CN113996324A - For CO2Preparation method of SiC-C composite aerogel through photocatalytic reduction - Google Patents
For CO2Preparation method of SiC-C composite aerogel through photocatalytic reduction Download PDFInfo
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- 238000000034 method Methods 0.000 title claims abstract description 27
- 239000002131 composite material Substances 0.000 title claims abstract description 26
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 17
- 238000010438 heat treatment Methods 0.000 claims abstract description 21
- 239000002243 precursor Substances 0.000 claims abstract description 15
- 238000002360 preparation method Methods 0.000 claims abstract description 10
- 238000000352 supercritical drying Methods 0.000 claims abstract description 10
- 239000012298 atmosphere Substances 0.000 claims abstract description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 48
- 239000000463 material Substances 0.000 claims description 26
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 25
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 25
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 21
- YCIMNLLNPGFGHC-UHFFFAOYSA-N catechol Chemical compound OC1=CC=CC=C1O YCIMNLLNPGFGHC-UHFFFAOYSA-N 0.000 claims description 18
- GHMLBKRAJCXXBS-UHFFFAOYSA-N resorcinol Chemical compound OC1=CC=CC(O)=C1 GHMLBKRAJCXXBS-UHFFFAOYSA-N 0.000 claims description 18
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 16
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims description 16
- 238000001035 drying Methods 0.000 claims description 16
- 239000002904 solvent Substances 0.000 claims description 15
- 239000001569 carbon dioxide Substances 0.000 claims description 12
- 239000000203 mixture Substances 0.000 claims description 12
- 238000003756 stirring Methods 0.000 claims description 11
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 10
- 238000006243 chemical reaction Methods 0.000 claims description 10
- NBBJYMSMWIIQGU-UHFFFAOYSA-N Propionic aldehyde Chemical compound CCC=O NBBJYMSMWIIQGU-UHFFFAOYSA-N 0.000 claims description 8
- HUMNYLRZRPPJDN-UHFFFAOYSA-N benzaldehyde Chemical compound O=CC1=CC=CC=C1 HUMNYLRZRPPJDN-UHFFFAOYSA-N 0.000 claims description 8
- 239000000499 gel Substances 0.000 claims description 7
- 239000011240 wet gel Substances 0.000 claims description 7
- WYTZZXDRDKSJID-UHFFFAOYSA-N (3-aminopropyl)triethoxysilane Chemical compound CCO[Si](OCC)(OCC)CCCN WYTZZXDRDKSJID-UHFFFAOYSA-N 0.000 claims description 6
- 230000032683 aging Effects 0.000 claims description 6
- 150000001299 aldehydes Chemical class 0.000 claims description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- IKHGUXGNUITLKF-XPULMUKRSA-N acetaldehyde Chemical compound [14CH]([14CH3])=O IKHGUXGNUITLKF-XPULMUKRSA-N 0.000 claims description 4
- ZTQSAGDEMFDKMZ-UHFFFAOYSA-N butyric aldehyde Natural products CCCC=O ZTQSAGDEMFDKMZ-UHFFFAOYSA-N 0.000 claims description 4
- JJQZDUKDJDQPMQ-UHFFFAOYSA-N dimethoxy(dimethyl)silane Chemical compound CO[Si](C)(C)OC JJQZDUKDJDQPMQ-UHFFFAOYSA-N 0.000 claims description 4
- BFXIKLCIZHOAAZ-UHFFFAOYSA-N methyltrimethoxysilane Chemical compound CO[Si](C)(OC)OC BFXIKLCIZHOAAZ-UHFFFAOYSA-N 0.000 claims description 4
- QNGNSVIICDLXHT-UHFFFAOYSA-N para-ethylbenzaldehyde Natural products CCC1=CC=C(C=O)C=C1 QNGNSVIICDLXHT-UHFFFAOYSA-N 0.000 claims description 4
- 229920000642 polymer Polymers 0.000 claims description 4
- 230000001681 protective effect Effects 0.000 claims description 4
- CPUDPFPXCZDNGI-UHFFFAOYSA-N triethoxy(methyl)silane Chemical compound CCO[Si](C)(OCC)OCC CPUDPFPXCZDNGI-UHFFFAOYSA-N 0.000 claims description 4
- JPYHHZQJCSQRJY-UHFFFAOYSA-N Phloroglucinol Natural products CCC=CCC=CCC=CCC=CCCCCC(=O)C1=C(O)C=C(O)C=C1O JPYHHZQJCSQRJY-UHFFFAOYSA-N 0.000 claims description 3
- KPUWHANPEXNPJT-UHFFFAOYSA-N disiloxane Chemical class [SiH3]O[SiH3] KPUWHANPEXNPJT-UHFFFAOYSA-N 0.000 claims description 3
- 239000001307 helium Substances 0.000 claims description 3
- 229910052734 helium Inorganic materials 0.000 claims description 3
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 claims description 3
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 claims description 3
