CN112624166B - Preparation method of silicon-aluminum-based aerogel and application of prepared silicon-aluminum-based aerogel in heavy metal gas adsorption - Google Patents
Preparation method of silicon-aluminum-based aerogel and application of prepared silicon-aluminum-based aerogel in heavy metal gas adsorption Download PDFInfo
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- 239000004964 aerogel Substances 0.000 title claims abstract description 89
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 title claims abstract description 73
- 238000002360 preparation method Methods 0.000 title abstract description 16
- 238000001179 sorption measurement Methods 0.000 title description 51
- 229910001385 heavy metal Inorganic materials 0.000 title description 34
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 72
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 50
- 238000003756 stirring Methods 0.000 claims abstract description 42
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 32
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 claims abstract description 30
- 239000000463 material Substances 0.000 claims abstract description 27
- 238000002156 mixing Methods 0.000 claims abstract description 25
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 claims abstract description 25
- 239000000243 solution Substances 0.000 claims abstract description 23
- 238000010438 heat treatment Methods 0.000 claims abstract description 20
- 239000002243 precursor Substances 0.000 claims abstract description 19
- 239000011259 mixed solution Substances 0.000 claims abstract description 18
- SMZOGRDCAXLAAR-UHFFFAOYSA-N aluminium isopropoxide Chemical compound [Al+3].CC(C)[O-].CC(C)[O-].CC(C)[O-] SMZOGRDCAXLAAR-UHFFFAOYSA-N 0.000 claims abstract description 15
- 239000002904 solvent Substances 0.000 claims abstract description 15
- 239000011240 wet gel Substances 0.000 claims abstract description 15
- 238000001035 drying Methods 0.000 claims abstract description 14
- 239000007788 liquid Substances 0.000 claims abstract description 10
- 238000001816 cooling Methods 0.000 claims abstract description 9
- 230000007935 neutral effect Effects 0.000 claims abstract description 9
- 238000010992 reflux Methods 0.000 claims abstract description 9
- 238000001291 vacuum drying Methods 0.000 claims abstract description 9
- 230000002378 acidificating effect Effects 0.000 claims abstract description 6
- 230000001105 regulatory effect Effects 0.000 claims abstract description 6
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims abstract description 4
- 238000000034 method Methods 0.000 claims description 20
- 238000000197 pyrolysis Methods 0.000 claims description 12
- 229910052782 aluminium Inorganic materials 0.000 claims description 3
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims 1
- 239000010703 silicon Substances 0.000 claims 1
- 239000007789 gas Substances 0.000 description 26
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 24
- 238000002474 experimental method Methods 0.000 description 12
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 10
- 239000004965 Silica aerogel Substances 0.000 description 8
- 239000011148 porous material Substances 0.000 description 8
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 6
- 244000282866 Euchlaena mexicana Species 0.000 description 6
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 6
- 239000003463 adsorbent Substances 0.000 description 6
- 235000011114 ammonium hydroxide Nutrition 0.000 description 6
- 239000003814 drug Substances 0.000 description 6
- 239000010419 fine particle Substances 0.000 description 6
- 238000000227 grinding Methods 0.000 description 6
- 239000004570 mortar (masonry) Substances 0.000 description 6
- 238000012216 screening Methods 0.000 description 6
- 238000010517 secondary reaction Methods 0.000 description 6
- 230000032683 aging Effects 0.000 description 5
- 150000001805 chlorine compounds Chemical class 0.000 description 4
- 239000002910 solid waste Substances 0.000 description 4
- 229910003439 heavy metal oxide Inorganic materials 0.000 description 3
- 229910004298 SiO 2 Inorganic materials 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 230000003247 decreasing effect Effects 0.000 description 2
- 238000001095 inductively coupled plasma mass spectrometry Methods 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 239000005995 Aluminium silicate Substances 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 241000282414 Homo sapiens Species 0.000 description 1
- 235000019738 Limestone Nutrition 0.000 description 1
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 1
- 235000012211 aluminium silicate Nutrition 0.000 description 1
- 229960000892 attapulgite Drugs 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000012295 chemical reaction liquid Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 230000029087 digestion Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 239000000411 inducer Substances 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 1
- 239000006028 limestone Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 229910052625 palygorskite Inorganic materials 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
- C01F7/00—Compounds of aluminium
- C01F7/02—Aluminium oxide; Aluminium hydroxide; Aluminates
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
-
- 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
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
- B01J20/08—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04 comprising aluminium oxide or hydroxide; comprising bauxite
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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
- 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
