CN111085277A - Silicon oxide and carbon composite material and synthesis method thereof - Google Patents
Silicon oxide and carbon composite material and synthesis method thereof Download PDFInfo
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- CN111085277A CN111085277A CN201811241355.4A CN201811241355A CN111085277A CN 111085277 A CN111085277 A CN 111085277A CN 201811241355 A CN201811241355 A CN 201811241355A CN 111085277 A CN111085277 A CN 111085277A
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 101
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 99
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 title claims abstract description 88
- 239000002131 composite material Substances 0.000 title claims abstract description 70
- 229910052814 silicon oxide Inorganic materials 0.000 title claims abstract description 60
- 238000001308 synthesis method Methods 0.000 title claims abstract description 16
- 238000003756 stirring Methods 0.000 claims abstract description 50
- 238000002156 mixing Methods 0.000 claims abstract description 36
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 33
- 238000005406 washing Methods 0.000 claims abstract description 28
- 239000007853 buffer solution Substances 0.000 claims abstract description 27
- 238000001035 drying Methods 0.000 claims abstract description 22
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims abstract description 21
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 21
- 239000010703 silicon Substances 0.000 claims abstract description 21
- 239000002904 solvent Substances 0.000 claims abstract description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 61
- 238000000034 method Methods 0.000 claims description 50
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 claims description 36
- 230000002194 synthesizing effect Effects 0.000 claims description 35
- 239000000243 solution Substances 0.000 claims description 34
- 239000010410 layer Substances 0.000 claims description 19
- 239000000463 material Substances 0.000 claims description 17
- 239000000377 silicon dioxide Substances 0.000 claims description 17
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims description 13
- 238000009210 therapy by ultrasound Methods 0.000 claims description 13
- 238000006243 chemical reaction Methods 0.000 claims description 11
- 239000002245 particle Substances 0.000 claims description 11
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 claims description 8
- 239000008103 glucose Substances 0.000 claims description 8
- 239000012752 auxiliary agent Substances 0.000 claims description 7
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 6
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 claims description 6
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 4
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 claims description 4
- 229930006000 Sucrose Natural products 0.000 claims description 4
- CZMRCDWAGMRECN-UGDNZRGBSA-N Sucrose Chemical compound O[C@H]1[C@H](O)[C@@H](CO)O[C@@]1(CO)O[C@@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 CZMRCDWAGMRECN-UGDNZRGBSA-N 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- ZXEKIIBDNHEJCQ-UHFFFAOYSA-N isobutanol Chemical compound CC(C)CO ZXEKIIBDNHEJCQ-UHFFFAOYSA-N 0.000 claims description 4
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 claims description 4
- FYKDNWHPKQOZOT-UHFFFAOYSA-M sodium;dihydrogen phosphate;2-hydroxypropane-1,2,3-tricarboxylic acid Chemical compound [Na+].OP(O)([O-])=O.OC(=O)CC(O)(C(O)=O)CC(O)=O FYKDNWHPKQOZOT-UHFFFAOYSA-M 0.000 claims description 4
- 239000005720 sucrose Substances 0.000 claims description 4
- 229920001214 Polysorbate 60 Polymers 0.000 claims description 3
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 claims description 3
- 239000012792 core layer Substances 0.000 claims description 3
- 235000010482 polyoxyethylene sorbitan monooleate Nutrition 0.000 claims description 3
- 229920000053 polysorbate 80 Polymers 0.000 claims description 3
- 239000001632 sodium acetate Substances 0.000 claims description 3
- 235000017281 sodium acetate Nutrition 0.000 claims description 3
- 229920001213 Polysorbate 20 Polymers 0.000 claims description 2
- 150000001298 alcohols Chemical class 0.000 claims description 2
- CDQSJQSWAWPGKG-UHFFFAOYSA-N butane-1,1-diol Chemical compound CCCC(O)O CDQSJQSWAWPGKG-UHFFFAOYSA-N 0.000 claims description 2
- 125000002791 glucosyl group Chemical group C1([C@H](O)[C@@H](O)[C@H](O)[C@H](O1)CO)* 0.000 claims description 2
- 239000012299 nitrogen atmosphere Substances 0.000 claims description 2
- 239000000256 polyoxyethylene sorbitan monolaurate Substances 0.000 claims description 2
- 235000010486 polyoxyethylene sorbitan monolaurate Nutrition 0.000 claims description 2
- QTYWBJZOZDYCGB-UHFFFAOYSA-L potassium;sodium;2-carboxybenzoate;hydroxide Chemical compound [OH-].[Na+].[K+].OC(=O)C1=CC=CC=C1C([O-])=O QTYWBJZOZDYCGB-UHFFFAOYSA-L 0.000 claims description 2
- LFQCEHFDDXELDD-UHFFFAOYSA-N tetramethyl orthosilicate Chemical compound CO[Si](OC)(OC)OC LFQCEHFDDXELDD-UHFFFAOYSA-N 0.000 claims description 2
- ZQZCOBSUOFHDEE-UHFFFAOYSA-N tetrapropyl silicate Chemical compound CCCO[Si](OCCC)(OCCC)OCCC ZQZCOBSUOFHDEE-UHFFFAOYSA-N 0.000 claims description 2
- 239000011258 core-shell material Substances 0.000 abstract description 20
- 239000012153 distilled water Substances 0.000 description 33
- 239000012265 solid product Substances 0.000 description 32
- 239000000203 mixture Substances 0.000 description 22
- 238000002360 preparation method Methods 0.000 description 17
- 239000011257 shell material Substances 0.000 description 17
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 16
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 12
- 239000003575 carbonaceous material Substances 0.000 description 9
- 239000002808 molecular sieve Substances 0.000 description 8
- 230000007935 neutral effect Effects 0.000 description 8
- 229910052757 nitrogen Inorganic materials 0.000 description 8
- 239000000047 product Substances 0.000 description 8
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 238000000926 separation method Methods 0.000 description 7
- 239000006174 pH buffer Substances 0.000 description 6
- 239000000872 buffer Substances 0.000 description 5
