
Fig. 2 is silicon carbide-based double midwifery hydrogen catalysis materials of GO load capacity variation prepared by pure SiC and embodiment 5-9
XRD spectra.As shown in Figure 2, compared to pure SiC, right avertence shifting occurs for other sample characteristic peaks, and wherein sample SMG-2.5 is deviated
Degree is maximum, and its characteristic peak enhanced strength degree is maximum.Thus illustrate, the change of GO load capacity there is rush to SiC crystal growth
Into effect.Sample SMG-3 slightly dies down compared to the intensity of sample SMG-2.5 characteristic peak and moves to right degree reduction, illustrates sample
There are GO optimum load ranges for preparation process.Sample SMG-2.5 crystal form is best, and good crystallization can reduce conductor photocatalysis
Defect is transmitted between lattice in lattice conducive to photo-generated carrier, to improve light-catalysed activity.
Comparative example 1
SiC powder is placed in Muffle furnace, 5h is roasted at 700 DEG C, is down to room temperature naturally, to remove carbon impurity, then 2%
Sealing is protected from light immersion one the whole night in HF solution, removes SiO2With other oxides；Washing is centrifuged repeatedly 12 times extremely with deionized water
PH=7 are placed in vacuum oven, are dried in vacuo at 60 DEG C, obtain pure SiC.
Comparative example 2
(1) it prepares pure SiC: SiC powder is placed in Muffle furnace, 5h is roasted at 700 DEG C, is down to room temperature naturally, to go to clean
Matter carbon；Sealing is protected from light immersion one the whole night in 2%HF solution, removes SiO2With other oxides；It is centrifuged repeatedly and is washed with deionized water
11 times are washed to pH=7, vacuum oven is placed in, is dried in vacuo at 60 DEG C；
(2) MoS2Suspension: at room temperature, by 0.7769gMoS2It is placed in 100mL deionized water, is uniformly mixed, obtains MoS2It suspends
Liquid；
(3) it mixes: at room temperature, 5.0g pure SiC, 0.5898gMoS is sequentially added into molybdenum disulfide solution2(in hydrothermal system
Mass fraction is 0.85%) and 2 drop 1- butyl -3- methyl miaow diindyl hexafluorophosphoric acid ionic liquids, ultrasonic agitation 10h make its mixing
Uniformly；
(4) hydrothermal synthesis method prepares SiC/M-8 and produces hydrogen catalysis material: it is anti-that the solution after above-mentioned ultrasound is placed in 300mL high temperature
It answers in kettle, reacts 20h at 220 DEG C, be then centrifuged for washing 5 times to pH=7, place it in vacuum oven, carried out at 60 DEG C
Vacuum drying, obtains SiC/M-8 catalysis material.
Comparative example 3
(1) it prepares pure SiC: SiC powder is placed in Muffle furnace, 3h is roasted at 700 DEG C, is down to room temperature naturally, to go to clean
Matter carbon；Sealing, which is protected from light, in 2%HF solution impregnates 5h, removes SiO2With other oxides；Washing 11 is centrifuged repeatedly with deionized water
It is secondary to pH=7, be placed in vacuum oven, be dried in vacuo at 60 DEG C；
(2) GO suspension: at room temperature, being placed in 100mL deionized water for 0.4391gGO, is uniformly mixed, obtains GO suspension；
(3) at room temperature, 5.0g pure SiC, 0.05gGO and 2 drop 1- butyl -3- methyl miaow diindyl hexafluoros are sequentially added into GO suspension
Phosphate ion liquid, ultrasonic agitation 10h are uniformly mixed it；
(4) hydrothermal synthesis method prepares SiC/GO and produces hydrogen catalysis material: the solution after above-mentioned ultrasound is placed in 300mL pyroreaction
In kettle, 20h is reacted at 220 DEG C, washing 5 times is then centrifuged for pH=7, places it in vacuum oven, carried out at 60 DEG C true
Sky is dry, obtains SiC/GO catalysis material.Mass percent of the GO in hydrothermal system in the step (2) be 8%(with
Carbon calculates).