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28014—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their form
- B01J20/28047—Gels
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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
- C01B33/00—Silicon; Compounds thereof
- C01B33/113—Silicon oxides; Hydrates thereof
- C01B33/12—Silica; Hydrates thereof, e.g. lepidoic silicic acid
- C01B33/14—Colloidal silica, e.g. dispersions, gels, sols
- C01B33/157—After-treatment of gels
- C01B33/158—Purification; Drying; Dehydrating
- C01B33/1585—Dehydration into aerogels
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/60—Heavy metals or heavy metal compounds
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- 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
- C01P2004/82—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases
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- C01P2006/12—Surface area
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- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
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- C01P2006/14—Pore volume
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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
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Abstract
The invention discloses a preparation method of silicon-aluminum-based aerogel, which comprises the following steps: (1) Adding aluminum isopropoxide into a mixed solution of ethanol and water to obtain a mixed material, heating and refluxing the mixed material under stirring, stopping stirring, continuing heating, cooling to room temperature after heating, and regulating the pH value of the solution to enable the solution to be acidic to obtain alumina wet sol; (2) Adding ethyl orthosilicate into a mixed solution of ethanol and water, stirring, and then adjusting the pH value of the solution to enable the solution to be acidic to obtain a silica sol precursor solution; (3) Mixing the alumina wet sol in the step (1) with the silica sol precursor liquid in the step (2), stirring, regulating the pH value of the mixed liquid to be neutral, standing the mixed liquid for at least 12 hours to form silicon-aluminum wet gel, carrying out solvent exchange on the silicon-aluminum wet gel by using n-hexane, and then placing the silicon-aluminum wet gel into a vacuum drying oven for drying to obtain the silicon-aluminum-based aerogel.
Description
Technical Field
The invention relates to a preparation method of silicon-aluminum-based aerogel and also relates to application of the silicon-aluminum-based aerogel prepared by the preparation method in the aspect of heavy metal gas adsorption.
Background
Solid waste generated in the production and life of human beings seriously pollutes water and soil in nature. Pyrolysis technology is generally adopted to make solid waste harmless. However, in the solid waste pyrolysis process, particularly when the solid waste containing chlorine element is pyrolyzed, volatile and semi-volatile heavy metals can be easily volatilized into the external environment in the form of chloride, so that secondary pollution of the environment is caused. Therefore, a material capable of efficiently adsorbing heavy metal gas needs to be found. At present, materials for adsorbing the heavy metal gases are mainly natural raw materials rich in Si and Al elements, such as kaolin, attapulgite, limestone and the like. However, these materials often occur on the surface of the adsorbent when adsorbing and solidifying heavy metal gas, and cannot penetrate into the adsorbent, resulting in low utilization rate of the adsorbent.
In recent years, silica aerogel has been increasingly valued due to its unique pore structure. The silica aerogel has larger specific surface area and porosity, can adsorb and contain more particles, and is favorable for being applied to the adsorption of heavy metal gas in the pyrolysis process. However, the silica aerogel is poor in thermal stability, and the pore canal is easy to collapse at high temperature, so that the structure is densified, and the silica aerogel cannot be applied to heavy metal gas adsorption in the actual pyrolysis process.
Disclosure of Invention
The invention aims to: aiming at the problem that the silica aerogel in the prior art cannot adsorb heavy metal gas in the pyrolysis process, the invention provides the preparation method of the silica-alumina-based aerogel, and the silica-alumina-based aerogel obtained by the preparation method has high thermal stability on the basis of large specific surface area and porosity, so that the silica-alumina-based aerogel can be applied to heavy metal gas adsorption in the pyrolysis process.
The technical scheme is as follows: the preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) Adding aluminum isopropoxide into a mixed solution of ethanol and water to obtain a mixed material, heating and refluxing the mixed material under stirring, stopping stirring, continuing heating, cooling to room temperature after heating, and regulating the pH value of the solution to be acidic to obtain alumina wet sol;
(2) Adding ethyl orthosilicate into a mixed solution of ethanol and water, stirring for not more than 0.5h, and then adjusting the pH value of the solution to be acidic to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor liquid in the step (2), stirring, regulating the pH value of the mixed liquid to be neutral, standing the mixed liquid for at least 12 hours to form silicon-aluminum mixed wet gel, carrying out solvent exchange on the silicon-aluminum mixed wet gel by using n-hexane, and drying the silicon-aluminum mixed wet gel in a vacuum drying oven to obtain the silicon-aluminum-based aerogel.