- 229910052681 coesite Inorganic materials 0.000 description 5
- 229910052906 cristobalite Inorganic materials 0.000 description 5
- 229910052682 stishovite Inorganic materials 0.000 description 5
- 229910052905 tridymite Inorganic materials 0.000 description 5
- 230000015572 biosynthetic process Effects 0.000 description 4
- 239000008367 deionised water Substances 0.000 description 4
- 229910021641 deionized water Inorganic materials 0.000 description 4
- 229910000403 monosodium phosphate Inorganic materials 0.000 description 4
- 235000019799 monosodium phosphate Nutrition 0.000 description 4
- AJPJDKMHJJGVTQ-UHFFFAOYSA-M sodium dihydrogen phosphate Chemical compound [Na+].OP(O)([O-])=O AJPJDKMHJJGVTQ-UHFFFAOYSA-M 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 238000003786 synthesis reaction Methods 0.000 description 4
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 3
- 230000007062 hydrolysis Effects 0.000 description 3
- 238000006460 hydrolysis reaction Methods 0.000 description 3
- 235000012239 silicon dioxide Nutrition 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- 108010029541 Laccase Proteins 0.000 description 2
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 239000003054 catalyst Substances 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 239000011246 composite particle Substances 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- GDVKFRBCXAPAQJ-UHFFFAOYSA-A dialuminum;hexamagnesium;carbonate;hexadecahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Al+3].[Al+3].[O-]C([O-])=O GDVKFRBCXAPAQJ-UHFFFAOYSA-A 0.000 description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- 229910001701 hydrotalcite Inorganic materials 0.000 description 2
- 229960001545 hydrotalcite Drugs 0.000 description 2
- 239000002608 ionic liquid Substances 0.000 description 2
- 239000004005 microsphere Substances 0.000 description 2
- 239000002086 nanomaterial Substances 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 238000003980 solgel method Methods 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- WDCYWAQPCXBPJA-UHFFFAOYSA-N 1,3-dinitrobenzene Chemical compound [O-][N+](=O)C1=CC=CC([N+]([O-])=O)=C1 WDCYWAQPCXBPJA-UHFFFAOYSA-N 0.000 description 1
- WZCQRUWWHSTZEM-UHFFFAOYSA-N 1,3-phenylenediamine Chemical compound NC1=CC=CC(N)=C1 WZCQRUWWHSTZEM-UHFFFAOYSA-N 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- 125000003184 C60 fullerene group Chemical group 0.000 description 1
- 102000002322 Egg Proteins Human genes 0.000 description 1
- 108010000912 Egg Proteins Proteins 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- 239000006087 Silane Coupling Agent Substances 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- NCZAACDHEJVCBX-UHFFFAOYSA-N [Si]=O.[C] Chemical compound [Si]=O.[C] NCZAACDHEJVCBX-UHFFFAOYSA-N 0.000 description 1
- 229960000583 acetic acid Drugs 0.000 description 1
- 239000003463 adsorbent Substances 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- 150000003863 ammonium salts Chemical class 0.000 description 1
- 229910052908 analcime Inorganic materials 0.000 description 1
- 229910001566 austenite Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000001588 bifunctional effect Effects 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 210000003278 egg shell Anatomy 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 238000007306 functionalization reaction Methods 0.000 description 1
- 239000012362 glacial acetic acid Substances 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 229910021389 graphene Inorganic materials 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 238000005216 hydrothermal crystallization Methods 0.000 description 1
- 238000001027 hydrothermal synthesis Methods 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000011147 inorganic material Substances 0.000 description 1
- VBMVTYDPPZVILR-UHFFFAOYSA-N iron(2+);oxygen(2-) Chemical group [O-2].[Fe+2] VBMVTYDPPZVILR-UHFFFAOYSA-N 0.000 description 1
- 229940018564 m-phenylenediamine Drugs 0.000 description 1
- 239000006249 magnetic particle Substances 0.000 description 1
- 239000000320 mechanical mixture Substances 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 239000002159 nanocrystal Substances 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
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- 230000035484 reaction time Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
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- 238000004729 solvothermal method Methods 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D15/00—Separating processes involving the treatment of liquids with solid sorbents; Apparatus therefor
- B01D15/08—Selective adsorption, e.g. chromatography
- B01D15/10—Selective adsorption, e.g. chromatography characterised by constructional or operational features
- B01D15/20—Selective adsorption, e.g. chromatography characterised by constructional or operational features relating to the conditioning of the sorbent material
-
- 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
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/103—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate comprising silica
-
- 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
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
-
- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/18—Carbon
-
- 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
- C01B32/05—Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/60—Particles characterised by their size
- C01P2004/61—Micrometer sized, i.e. from 1-100 micrometer
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/80—Particles consisting of a mixture of two or more inorganic phases
Abstract
The invention discloses a silicon oxide and carbon composite material and a synthesis method thereof. The synthesis method comprises the steps of mixing carbon and an alcohol solvent, adding a buffer solution and a silicon source, stirring, standing, washing, drying, and roasting to obtain the silicon oxide/carbon composite material. The silicon oxide/carbon composite material provided by the invention has a core-shell structure, the shell layer is stably coated and is not easy to fall off, and the synthesis method is simple and feasible.