- 125000005375 organosiloxane group Chemical group 0.000 claims description 3
- QCDYQQDYXPDABM-UHFFFAOYSA-N phloroglucinol Chemical compound OC1=CC(O)=CC(O)=C1 QCDYQQDYXPDABM-UHFFFAOYSA-N 0.000 claims description 3
- 229960001553 phloroglucinol Drugs 0.000 claims description 3
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 238000004321 preservation Methods 0.000 claims description 2
- 238000002210 supercritical carbon dioxide drying Methods 0.000 claims 1
- 238000005516 engineering process Methods 0.000 abstract description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052799 carbon Inorganic materials 0.000 abstract description 3
- 239000007783 nanoporous material Substances 0.000 abstract description 3
- 239000011941 photocatalyst Substances 0.000 abstract description 3
- 238000005265 energy consumption Methods 0.000 abstract description 2
- 239000011261 inert gas Substances 0.000 abstract description 2
- 230000031700 light absorption Effects 0.000 abstract description 2
- 238000004519 manufacturing process Methods 0.000 abstract 1
- 238000006386 neutralization reaction Methods 0.000 abstract 1
- 238000003980 solgel method Methods 0.000 abstract 1
- 239000011259 mixed solution Substances 0.000 description 5
- IKHGUXGNUITLKF-UHFFFAOYSA-N Acetaldehyde Chemical compound CC=O IKHGUXGNUITLKF-UHFFFAOYSA-N 0.000 description 4
- 229910052681 coesite Inorganic materials 0.000 description 4
- 229910052906 cristobalite Inorganic materials 0.000 description 4
- 239000000377 silicon dioxide Substances 0.000 description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 4
- 229910052682 stishovite Inorganic materials 0.000 description 4
- 229910052905 tridymite Inorganic materials 0.000 description 4
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- 239000012300 argon atmosphere Substances 0.000 description 2
- 238000007334 copolymerization reaction Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000012299 nitrogen atmosphere Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000002800 charge carrier Substances 0.000 description 1
- 239000000084 colloidal system Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- PKTOVQRKCNPVKY-UHFFFAOYSA-N dimethoxy(methyl)silicon Chemical compound CO[Si](C)OC PKTOVQRKCNPVKY-UHFFFAOYSA-N 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 239000002784 hot electron Substances 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
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- 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
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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
- 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
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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
- C01B32/00—Carbon; Compounds thereof
- C01B32/40—Carbon monoxide
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
- C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
- C07C1/12—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon dioxide with hydrogen
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Abstract
The invention belongs to the field of preparation technology of nano porous materials, and relates to a method for preparing CO2A preparation method of SiC-C composite aerogel through photocatalytic reduction. Preparing organic-inorganic hybrid precursor aerogel by adopting a sol-gel method and combining a supercritical drying process, and then carrying out high-temperature heat treatment in a tubular furnace containing inert gas atmosphere, thereby preparing the SiC-C composite aerogel. The photocatalyst prepared by the invention has the advantages of simple method, low energy consumption, low density, high specific surface and better CO2The photocatalytic reduction performance meets the requirements of green and low carbonThe life concept of (1). The high specific surface, high conductivity and excellent light absorption performance of the C-based aerogel enable the SiC-C composite aerogel to have better photoresponse capability, and have positive production significance for realizing carbon neutralization and carbon peak reaching.