Wherein, in the step (1), the mixing volume ratio of the ethanol to the water is 15-30:5-10.
Wherein, in the step (2), the mixing mole ratio of the ethanol and the water is 5-7:1-3.
Wherein in the step (3), the drying temperature is 50-60 ℃ and the drying time is 6-10 h.
Wherein in the step (3), the molar ratio of the silicon aluminum elements in the obtained silicon aluminum-based aerogel is 1:1.
The silicon-aluminum-based aerogel prepared by the preparation method of the silicon-aluminum-based aerogel is applied to the aspect of heavy metal gas adsorption.
Wherein the silicon-aluminum-based aerogel is used for adsorbing heavy metal gas in the pyrolysis process, and the temperature of the pyrolysis process is 600-900 ℃.
The silicon-aluminum-based aerogel prepared by the method has large specific surface area and porosity, so that heavy metal gas can enter the pore canal of the aerogel material, the utilization rate of the material is improved, and meanwhile, the silicon-aluminum-based aerogel can well solidify heavy metal, so that the heavy metal adsorption efficiency is improved; the silicon-aluminum-based aerogel contains rich Si elements and can form silicate with heavy metal oxides; meanwhile, aiming at heavy metal chlorides, aluminum oxide in the silica-alumina-based aerogel can react with the chlorides in the heavy metal gas to generate heavy metal oxides, then the heavy metal oxides continue to react with silicon dioxide in the aerogel to generate silicate, specifically, one part of the heavy metal chlorides can be fixed in the pore canal of the silica-alumina-based aerogel in a physical adsorption mode, and the other part of the heavy metal chlorides and the silica-alumina-based aerogel form stable silicate, so that the adsorption efficiency and the utilization rate of aerogel materials are improved,(e.g. PbCl) 2 The reaction mechanism is as follows: pbCl 2 +SiO 2 +H 2 O＝PbSiO 3 +2HCl；3PbCl 2 +Al 2 O 3 ＝2AlCl 3 +3PbO，PbO+SiO 2 ＝PbSiO 3 )。
The beneficial effects are that: the preparation method disclosed by the invention is simple in process, the alumina sol can be obtained without using an inducer or a catalyst, and secondly, the silica sol precursor liquid is obtained by controlling the hydrolysis time of the tetraethoxysilane and the pH value of the reaction liquid; the silicon-aluminum-based aerogel prepared by the method has good thermal stability, large specific surface area and porosity, and can keep a stable pore structure within 500-900 ℃, so that the silicon-aluminum-based aerogel can be used for adsorbing heavy metal gas in the pyrolysis process.
Drawings
FIG. 1 shows the silica-alumina based aerogel obtained in examples 1 to 6 against a heavy metal gas PbCl 2 Adsorption performance of (c) is compared with a graph of adsorption performance of (c).
Detailed Description
The technical scheme of the invention is further described below with reference to specific embodiments.
Example 1
The preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) 2.5g of Aluminum Isopropoxide (AIP) was added to a mixed solution of ethanol and water in a mixed volume ratio of 15mL:5mL, after mixing, heating and refluxing for 3h under the stirring condition at 80 ℃, stopping stirring, continuing to heat for 1h, cooling to room temperature, adding hydrochloric acid to adjust pH to be 3, and stirring for 10min to obtain alumina wet sol;
(2) Adding 2.55g of TEOS into a mixed solution of ethanol and water, wherein the mixed molar ratio of the ethanol to the water is 7:3, mixing and stirring for 0.5h (silica sol cannot be formed in a short treatment time), and then adjusting the pH=2 by using hydrochloric acid to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor in the step (2), stirring for 2 hours, adding ammonia water to adjust the pH to be neutral, standing for 12 hours to form a silicon-aluminum mixed wet gel, performing solvent exchange with n-hexane (ethanol solvent is exchanged with n-hexane and the structure of a material is changed by changing the polarity of the solution), and drying at 50 ℃ for 6 hours in a vacuum drying oven to obtain silicon-aluminum-based aerogel (the silicon-aluminum molar ratio in the silicon-aluminum-based aerogel is 1:1); grinding the dried silicon-aluminum-based aerogel into fine particles by using a mortar, and screening the materials with the size of 40-60 meshes by using a medicine sieve to perform adsorption experiments.