Description
Technical Field
The invention belongs to the field of synthesis of porous inorganic materials, and particularly relates to a silicon oxide-containing composite material and a synthesis method thereof.
Background
The material with a core-shell structure is an important novel material, and is characterized in that a certain material is used as a core phase, and a layer of material of the same kind or different kinds grows on the outer surface of the core phase to form a shell layer, so that a composite structure similar to an eggshell form is formed. The core-shell material has a unique structure, so that the core-shell material has the advantages which are not possessed by a single-structure material, and has good application prospects in the fields of chemical industry, environmental protection and optics. But because of its unique and complex structure, the synthesis difficulty is far higher than that of common materials, mainly its structure is difficult to control, and its structure control and functionalization still need further research.
Since the discovery of C60, carbon nanotubes, and graphene, carbon nanostructured materials have received much attention due to their remarkable physical and chemical properties, such as high specific surface area, low density, high strength, and excellent thermal and chemical stability. Various types of functional carbon materials have been developed and widely used in the fields of adsorption, catalysis, electrochemistry, and the like. A series of hollow carbon spheres with adjustable particle sizes are prepared by hydrothermal synthesis of size-controllable hollow carbon spheres (rare metal materials and engineering, 2011, volume 40), and the preparation method has a good application prospect.
CN103007847A discloses a composite particle based on magnetic nano immobilized laccase and ionic liquid, a preparation method thereof and application thereof in removing pollutants in water. Firstly, magnetic gamma-Fe is prepared2O3A nanoparticle; then, the nano magnetic particles are used as a core phase, tetraethoxysilane and silane coupling agent are used as silicon sources, and a sol-gel method is utilized to prepare the nano core-shell type magnetic silicon dioxide with the surface amino functionalized; then, magnetic nano immobilized laccase and ionic liquid composite particles are prepared through a series of functional operations and can be applied to treatment for removing pollutants in water.
CN105036070A discloses a gold nanorod-silicon dioxide core-shell structure nanomaterial, a preparation method and application thereof, wherein the preparation method comprises the steps of preparing a chiral gold nanorod shoulder-side assembly body, and taking the assembly body as a core; and then coating the chiral gold nanorod side-by-side assembly body with a silicon dioxide shell layer in an alcohol-water system to prepare the functional material with the shell layer structure.
CN102160985A discloses a magnetic silica microsphere with core-shell structure and surface anisotropic dual-functional groups and a preparation method thereof, wherein the preparation method comprises the steps of firstly preparing superparamagnetic microspheres as iron oxide cores by a solvothermal method; then coating a layer of silicon dioxide on the iron oxide by using a sol-gel method to obtain a material with a core-shell structure; then, the material is functionalized, and finally the magnetic silica core-shell material with high magnetic responsiveness and surface bifunctional groups is obtained.
CN101885493A discloses a method for synthesizing a ZSM-5/β core-shell type molecular sieve, which comprises the steps of treating a core-phase ZSM-5 molecular sieve to enable the surface of the core-phase ZSM-5 molecular sieve to adsorb β nano crystals, then adding other raw materials, and carrying out hydrothermal crystallization reaction to obtain the ZSM-5/β core-shell type zeolite molecular sieve.
CN106475134A discloses a core-shell catalyst with hydrotalcite as shell/molecular sieve as core, its preparation and application, the preparation process is mixing hydrogen type molecular sieve with deionized water, ultrasonic processing to make A solution; mixing nitrate, ammonium salt and deionized water to prepare a solution B; then mixing the solution A and the solution B, and dropwise adding ammonia water to prepare a solution C; and then stirring the solution C at a high temperature to finally obtain the molecular sieve with the shape of the core-shell structure, wherein the molecular sieve is used as a core and the petal-shaped hydrotalcite is used as a shell. Can be used for the catalytic reaction of m-dinitrobenzene hydrogenation to synthesize m-phenylenediamine.