Description
Technical Field
The invention belongs to the field of preparation technology of nano porous materials, and relates to a method for preparing CO2A preparation method of SiC-C composite aerogel through photocatalytic reduction, in particular to a preparation method of SiC-C aerogel material through copolymerization, supercritical drying process and high-temperature heat treatment.
Background
In recent years, combustion of fossil fuels has produced large amounts of CO2The global greenhouse effect is becoming more serious, and fossil energy is also facing the problem of energy exhaustion. Carbon dioxide is an inert gas, which makes it difficult to activate carbon dioxide. Reduction of CO2The method can be realized by a photocatalytic technology, an electrocatalytic technology, hydrogenation reduction, thermocatalytic reduction and the like. In which the photocatalytic technique is applied to CO2The reduction only needs illumination, the operation is simple, electric energy and heat energy are not consumed, and secondary pollution is not caused. The problem of greenhouse effect is relieved, and simultaneously, carbon resources are effectively converted and utilized, so that CO is reduced by photocatalysis2The technology is widely concerned at home and abroad.
The C-based material has higher specific surface area and higher electric conductivity, and is used for CO2Photocatalytic reduction would be a good material. Preparation of Ag-doped g-C by one-step pyrolysis of Li and the like3N4the/C composite material promotes the separation of photogenerated electron-hole pairs, generates additional active hot electrons, improves the utilization efficiency of light energy, and has the CO yield of 33.3 mu mol/(g.h) under visible light (Journal of Colloid and Interface Science,2021.08 (176)). Huang et al prepared g-C of inverse opal structure by hard template method3N4Introduction of phosphorus by heat treatment greatly enhances g-C3N4The light absorption capacity of the material, the band gap is reduced, the recombination of photogenerated charge carriers is inhibited, and the CO adding yield is up to 32.22 mu mol/(g.h). (Catalysis Science)&Technology,2021,10(11))。The aerogel material is a three-dimensional nano porous material with the characteristics of high specific surface area, low density, high porosity and the like, and is an ideal catalyst carrier. By combining the aerogel technology with the photocatalytic technology, the photocatalyst is fixed by utilizing the huge surface area and stable physicochemical properties of the aerogel, the photocatalyst is highly dispersed, and a light receiving surface and reaction sites are increased, so that the photocatalytic performance of the material is improved.
Disclosure of Invention
The invention aims to provide a method for preparing CO2A preparation method of SiC-C composite aerogel through photocatalytic reduction, wherein a copolymerization method is used for preparing the SiC-C composite aerogel material, and the SiC-C composite aerogel material has a three-dimensional nano porous network structure, a larger specific surface area and a more uniform network framework structure and can be used for CO2Has excellent adsorption performance and is more convenient to activate CO2. The method has the advantages of simple adopted raw materials and process, low energy consumption and ideal photocatalytic material. The prepared SiC-C composite aerogel has excellent photocatalytic CO2And (4) performance.
The technical scheme of the invention is as follows: for CO2The preparation method of the SiC-C composite aerogel through photocatalytic reduction comprises the following specific steps:
(1) uniformly mixing phenol, aldehyde and an alcohol solvent, and uniformly stirring to obtain a polymer precursor A;
(2) adding organic siloxane into the polymer precursor A, uniformly stirring the mixture until the mixture is gelled, and standing the mixture at room temperature;
(3) adding the gel obtained in the step (2) into an aging solution, aging in an oven, and then carrying out solvent replacement;
(4) performing carbon dioxide supercritical drying on the wet gel obtained in the step (3) to obtain an organic-inorganic hybrid precursor aerogel material;
(5) and (4) carrying out heat treatment on the organic-inorganic hybrid precursor aerogel material obtained in the step (4) in a tubular furnace containing protective atmosphere to finally obtain the SiC-C composite aerogel material.