The specific surface area of the silica-alumina-based aerogel obtained in example 1 was 686.22m 2 ·g -1 Porosity of 0.57cm 3 ·g -1 。
0.6g of the silica-alumina based aerogel was weighed out, and 0.06g of PbCl was weighed out 2 Adding into a secondary reaction furnace for PbCl 2 And (3) gas adsorption experiments. Adsorbing PbCl at 800 ℃ for 40min 2 The adsorption removal rate of (2) was 72.58%, indicating that the silica-alumina-based aerogel prepared in example 1 has good heavy metal gas adsorption performance.
Example 2
The preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) 2.5g of Aluminum Isopropoxide (AIP) was added to a mixed solution of ethanol and water in a mixed volume ratio of 15mL:5mL, after mixing, heating and refluxing for 3h under the stirring condition at 80 ℃, stopping stirring, continuing to heat for 1h, cooling to room temperature, adding hydrochloric acid to adjust pH to be 3, and stirring for 10min to obtain alumina wet sol;
(2) Adding 2.55g of TEOS into a mixed solution of ethanol and water, wherein the mixed molar ratio of the ethanol to the water is 7:3, mixing and stirring for 0.5h (no silica sol is formed in a short treatment time), and then adjusting the pH=2 by using hydrochloric acid to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor in the step (2), stirring for 2 hours, adding ammonia water to adjust the pH to be neutral, standing for 12 hours to form a silicon-aluminum mixed wet gel, performing solvent exchange with n-hexane (the ethanol solvent is exchanged with n-hexane and the structure of a material is changed by changing the polarity of the solution) without heating and aging, and drying in a vacuum drying oven for 10 hours at 60 ℃ to obtain silicon-aluminum based aerogel (the silicon-aluminum molar ratio in the silicon-aluminum based aerogel is 1:1); grinding the dried silicon-aluminum-based aerogel into fine particles by using a mortar, and screening the materials with the size of 40-60 meshes by using a medicine sieve to perform adsorption experiments.
0.6g of the silica-alumina based aerogel was weighed out, and 0.06g of PbCl was weighed out 2 Adding into a secondary reaction furnace for PbCl 2 And (3) gas adsorption experiments. Adsorbing PbCl at 800 ℃ for 40min 2 The adsorption removal rate of (2) was 71.11%, indicating that the drying temperature and time had little effect on the adsorption efficiency.
Example 3
The preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) 2.5g of Aluminum Isopropoxide (AIP) was added to a mixed solution of ethanol and water in a mixed volume ratio of 30mL:10mL, after mixing, heating and refluxing for 3h under the stirring condition at 80 ℃, stopping stirring, continuing to heat for 1h, cooling to room temperature, adding hydrochloric acid to adjust pH to be 3, and stirring for 10min to obtain alumina wet sol;
(2) Adding 2.55g of TEOS into a mixed solution of ethanol and water, wherein the mixed molar ratio of the ethanol to the water is 7:3, mixing and stirring for 0.5h (no silica sol is formed in a short treatment time), and then adjusting the pH=2 by using hydrochloric acid to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor in the step (2), stirring for 2 hours, adding ammonia water to adjust the pH to be neutral, standing for 12 hours to form a silicon-aluminum mixed wet gel, performing solvent exchange with n-hexane (the ethanol solvent is exchanged with n-hexane and the structure of a material is changed by changing the polarity of the solution) without heating and aging, and drying in a vacuum drying oven for 6 hours at 50 ℃ to obtain silicon-aluminum based aerogel (the silicon-aluminum molar ratio in the silicon-aluminum based aerogel is 1:1); grinding the dried silicon-aluminum-based aerogel into fine particles by using a mortar, and screening the materials with the size of 40-60 meshes by using a medicine sieve to perform adsorption experiments.
0.6g of the silica-alumina based aerogel was weighed out, and 0.06g of PbCl was weighed out 2 Adding into a secondary reaction furnace for PbCl 2 And (3) gas adsorption experiments. Adsorbing PbCl at 800 ℃ for 40min 2 The adsorption removal rate of (2) is 66.54%, which shows that the increase of the ethanol and water content in the step (1) is unfavorable for the adsorption of the silica-aluminum-based aerogel to the heavy metal gas, because the aerogel prepared by the ethanol and water with the content has irregular structure, pore channels are easy to collapse at high temperature, the structure is densified, and the adsorption performance to the heavy metal gas is reduced.