In summary, some core-shell structure materials and preparation methods thereof have been disclosed in the prior art, but the materials obtained by the currently disclosed preparation methods have some defects, and the preparation methods are relatively complex and have high cost.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a silicon oxide/carbon composite material and a synthesis method thereof. The silicon oxide/carbon composite material provided by the invention has a core-shell structure, the shell layer is stably coated and is not easy to fall off, and the synthesis method is simple and feasible.
In a first aspect, the invention provides a silica/carbon composite material comprising carbonThe silicon oxide is taken as a core layer and a shell layer, wherein the diameter of the core layer is 1-5 mu m; the thickness of the shell layer is 10-200 nm; the specific surface area is 500-900 m2/g。
The second aspect of the present invention provides a method for synthesizing a silicon oxide/carbon composite material, which comprises the following steps:
(1) mixing carbon and a micromolecular alcohol solvent, and adding a pH buffer solution after uniformly mixing;
(2) adding a silicon source into the material obtained in the step (1) under the condition of stirring, uniformly mixing, and then standing;
(3) and (3) washing, drying and thermally treating the material obtained in the step (2) to obtain the silicon oxide/carbon composite material.
In the synthesis method of the silicon oxide/carbon composite material, the carbon is common carbon, and the particle size range of the carbon is 1-5 mu m; the carbon is subjected to a purification treatment prior to use to remove the adsorbed impurities from the zeolite, using purification means known in the art, such as washing with water or a solvent, the selection of which is well known to those skilled in the art.
In the method for synthesizing the silicon oxide/carbon composite material, the carbon is preferably prepared by the following method: firstly, mixing a carbon source, formaldehyde and water, uniformly mixing, then sending into a reaction kettle for treatment, and then separating, washing, drying and roasting to obtain carbon.
In the above method, the carbon source is glucose and/or sucrose.
In the method, the mass ratio of the carbon source to the formaldehyde to the water is 1: 0.2-1.5: 8-50, preferably 1: 0.3-1.3: 10 to 40.
In the method, the treatment temperature is 100-180 ℃, and preferably 110-170 ℃; the treatment time is 4-20 h, preferably 5-18 h.
In the above-described process, the separation and washing are conventional procedures well known to those skilled in the art. If the separation is carried out by filtration, washing is generally referred to as washing with deionized water. Usually comprises a plurality of separation and washing operations, generally 1 to 6 times. The drying condition is generally drying for 5-15 h at 100-140 ℃.
In the method, the roasting is carried out in a nitrogen atmosphere, and the roasting temperature is 700-1100 ℃, preferably 800-1000 ℃; the roasting time is 3-9 h, preferably 4-8 h.
In the method for synthesizing the silicon oxide/carbon composite material, the micromolecular alcohol solvent in the step (1) is C2-C4 alcohol, and specifically can be one or more of ethanol, propanol, isopropanol, n-butanol, isobutanol, ethylene glycol, propylene glycol and butanediol.
In the synthesis method of the silicon oxide/carbon composite material, the mass ratio of the micromolecular alcohol solvent to carbon in the step (1) is 5-40: 1, preferably 10 to 30: 1.
in the synthesis method of the silicon oxide/carbon composite material, the mixing treatment in the step (1) can adopt any means capable of realizing full mixing, such as one or more of stirring and ultrasonic treatment, preferably adopts a stirring and ultrasonic treatment combined mode, more preferably adopts a method of firstly stirring and then mixing in ultrasonic, the frequency of the ultrasonic is 15KHz-10MHz, and the power is 20-100W/L according to the volume of the solution. The stirring time is 0.1-2 h, preferably 0.2-1.8 h; the ultrasonic time is 1-6 h, preferably 2-5 h.
In the method for synthesizing the silicon oxide/carbon composite material, the pH value of the pH buffer solution in the step (1) is 4-6, and preferably 4.5-5.8. The pH buffer may be one or more of sodium dihydrogen phosphate-citric acid pH buffer, sodium acetate pH buffer, potassium hydrogen phthalate-sodium hydroxide pH buffer, preferably sodium dihydrogen phosphate-citric acid pH buffer. The method of formulating the pH buffer is well known to those skilled in the art and can be carried out by methods known in the art.
In the synthesis method of the silicon oxide/carbon composite material, the mass ratio of the pH buffer solution to carbon in the step (1) is 8-40: 1, preferably 11 to 31: 1.
in the method for synthesizing the silicon oxide/carbon composite material, an auxiliary agent can be added in the step (1), wherein the auxiliary agent comprises one or more of tween-20, tween-60 and tween-80; the mass ratio of the auxiliary agent to the micromolecular alcohols is 1: 5-40, preferably 1: 10 to 30.
In the method for synthesizing the silicon oxide/carbon composite material, the silicon source in the step (2) is one or more of methyl orthosilicate, ethyl orthosilicate and propyl orthosilicate, and preferably ethyl orthosilicate.
In the synthetic method, the mass ratio of the silicon source in the step (2) to the carbon in the step (1) is 0.2-1.5: 1, preferably 0.25 to 1.35: 1.
in the method for synthesizing the silicon oxide/carbon composite material, the silicon source is added in the step (2) under the condition of 45-80 ℃, preferably 50-70 ℃.