(as shown in Figure 3) weighs multiple made from embodiment 1-9 and comparative example 1-3 respectively in self-control light-catalyzed reaction system
It closes visible-light photocatalyst 0.5g and is scattered in 100mL Na containing 0.1M2S·9H2O and 0.1M Na2SO3For the aqueous solution of sacrifice agent
In, and open magnetic stirring apparatus.Before illumination, it is passed through N230min is to guarantee entire reaction system in N2Protection under carry out, 4h
Afterwards, 1mL gas is extracted with airtight needle, with gas Chromatographic Determination hydrogen output.Hydrogen generation efficiency is shown in Fig. 4 and Fig. 5 after 4h.
By Fig. 4 and Fig. 5 it is found that under experimental conditions, the hydrogen generation efficiency of embodiment 8 is compared to other embodiments and right
Ratio, hydrogen generation efficiency highest.By comparing each embodiment and each comparative example, it can be seen that GO and MoS2Double co-catalysts can be with
The photocatalytic activity for improving SiC, to improve hydrogen generation efficiency.
Embodiment 1- 4 and the sample of comparative example 1 are characterized using ultraviolet-visible diffuse reflectance spectrum respectively.Ultraviolet-
It can be seen that diffusing reflection spectrum is shown in Fig. 6.
It will be appreciated from fig. 6 that embodiment, compared to comparative example 1, obvious red shift, and embodiment 3 and implementation occur for absorption peak side length
4 red shift degree of example is close.
The above description is only an embodiment of the present invention, is not intended to limit protection scope of the present invention, all to utilize this hair
Equivalent structure made by bright specification or equivalent process exchange, are applied directly or indirectly in other related fieldss, similarly wrap
It includes in protection protection scope of the invention.
Claims (7)
1. a kind of preparation method of silicon carbide-based photochemical catalyst, which is characterized in that specifically includes the following steps:
(1) pure SiC preparation: SiC powder is roasted at high temperature, is down to room temperature naturally, to remove carbon impurity；Then in quality point
Number is that sealing is protected from light immersion in 2%HF solution, removes SiO2With other oxides；Finally washing is centrifuged repeatedly extremely with deionized water
PH=7 are placed in vacuum oven, obtain pure SiC；
(2) MoS2Suspension: by MoS2It is placed in deionized water, is uniformly mixed, obtains MoS2Suspension；
(3) it mixes: to MoS2In suspension, pure SiC, GO and ionic liquid are sequentially added, ultrasonic agitation is uniformly mixed it；
(4) hydro-thermal reaction prepares silicon carbide-based photochemical catalyst: the solution that step (3) obtains is transferred in pyroreaction kettle, in
A period of time is reacted at 220 DEG C, is then centrifuged for washing to pH=7, vacuum drying obtains catalysis material, the hydro-thermal reaction body
In system, the MoS in terms of molybdenum element2Mass percent be 2-10%, the mass percent of the GO in terms of carbon is 0.5-3%.
2. the preparation method of silicon carbide-based photochemical catalyst according to claim 1, which is characterized in that in the step (1)
Maturing temperature is 600-800 DEG C, calcining time 2-6h, and vacuum drying temperature is 60 DEG C.
3. the preparation method of silicon carbide-based photochemical catalyst according to claim 1, which is characterized in that in the step (1)
Maturing temperature is 700 DEG C, calcining time 5h.
4. the preparation method of silicon carbide-based photochemical catalyst according to claim 1, which is characterized in that in hydro-thermal reaction system
In, the MoS in terms of molybdenum element2Mass percent be 8%, the mass percent of the GO in terms of carbon is 0.85%.
5. the preparation method of silicon carbide-based photochemical catalyst according to claim 1, which is characterized in that in the step (3)
The ultrasonic agitation time is 10h, and the hydro-thermal reaction time is 20h in the step (4), and vacuum drying temperature is 60 DEG C.
6. the preparation method of silicon carbide-based photochemical catalyst according to claim 1, which is characterized in that in the step (3)
Ionic liquid be 1- butyl -3- methyl miaow diindyl hexafluorophosphate, 1- butyl -3- methyl imidazolium tetrafluoroborate, 1- butyl -3-
One of methylimidazole bromide and 1- ethyl-3-methylimidazole tetrafluoroborate.
7. application of the photochemical catalyst of claim 1-6 the method preparation in terms of photocatalytic water.
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| CN113083339B (en) * | 2021-04-15 | 2022-11-08 | 万华化学(四川)有限公司 | Catalyst for preparing vitamin E and preparation method and application thereof |
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