Example 4
The preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) 2.5g of Aluminum Isopropoxide (AIP) was added to a mixed solution of ethanol and water in a mixed volume ratio of 15mL:5mL, after mixing, heating and refluxing for 3h under the stirring condition at 80 ℃, stopping stirring, continuing to heat for 1h, cooling to room temperature, adding hydrochloric acid to adjust pH to be 3, and stirring for 10min to obtain alumina wet sol;
(2) Adding 2.55g of TEOS into a mixed solution of ethanol and water, wherein the mixed molar ratio of the ethanol to the water is 5:1, mixing and stirring for 0.5h (no silica sol is formed in a short treatment time), and then adjusting the pH=2 by using hydrochloric acid to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor in the step (2), stirring for 2 hours, adding ammonia water to adjust the pH to be neutral, standing for 12 hours to form a silicon-aluminum mixed wet gel, performing solvent exchange with n-hexane (the ethanol solvent is exchanged with n-hexane and the structure of a material is changed by changing the polarity of the solution) without heating and aging, and drying in a vacuum drying oven for 6 hours at 50 ℃ to obtain silicon-aluminum based aerogel (the silicon-aluminum molar ratio in the silicon-aluminum based aerogel is 1:1); grinding the dried silicon-aluminum-based aerogel into fine particles by using a mortar, and screening the materials with the size of 40-60 meshes by using a medicine sieve to perform adsorption experiments.
0.6g of silicon-aluminum based aerogel is weighedWeighing 0.06g of PbCl 2 Adding into a secondary reaction furnace for PbCl 2 And (3) gas adsorption experiments. Adsorbing PbCl at 800 ℃ for 40min 2 The adsorption removal rate of (2) is 52.31%, which shows that after the alcohol-water ratio in the step is increased, the prepared silicon-aluminum-based aerogel has a reaction rate of PbCl 2 The adsorption efficiency of the silica-alumina based aerogel is lowered because the pore structure and shape of the prepared silica-alumina based aerogel are unfavorable for the adsorption of heavy metal gas.
Example 5
The preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) 5g of Aluminum Isopropoxide (AIP) was added to a mixed solution of ethanol and water in a mixed volume ratio of 15mL:5mL, after mixing, heating and refluxing for 3h under the stirring condition at 80 ℃, stopping stirring, continuing to heat for 1h, cooling to room temperature, adding hydrochloric acid to adjust pH to be 3, and stirring for 10min to obtain alumina wet sol;
(2) Adding 2.55g of TEOS into a mixed solution of ethanol and water, wherein the mixed molar ratio of the ethanol to the water is 7:3, mixing and stirring for 0.5h (no silica sol is formed in a short treatment time), and then adjusting the pH=2 by using hydrochloric acid to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor in the step (2), stirring for 2 hours, adding ammonia water to adjust the pH to be neutral, standing for 12 hours to form a silicon-aluminum mixed wet gel, performing solvent exchange with n-hexane (the ethanol solvent is exchanged with n-hexane and the structure of a material is changed by changing the polarity of the solution) without heating and aging, and drying in a vacuum drying oven for 6 hours at 50 ℃ to obtain silicon-aluminum based aerogel (the silicon-aluminum molar ratio in the silicon-aluminum based aerogel is 1:1); grinding the dried silicon-aluminum-based aerogel into fine particles by using a mortar, and screening the materials with the size of 40-60 meshes by using a medicine sieve to perform adsorption experiments.
0.6g of the silica-alumina based aerogel was weighed out, and 0.06g of PbCl was weighed out 2 Adding into a secondary reaction furnace for PbCl 2 And (3) gas adsorption experiments. Adsorbing PbCl at 800 ℃ for 40min 2 The adsorption removal rate of (2) was 44.37%, which indicates that the silica-alumina ratio in the silica-alumina based aerogel was reduced to thereby allowThe adsorption efficiency is greatly reduced. This is because heavy metals are solidified in the form of silicate by silica-alumina based aerogel at high temperature, and decreasing the silica-alumina ratio reduces the formation of silicate, decreasing adsorption efficiency.