In the method for synthesizing the silicon oxide/carbon composite material, the silicon source is added under the stirring condition in the step (2), the stirring speed is 100-300 r/min, preferably 120-280 r/min, the stirring is continued for a period of time after the silicon source is dripped, and the stirring speed is 10-60 r/min, preferably 20-50 r/min; the stirring time is 1-10 h, preferably 2-9 h.
In the method for synthesizing the silicon oxide/carbon composite material, the standing condition in the step (2) is as follows: the temperature is 25-40 ℃, and preferably 25-35 ℃; the time is 5-24 h, preferably 6-20 h.
In the method for synthesizing the silica/carbon composite material according to the present invention, the separation and washing in step (3) are conventional procedures well known to those skilled in the art. If the separation is carried out by filtration, washing is generally referred to as washing with deionized water. Usually, the method comprises more than one separation and washing operation, and the number of the separation and washing operations is generally 1-6. The drying condition is generally drying for 5-15 h at 100-140 ℃.
In the synthesis method of the silicon oxide/carbon composite material, the heat treatment temperature in the step (3) is 180-300 ℃, and preferably 200-280 ℃; the heat treatment time is 1-6 h, preferably 2-5 h.
The silicon oxide-carbon composite material provided by the invention can be used as a catalyst carrier, an adsorbent and a chromatographic column filler, and can also be used as a synthetic template of an inorganic organic material.
Compared with the prior art, the silicon oxide/carbon composite material and the synthesis method thereof provided by the invention have the following advantages:
(1) the silicon oxide/carbon composite material provided by the invention is a composite material with a core-shell structure, and the shell layer of the composite material is stably coated and is not easy to fall off.
(2) According to the method for synthesizing the silicon oxide/carbon composite material, the pH buffer solution is used for providing protons for the hydrolysis of the silicon source, the concentration of the protons in a synthesis system can be kept unchanged by adding the pH buffer solution, the hydrolysis speed of the organic silicon source can be kept constant, the particle size of the silicon oxide particles is kept consistent at all reaction time points, and further, the shell layer of the core-shell structure formed by uniformly covering the silicon oxide particles with uniform particle sizes on the outer surface of the carbon is dense and ordered, so that the generated core-shell structure composite material is not easy to damage. The problems that in the prior art, the size of the obtained silicon oxide particles is not uniform, so that the accumulated silicon oxide shell layer is loose and easy to damage, and the finally formed core-shell structure composite material is unstable in structure are solved.
(3) In the method for synthesizing the silicon oxide/carbon composite material, the operation of adding the silicon source in the step (2) is particularly important for controlling the stirring condition, the stirring process needs to be carried out in a limited mode, the stirring speed is controlled to ensure the hydrolysis speed of the organic silicon source, and the phenomenon that the organic silicon source is hydrolyzed too fast due to too fast stirring to generate large-particle silicon oxide particles which cannot be adsorbed by the outer surface of carbon and are not beneficial to generating a shell structure and are easy to generate a mechanical mixture of the carbon and the large-particle silicon oxide is avoided.
(4) In the synthesis method of the silicon oxide/carbon composite material, the auxiliary agent is added and used in combination with other means such as pH buffer solution and a silicon source adding control mode, so that a shell layer is formed, the shell layer distribution is more uniform, mesoporous channels can be formed in the silicon oxide shell layer, and the transmission of substances can be accelerated.
Drawings
FIG. 1 is a TEM photograph of a synthesized sample of example 2.
FIG. 2 is a TEM photograph of a synthesized sample of comparative example 1.
Detailed Description
The synthesis of the analcime of the present invention is described in detail below by way of specific examples, but is not limited thereto.
The structural characteristics and the sizes of the composite materials in the embodiments and the comparative examples are characterized and tested by a transmission electron microscope, and the surface area is characterized and tested by a physical adsorption instrument.
Example 1: preparation of buffers of different pH
preparation of buffer solution at pH 4.5: 18g of sodium acetate and 9.8mL of glacial acetic acid are taken and diluted by adding distilled water until the total volume is 1000 mL.
preparation of pH4.8 buffer: mixing 19.96g of sodium dihydrogen phosphate with 99.8mL of distilled water to form solution A; mixing 10.14g of citric acid with 101.4mL of distilled water to form solution B; and mixing the solution A and the solution B to obtain a buffer solution.
preparation of pH5.0 buffer: mixing 20.6g of sodium dihydrogen phosphate with 103mL of distilled water to form solution A; mixing 9.7g of citric acid with 97mL of distilled water to form solution B; and mixing the solution A and the solution B to obtain a buffer solution.
preparation of pH5.2 buffer: 21.44g of sodium dihydrogen phosphate is mixed with 107.2mL of distilled water to form solution A; mixing 9.28g of citric acid with 92.8mL of distilled water to form solution B; and mixing the solution A and the solution B to obtain a buffer solution.
preparation of pH5.6 buffer: mixing 23.2g of sodium dihydrogen phosphate with 116mL of distilled water to form solution A; mixing 8.4g of citric acid with 84mL of distilled water to form solution B; and mixing the solution A and the solution B to obtain a buffer solution.