Preferably, the phenol in the step (1) is one or more of catechol, resorcinol or phloroglucinol; the aldehyde is one or more of formaldehyde, acetaldehyde, propionaldehyde or benzaldehyde; the alcohol solvent is one or more of methanol, ethanol or isopropanol; the aldehyde, the phenol and the alcohol solvent are uniformly mixed according to the volume ratio of (1-5) to (1) - (5-15).
Preferably, the stirring temperature in the step (1) is 20-40 ℃, and the stirring time is 20-60 min.
Preferably, the organic siloxane in the step (2) is one or more of 3-aminopropyltriethoxysilane, methyltriethoxysilane, methyltrimethoxysilane or dimethyldimethoxysilane; the organosiloxane and the phenol are mixed in a volume ratio of (0.5-3): 1.
Preferably, the temperature for uniform stirring in the step (2) is 20-40 ℃; the standing time is 15-30 h.
Preferably, the aging solution in step (3) is a mixture of one or more of methanol, ethanol, diethyl ether or isopropanol.
Preferably, the temperature of the oven in the step (3) is 20-60 ℃; the solvent replacement times are 3-9 times, and the interval time of each time is 8-24 hours.
Preferably, the carbon dioxide supercritical drying method in the step (4) comprises: carbon dioxide is used as a drying medium, the reaction temperature is 40-90 ℃, the pressure in the high-pressure reaction kettle is 8-12 MPa, the drying rate is 5-10L/min, and the drying time is 8-16 h.
Preferably, the protective atmosphere in the step (5) is one or a mixture of argon, helium and nitrogen; the heat treatment temperature is 1000-1600 ℃, the heating rate is 1-5 ℃/min, and the heat treatment heat preservation time is 2-8 h.
Has the advantages that:
(1) the method has the advantages of easily available raw materials, low cost and simple process.
(2) The SiC/C composite aerogel prepared by the method is a complete block aerogel material with high porosity, is convenient to recover and is convenient for industrial production.
(3) The SiC/C composite aerogel prepared by the method has larger specific surface area, more uniform network framework structure and good photocatalytic performance.
Drawings
FIG. 1 is a photocatalytic reduction of CO of the SiC-C composite aerogel prepared in example 12CH (A) of4And CO2Yield map of (a);
FIG. 2 is a physical diagram of the SiC-C composite aerogel prepared in example 2.
Detailed Description
The invention is further illustrated by the following examples, without limiting the scope of protection.
Example 1
1.34g of catechol, 3mL of formaldehyde and 12mL of ethanol were added to a beaker, stirred at 30 ℃ for 30min to form a uniformly mixed solution (the volume ratio of formaldehyde, catechol and ethanol was 3:1:12), followed by addition of 1.5mL of 3-aminopropyltriethoxysilane (the volume ratio of 3-aminopropyltriethoxysilane to catechol was 1.5:1), stirred at 30 ℃ to gel, and allowed to stand at room temperature for 24 h. Ethanol was added to the samples and aged in an oven at 50 ℃ during which time the samples were washed 9 times with ethanol at 8h intervals. And after the solvent replacement is finished, carrying out carbon dioxide supercritical drying on the wet gel, setting the drying temperature to be 50 ℃, the drying speed to be 8L/min, maintaining the constant pressure to be 10MPa for 12h, closing air inlet, and releasing the pressure in the reaction kettle to obtain the precursor aerogel material. And taking out the precursor aerogel material, heating to 1500 ℃ at the heating rate of 5 ℃/min in a tubular furnace containing argon atmosphere, and preserving heat for 3h to obtain the SiC/C composite aerogel. FIG. 1 shows the photocatalytic reduction of CO by the prepared SiC/C composite aerogel2CH (A) of4And CO2From the graph, it can be seen that CH is present under the condition of 2 hours of visible light irradiation4The yield of (2) is 4.36 mu mol/(g.h), and the yield of CO is 1.18 mu mol/(g.h).