Example 6
The preparation method of the silicon-aluminum-based aerogel comprises the following steps:
(1) 2.5g of Aluminum Isopropoxide (AIP) was added to a mixed solution of ethanol and water in a mixed volume ratio of 15mL:5mL, after mixing, heating and refluxing for 3h under the stirring condition at 80 ℃, stopping stirring, continuing to heat for 1h, cooling to room temperature, adding hydrochloric acid to adjust pH to be 3, and stirring for 10min to obtain alumina wet sol;
(2) Adding 2.55g of TEOS into a mixed solution of ethanol and water, wherein the mixed molar ratio of the ethanol to the water is 7:3, mixing and stirring for 0.5h (no silica sol is formed in a short treatment time), and then adjusting the pH=2 by using hydrochloric acid to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor in the step (2), stirring for 2 hours, adding ammonia water to adjust the pH to be neutral, standing for 12 hours to form a silicon-aluminum mixed wet gel, performing solvent exchange with n-hexane (the ethanol solvent is exchanged with n-hexane and the structure of a material is changed by changing the polarity of the solution) without heating and aging, and drying in a vacuum drying oven for 6 hours at 50 ℃ to obtain silicon-aluminum based aerogel (the silicon-aluminum molar ratio in the silicon-aluminum based aerogel is 1:1); grinding the dried silicon-aluminum-based aerogel into fine particles by using a mortar, and screening the materials with the size of 40-60 meshes by using a medicine sieve to perform adsorption experiments.
0.6g of the silica-alumina based aerogel was weighed out, and 0.06g of PbCl was weighed out 2 Adding into a secondary reaction furnace for PbCl 2 And (3) gas adsorption experiments. Adsorbing PbCl at 600deg.C for 40min 2 The adsorption removal rate of 54.25%, which shows that the adsorption temperature has a great influence on the adsorption efficiency of the adsorbent, because the effective collision between heavy metal and silicon-aluminum based aerogel is reduced due to the reduced temperature, pbCl2 captured by adsorption sites is reduced, and meanwhile, the generation of silicate is also unfavorable, so that the adsorption efficiency is reduced.
The adsorption efficiency of the silica-alumina based aerogels prepared in examples 1 to 6 was calculated as follows:
1. the mass ratio of the added heavy metal to the adsorbent:
m 1 for adding heavy metal mass, m 2 Is the mass of the adsorbent aerogel.
2. Determination of heavy Metal content in adsorption Material after adsorption
After the adsorption material is digested, the concentration w of heavy metal in the adsorbed material is measured by ICP-MS
3. Calculation of adsorption efficiency μ
V is the constant volume, C is the metal concentration measured by ICP-MS, M 1 Is PbCl 2 Molar mass, m 1 ' is the mass of the absorbed aerogel obtained by digestion and weighing, M 2 Is the molar mass of Pb, m 2 ' is the mass, m, of the aerogel weighed after adsorption 3 Is the mass of heavy metals adsorbed by the aerogel.
Table 1 shows the adsorption of PbCl by silica aerogel at 800℃and silica-alumina based aerogel obtained in example 1 2 Comparison of specific surface area and porosity before and after
As can be seen from Table 1, the silica-alumina-based aerogel prepared in example 1 of the present invention has higher thermal stability and larger specific surface area and porosity than those of silica aerogel. After high-temperature adsorption at 800 ℃, the specific surface area of the silica aerogel and the specific surface area of the silica-alumina-based aerogel prepared in the example 1 are respectively reduced by 150.71m 2 ·g -1 And 71.27m 2 ·g -1 The silicon-aluminum-based aerogel prepared in the embodiment 1 is not easy to collapse in pore channels at high temperature, has stable structure and high thermal stability, and can be applied to the adsorption of heavy metal gas in the actual pyrolysis process.