Example 2
Mixing 10g of glucose, 8g of formaldehyde and 200mL of distilled water, and stirring for 1 h; then the mixture is put into a reaction kettle for treatment for 12 hours at 180 ℃; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 5 hours at 900 ℃ in nitrogen to obtain a carbon material;
2.1g of the carbon was put in 45mL of ethanol and stirred for 0.5h, followed by ultrasonic treatment3h, the frequency of the ultrasonic wave is 1MHz, and the power is 50W/L according to the volume of the solution; then placing the mixture into a water bath at 63 ℃, adding 53.5mL of buffer solution with pH4.8, dropwise adding 1 mL of ethyl orthosilicate under the stirring condition of 120 r/min, stirring the mixture for 5 hours at the speed of 20 r/min after the dropwise adding is finished, and then placing the mixture into a water bath at 30 ℃ for standing for 12 hours; washing the obtained product with distilled water for 4 times to neutrality, drying at 120 deg.C for 12h, and heat treating at 260 deg.C for 3h to obtain SiO2The obtained sample number CL1 of the/carbon composite material is shown in Table 1, and the TEM image of the sample CL1 is shown in FIG. 1. As can be seen from fig. 1, the obtained sample has a core-shell structure.
Example 3
Mixing 10g of glucose, 2.4g of formaldehyde and 400mL of distilled water, and stirring for 0.2 h; then the mixture is put into a reaction kettle for treatment for 4 hours at 200 ℃; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 4 hours at 1000 ℃ in nitrogen to obtain a carbon material;
2g of the carbon is taken and placed in 20mL of ethanol to be stirred for 0.2h, and then ultrasonic treatment is carried out for 2h, the frequency of ultrasonic waves is 15KHz, and the power is 100W/L according to the volume of the solution; then placing the mixture into a water bath at 70 ℃, adding 22mL of buffer solution with pH of 5.0, and dropwise adding 0.4 mL of tetraethoxysilane under the stirring condition of 280 revolutions per minute; stirring at the speed of 50 r/min for 2h after the dropwise addition is finished, and standing in a water bath at the temperature of 25 ℃ for 6 h; washing the obtained product with distilled water for 4 times to neutrality, drying at 120 deg.C for 12h, and treating at 280 deg.C for 2h to obtain SiO2The/carbon composite material obtained is sample No. CL2, the properties of the samples are shown in Table 1.
Example 4
Mixing 10g of glucose, 10.4g of formaldehyde and 100mL of distilled water, and stirring for 1.8 h; then the mixture is put into a reaction kettle for treatment for 20 hours at 160 ℃; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 8 hours at 800 ℃ in nitrogen to obtain a carbon material;
2g of the carbon is taken and placed in 60mL of propanol to be stirred for 1.8h, and then ultrasonic treatment is carried out for 5h, wherein the frequency of ultrasonic waves is 10MHz, and the power is 20W/L according to the volume of the solution; then placing the mixture into a water bath at 50 ℃, adding 62mL of buffer solution with pH5.2, and dropwise adding 2.7 mL of tetraethoxysilane under the stirring condition of 120 revolutions per minute; stirring at 20 r/min after the dropwise addition is finished 9Standing in a water bath at 35 ℃ for 20 h; washing the obtained product with distilled water for 4 times to neutrality, drying at 120 deg.C for 12h, and treating at 220 deg.C for 3h to obtain SiO2The resulting sample number is CL 3, and the sample properties are shown in Table 1.
Example 5
Mixing 11g of sucrose, 8g of formaldehyde and 170mL of distilled water, and stirring for 1 h; is connected to a 185 ℃ place in a reaction kettle for 12 hours; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 5 hours at 950 ℃ in nitrogen to obtain a carbon material;
then putting 1.5g of carbon into 35 mL of propanol, adding 2g of Tween-60, stirring for 0.5h, and then carrying out ultrasonic treatment for 3h, wherein the frequency of ultrasonic waves is 1MHz, and the power is 50W/L according to the volume of the solution; then placing the mixture into a water bath at 55 ℃, adding 50mL of buffer solution with pH5.6, and then dropwise adding 1 mL of tetraethoxysilane while stirring at the speed of 240 revolutions per minute; then stirring the mixture for 5 hours at the speed of 30 r/min, and standing the mixture in a water bath at the temperature of 35 ℃ for 12 hours; washing the obtained product with distilled water for 4 times to neutrality, drying at 120 deg.C for 12h, and treating at 270 deg.C for 4h to obtain SiO2The resulting carbon composite material was designated as sample No. CL 4.