Example 2
1.27g of resorcinol, 1mL of acetaldehyde and 5mL of methanol were added to a beaker and stirred at 20 ℃ for 60min to form a uniformly mixed solution (acetaldehyde, resorcinol and methanol in a volume ratio of 1:1:5), followed by the addition of 0.5mL of methyltriethoxysilane (methyltriethoxysilane to resorcinol in a volume ratio of 0.5:1), stirred at 20 ℃ to gel and allowed to stand at room temperature for 15 h. To the sampleMethanol was added and the mixture was aged in an oven at 20 ℃ during which it was washed 3 times with methanol at 24h intervals. And after the solvent replacement is finished, carrying out carbon dioxide supercritical drying on the wet gel, setting the drying temperature to be 40 ℃, setting the drying speed to be 5L/min, maintaining the constant pressure at 12MPa for 8h, closing air inlet, and releasing the pressure in the reaction kettle to obtain the precursor aerogel material. And taking out the precursor aerogel material, heating to 1000 ℃ at the heating rate of 1 ℃/min in a tubular furnace containing helium atmosphere, and preserving heat for 8 hours to obtain the SiC/C composite aerogel. FIG. 2 is the SiC/C composite aerogel prepared in example 2, which is a brown block. Under visible light irradiation for 2 hours, CH4The yield of (2) was 3.22. mu. mol/(g.h), and the yield of CO was 2.30. mu. mol/(g.h).
Example 3
1.488g of phloroglucinol, 5mL of propionaldehyde and 15mL of isopropanol were added to a beaker, stirred at 40 ℃ for 20min to form a uniformly mixed solution (the volume ratio of propionaldehyde, catechol and isopropanol was 5:1:15), followed by the addition of 3mL of methyltrimethoxysilane (the volume ratio of methyltrimethoxysilane to resorcinol was 3:1), stirred at 40 ℃ to gel and left to stand at room temperature for 30 h. To the sample was added ether and the modification was left to stand in an oven at 60 ℃ during which time it was washed 8 times with ether at 12h intervals. And after the solvent is replaced, performing carbon dioxide supercritical drying on the wet gel, setting the drying temperature to be 90 ℃, the drying rate to be 10L/min, maintaining the constant pressure to be 10MPa for 16h, closing air inlet, and releasing the pressure in the reaction kettle to obtain the precursor aerogel material. And taking out the precursor aerogel material, heating to 1600 ℃ at a heating rate of 3 ℃/min in a tubular furnace containing nitrogen atmosphere, and preserving heat for 2h to obtain the SiC/C composite aerogel. Under visible light irradiation for 2 hours, CH4The yield of (2) is 5.36 mu mol/(g.h), and the yield of CO is 3.26 mu mol/(g.h).
Example 4
1.27g of resorcinol, 3mL of benzaldehyde and 10mL of ethanol were added to a beaker and stirred at 25 ℃ for 40min to form a uniformly mixed solution (the volume ratio of benzaldehyde, resorcinol and ethanol was 3:1:10), followed by 2mL of dimethyldimethoxysilane (dimethyl dimethoxy silane)The mass volume ratio of the methyldimethoxysilane to the resorcinol is 2:1), stirring to gel at 30 ℃, and standing for 20h at room temperature. Isopropanol was added to the sample and the modification was left to stand in an oven at 40 ℃ during which time it was washed 7 times with isopropanol at 18h intervals. After the solvent replacement is finished, carrying out carbon dioxide supercritical drying on the wet gel, setting the drying temperature at 70 ℃, the drying rate at 8L/min, maintaining the constant pressure at 12MPa for 10h, closing air inlet, and releasing the pressure in the reaction kettle to obtain the resorcinol-SiO2An aerogel material. Removing resorcinol-SiO2And (3) heating the aerogel material to 1200 ℃ at the heating rate of 4 ℃/min in a tubular furnace containing argon atmosphere, and preserving heat for 6h to obtain the SiC/C composite aerogel. Under visible light irradiation for 2 hours, CH4The yield of (2) was 6.32. mu. mol/(g.h), and the yield of CO was 2.23. mu. mol/(g.h).
Example 5
1.34g catechol, 2mL acetaldehyde and 8mL ethanol were added to a beaker, stirred at 35 ℃ for 50min to form a well-mixed solution (acetaldehyde, catechol and ethanol in a volume ratio of 2:1:8), followed by addition of 1mL 3-aminopropyltriethoxysilane (3-aminopropyltriethoxysilane to catechol in a volume ratio of 1:1), stirred at 35 ℃ to gel and allowed to stand at room temperature for 30 h. Ethanol was added to the samples and the samples were modified by standing in an oven at 60 ℃ during which they were washed 6 times with ethanol at 8h intervals. After the solvent replacement is finished, carrying out carbon dioxide supercritical drying on the wet gel, setting the drying temperature to be 60 ℃, the drying speed to be 10L/min, maintaining the constant pressure to be 8MPa for 15h, closing air inlet, and releasing the pressure in the reaction kettle to obtain the catechol-SiO2An aerogel material. Removing catechol-SiO2And (3) heating the aerogel material to 1600 ℃ at the heating rate of 2 ℃/min in a tubular furnace containing nitrogen atmosphere, and preserving heat for 3h to obtain the SiC/C composite aerogel. Under visible light irradiation for 2 hours, CH4The yield of (2) is 5.26 mu mol/(g.h), and the yield of CO is 1.23 mu mol/(g.h).
Claims (9)
1. For CO2The preparation method of the SiC-C composite aerogel through photocatalytic reduction comprises the following specific steps:
(1) uniformly mixing phenol, aldehyde and an alcohol solvent, and uniformly stirring to obtain a polymer precursor A;
(2) adding organic siloxane into the polymer precursor A, uniformly stirring the mixture until the mixture is gelled, and standing the mixture;
(3) adding the gel obtained in the step (2) into an aging solution, aging in an oven, and then carrying out solvent replacement;
(4) performing carbon dioxide supercritical drying on the wet gel obtained in the step (3) to obtain an organic-inorganic hybrid precursor aerogel material;
(5) and (4) carrying out heat treatment on the organic-inorganic hybrid precursor aerogel material obtained in the step (4) in a tubular furnace containing protective atmosphere to finally obtain the SiC-C composite aerogel material.
2. The method according to claim 1, wherein the phenol in the step (1) is one or more of catechol, resorcinol, and phloroglucinol; the aldehyde is one or more of formaldehyde, acetaldehyde, propionaldehyde or benzaldehyde; the alcohol solvent is one or more of methanol, ethanol or isopropanol; the aldehyde, the phenol and the alcohol solvent are uniformly mixed according to the volume ratio of (1-5) to (1) - (5-15).
3. The method according to claim 1, wherein the stirring temperature in the step (1) is 20 to 40 ℃ and the stirring time is 20 to 60 min.
4. The method according to claim 1, wherein the organosiloxane in step (2) is a mixture of one or more of 3-aminopropyltriethoxysilane, methyltriethoxysilane, methyltrimethoxysilane, or dimethyldimethoxysilane; the organosiloxane and the phenol are mixed in a volume ratio of (0.5-3): 1.
5. The method according to claim 1, wherein the temperature of the uniform stirring in the step (2) is 20 to 40 ℃; the standing time is 15-30 h.
6. The method according to claim 1, wherein the aging solution in step (3) is a mixture of one or more of methanol, ethanol, diethyl ether or isopropanol.
7. The preparation method according to claim 1, wherein the temperature of the oven in the step (3) is 20-60 ℃; the solvent replacement times are 3-9 times, and the interval time of each time is 8-24 hours.
8. The method according to claim 1, wherein the supercritical carbon dioxide drying method in the step (4) is: carbon dioxide is used as a drying medium, the reaction temperature is 40-90 ℃, the pressure in the high-pressure reaction kettle is 8-12 MPa, the drying rate is 5-10L/min, and the drying time is 8-16 h.
9. The method according to claim 1, wherein the protective atmosphere in the step (5) is one or a mixture of argon, helium and nitrogen; the heat treatment temperature is 1000-1600 ℃, the heating rate is 1-5 ℃/min, and the heat treatment heat preservation time is 2-8 h.
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