Example 6
Mixing 7g of sucrose, 8g of formaldehyde and 150mL of distilled water, and stirring for 1 h; is connected to a 180 ℃ position in a reaction kettle for 12 hours; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 5 hours at 900 ℃ in nitrogen to obtain a carbon material;
then putting 1.7g of carbon into 29mL of ethanol, adding 2g of Tween-80, stirring for 1h, and then carrying out ultrasonic treatment for 2h, wherein the frequency of ultrasonic waves is 1MHz, and the power is 50W/L according to the volume of the solution; then placing the mixture into a water bath at 60 ℃, adding 50mL of buffer solution with pH4.5, and then dropwise adding 0.75 mL of tetraethoxysilane while stirring at the speed of 265 r/min; then stirring the mixture for 5 hours at the speed of 30 r/min, and standing the mixture in a water bath at the temperature of 30 ℃ for 12 hours; washing the obtained product with distilled water for 4 times to neutrality, drying at 120 deg.C for 12h, and treating at 230 deg.C for 2.5h to obtain SiO2A/carbon composite material, sample No. CL 5.
Comparative example 1
Mixing 10g of glucose, 8g of formaldehyde and 200mL of distilled water, and stirring for 1 h; is connected to a 180 ℃ position in a reaction kettle for 12 hours; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 5 hours at 900 ℃ in nitrogen to obtain a carbon material;
2.1g of the carbon is taken and placed in 45mL of ethanol to be stirred for 0.5h, and then ultrasonic treatment is carried out for 3h, wherein the frequency of ultrasonic waves is 1MHz, and the power is 50W/L according to the volume of the solution; then placing the mixture in a water bath at 63 ℃, adding 53.5mL of hydrochloric acid solution with the pH value of 4.8, dropwise adding 1 mL of ethyl orthosilicate under the stirring condition of 120 r/min, stirring the mixture for 5 hours at the speed of 20 r/min after the dropwise adding is finished, and then placing the mixture in a water bath at 30 ℃ for standing for 12 hours; the obtained product was washed 4 times with distilled water to neutrality, dried at 120 ℃ for 12 hours, heat-treated at 260 ℃ for 3 hours, and obtained sample No. CL 6.
Comparative example 2
Referring to the material ratio of example 2, 10g of glucose, 8g of formaldehyde and 200mL of distilled water are mixed and stirred for 1 h; is connected to a 180 ℃ position in a reaction kettle for 12 hours; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 5 hours at 900 ℃ in nitrogen to obtain a carbon material;
2.1g of the carbon is taken and placed in 45mL of ethanol to be stirred for 0.5h, and then ultrasonic treatment is carried out for 3h, wherein the frequency of ultrasonic waves is 1MHz, and the power is 50W/L according to the volume of the solution; then placing the mixture into a water bath at 63 ℃, adding 53.5mL of buffer solution with pH4.8, dropwise adding 1 mL of ethyl orthosilicate under the stirring condition of 120 r/min, stirring the mixture for 5 hours at the speed of 350 r/min after the dropwise adding is finished, and then placing the mixture into a water bath at 30 ℃ for standing for 12 hours; the obtained product was washed 4 times with distilled water to neutrality, dried at 120 ℃ for 12 hours, heat-treated at 260 ℃ for 3 hours, and obtained sample No. CL 7.
Comparative example 3
Referring to the material ratio of example 2, 10g of glucose, 8g of formaldehyde and 200mL of distilled water are mixed and stirred for 1 h; is connected to a 180 ℃ position in a reaction kettle for 12 hours; then washing the solid product with distilled water for 4 times until the solid product is neutral, drying the solid product for 12 hours at 120 ℃, and then treating the solid product for 5 hours at 900 ℃ in nitrogen to obtain a carbon material;
2.1g of the carbon is taken and placed in 45mL of ethanol to be stirred for 0.5h, and then ultrasonic treatment is carried out for 3h, wherein the frequency of ultrasonic waves is 1MHz, and the power is 50W/L according to the volume of the solution; then placing the mixture into a water bath at 63 ℃, adding 53.5mL of buffer solution with pH4.8, dropwise adding 1 mL of ethyl orthosilicate under the stirring condition of 120 r/min, stirring for 5h at the speed of 4 r/min after dropwise adding, and then placing the mixture into a water bath at 30 ℃ for standing for 12 h; the obtained product was washed 4 times with distilled water to neutrality, dried at 120 ℃ for 12 hours, heat-treated at 260 ℃ for 3 hours, and obtained sample No. CL 8.
Stability evaluation test:
in order to further verify the stability of the structure of the samples obtained in the above examples and comparative examples, the samples were subjected to ultrasonic treatment for 24 hours, the frequency of the ultrasonic wave was 10MHz, and the power was 100W/L based on the volume of the solution. Through tests, the shell layer of the sample obtained in the example 2-6 is not dropped after ultrasonic treatment, which shows that the sample prepared by the invention has very stable structure, the shell layer is combined with the core very tightly, and the sample is not easy to be damaged by external force.
TABLE 1 physicochemical Properties of samples obtained in examples and comparative examples
Claims (26)
1. A silicon oxide/carbon composite material takes carbon as a core layer and silicon oxide as a shell layer.
2. The silica/carbon composite of claim 1 wherein: in the composite material, the diameter of a nuclear layer is 1-5 mu m; the thickness of the shell layer is 10-200 nm.
3. The silica/carbon composite of claim 1 wherein: the specific surface area of the composite material is 500-900 m2/g。
4. A synthesis method of a silicon oxide/carbon composite material comprises the following steps:
(1) mixing carbon and a micromolecular alcohol solvent, and adding a pH buffer solution after uniformly mixing;
(2) adding a silicon source into the material obtained in the step (1) under the condition of stirring, uniformly mixing, and then standing;
(3) and (3) washing, drying and thermally treating the material obtained in the step (2) to obtain the silicon oxide/carbon composite material.
5. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the particle size range of the carbon is 1-5 mu m.
6. The method for synthesizing a silicon oxide/carbon composite material according to claim 5, wherein: the carbon is prepared by the following method: mixing a carbon source, formaldehyde and water, uniformly mixing, sending into a reaction kettle for treatment, and then separating, washing, drying and roasting to obtain carbon.
7. The method for synthesizing a silicon oxide/carbon composite material according to claim 6, wherein: the carbon source is glucose or sucrose.
8. The method for synthesizing a silicon oxide/carbon composite material according to claim 6, wherein: the mass ratio of the carbon source to the formaldehyde to the water is 1: 0.2-1.5: 8-50, preferably 1: 0.3-1.3: 10 to 40.
9. The method for synthesizing a silicon oxide/carbon composite material according to claim 6, wherein: the treatment temperature is 100-180 ℃, and preferably 110-170 ℃; the treatment time is 4-20 h, preferably 5-18 h.
10. The method for synthesizing a silicon oxide/carbon composite material according to claim 6, wherein: the roasting is carried out in a nitrogen atmosphere, the roasting temperature is 700-1100 ℃, and 800-1000 ℃ is preferred; the roasting time is 3-9 h, preferably 4-8 h.
11. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the small molecular alcohol solvent in the step (1) is C2-C4 alcohol.
12. A method for synthesizing a silicon oxide/carbon composite material according to claim 4 or 11, wherein: the micromolecular alcohol solvent in the step (1) is one or more of ethanol, propanol, isopropanol, n-butanol, isobutanol, ethylene glycol, propylene glycol and butanediol.
13. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: in the step (1), the mass ratio of the micromolecular alcohol solvent to carbon is 5-40: 1, preferably 10 to 30: 1.
14. the method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the mixing treatment in the step (1) adopts one or more of stirring and ultrasonic treatment, preferably adopts a combined mode of stirring and ultrasonic treatment, and more preferably adopts a method of firstly stirring and then ultrasonically mixing.
15. A method of synthesizing a silica/carbon composite material as defined in claim 14 wherein: the frequency of the ultrasonic wave is 15KHz-10MHz, the power is 20-100W/L according to the volume of the solution, and the stirring time is 0.1-2 h, preferably 0.2-1.8 h; the ultrasonic time is 1-6 h, preferably 2-5 h.
16. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the pH value of the pH buffer solution in the step (1) is 4-6, and preferably 4.5-5.8.
17. A method for synthesizing a silicon oxide/carbon composite material according to claim 4 or 16, wherein: the pH buffer solution in the step (1) is one or more of sodium dihydrogen phosphate-citric acid pH buffer solution, sodium acetate pH buffer solution and potassium hydrogen phthalate-sodium hydroxide pH buffer solution, and is preferably sodium dihydrogen phosphate-citric acid pH buffer solution.
18. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the mass ratio of the pH buffer solution to the carbon in the step (1) is 8-40: 1, preferably 11 to 31: 1.
19. the method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: and (2) adding an auxiliary agent in the step (1), wherein the auxiliary agent comprises one or more of tween-20, tween-60 and tween-80.
20. A method of synthesizing a silica/carbon composite material as defined in claim 19 wherein: the mass ratio of the auxiliary agent to the micromolecular alcohols is 1: 5-40, preferably 1: 10 to 30.
21. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the silicon source in the step (2) is one or more of methyl orthosilicate, ethyl orthosilicate and propyl orthosilicate, and preferably ethyl orthosilicate.
22. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the mass ratio of the silicon source in the step (2) to the carbon in the step (1) is 0.2-1.5: 1, preferably 0.25 to 1.35: 1.
23. the method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the condition for adding the silicon source in the step (2) is that the silicon source is added at the temperature of 45-80 ℃, preferably 50-70 ℃.
24. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: adding a silicon source under the stirring condition in the step (2), wherein the stirring speed is 100-300 r/min, preferably 120-280 r/min, and stirring is continued for a period of time after the silicon source is dropwise added, wherein the stirring speed is 10-60 r/min, preferably 20-50 r/min; the stirring time is 1-10 h, preferably 2-9 h.
25. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the standing condition in the step (2) is as follows: the temperature is 25-40 ℃, and preferably 25-35 ℃; the time is 5-24 h, preferably 6-20 h.
26. The method for synthesizing a silicon oxide/carbon composite material according to claim 4, wherein: the heat treatment temperature in the step (3) is 180-300 ℃, and preferably 200-280 ℃; the heat treatment time is 1-6 h, preferably 2-5 h.
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