Claims (5)
1. Silica-alumina aerogel is adsorbing PbCl 2 The application of the silica-alumina based aerogel is characterized in that the silica-alumina based aerogel is prepared by adopting the following method, and specifically comprises the following steps:
(1) Adding aluminum isopropoxide into a mixed solution of ethanol and water to obtain a mixed material, heating and refluxing the mixed material under stirring, stopping stirring, continuing heating, cooling to room temperature after heating, and regulating the pH value of the solution to be acidic to obtain alumina wet sol;
(2) Adding ethyl orthosilicate into a mixed solution of ethanol and water, stirring for not more than 0.5h, and then adjusting the pH value of the solution to be acidic to obtain a silica sol precursor solution;
(3) Mixing the alumina wet sol in the step (1) with the silica sol precursor liquid in the step (2), regulating the pH value of the mixed liquid to be neutral after stirring, placing the mixed liquid for at least 12 hours to form silicon-aluminum mixed wet gel, carrying out solvent exchange on the silicon-aluminum mixed wet gel by using n-hexane, and placing the silicon-aluminum mixed wet gel into a vacuum drying oven for drying to obtain silicon-aluminum-based aerogel;
the silicon-aluminum-based aerogel is used for adsorbing PbCl 2 The application in the aspect comprises the following specific application processes: the silicon-aluminum-based aerogel is used for adsorbing PbCl in the pyrolysis process 2 The temperature of the pyrolysis process is 600-900 ℃.
2. The silica-alumina based aerogel according to claim 1 in adsorbing PbCl 2 The application of the method is characterized in that: in the step (1), the mixing volume ratio of ethanol to water is 15-30: 5-10.
3. The silica-alumina based aerogel according to claim 1 in adsorbing PbCl 2 The application of the method is characterized in that: in the step (2), the mixing mole ratio of the ethanol and the water is 5~7:1~3。
4. The silica-alumina based aerogel according to claim 1 in adsorbing PbCl 2 The application of the method is characterized in that: in the step (3), the drying temperature is 50-60 ℃ and the drying time is 6-10 h.
5. The silica-alumina based aerogel according to claim 1 in adsorbing PbCl 2 The application of the method is characterized in that: in the step (3), the molar ratio of the silicon to aluminum elements in the obtained silicon-aluminum-based aerogel is 1:1.
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Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TW201632353A (en) * | 2015-03-03 | 2016-09-16 | 國立臺灣大學 | Vacuum membrane distillation device and method including hydrophobic porous silica aerogel composite membrane |
| CN108607526A (en) * | 2018-05-15 | 2018-10-02 | 芜湖市宝艺游乐科技设备有限公司 | It is a kind of to utilize coal ash for manufacturing for SiO2The method of the cuprous adsorbent of gel combined oxidation |
| CN109621849A (en) * | 2019-01-25 | 2019-04-16 | 浙江工业大学 | A kind of atmospheric preparation method of coated with silica alumina composite aeroge |
| CN110038493A (en) * | 2019-04-30 | 2019-07-23 | 齐鲁工业大学 | A kind of atmospheric preparation method of Al2O3-SiO2 composite aerogel |
| CN111659324A (en) * | 2020-04-28 | 2020-09-15 | 南京工业大学 | Ozone catalytic system composite aerogel and preparation method and application thereof |
| CN111773928A (en) * | 2020-07-02 | 2020-10-16 | 中国科学院城市环境研究所 | Aerogel composite membrane and preparation method and application thereof |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TWI565681B (en) * | 2013-10-15 | 2017-01-11 | 中原大學 | Porous silica aerogel composite membrane and method for making the same and carbon dioxide sorption device |
-
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Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TW201632353A (en) * | 2015-03-03 | 2016-09-16 | 國立臺灣大學 | Vacuum membrane distillation device and method including hydrophobic porous silica aerogel composite membrane |
| CN108607526A (en) * | 2018-05-15 | 2018-10-02 | 芜湖市宝艺游乐科技设备有限公司 | It is a kind of to utilize coal ash for manufacturing for SiO2The method of the cuprous adsorbent of gel combined oxidation |
| CN109621849A (en) * | 2019-01-25 | 2019-04-16 | 浙江工业大学 | A kind of atmospheric preparation method of coated with silica alumina composite aeroge |
| CN110038493A (en) * | 2019-04-30 | 2019-07-23 | 齐鲁工业大学 | A kind of atmospheric preparation method of Al2O3-SiO2 composite aerogel |
| CN111659324A (en) * | 2020-04-28 | 2020-09-15 | 南京工业大学 | Ozone catalytic system composite aerogel and preparation method and application thereof |
| CN111773928A (en) * | 2020-07-02 | 2020-10-16 | 中国科学院城市环境研究所 | Aerogel composite membrane and preparation method and application thereof |
Non-Patent Citations (1)
| Title |
|---|
| Huijun Yu et al..Quartz fiber reinforced Al2O3-SiO2 aerogel composite with highly thermal stability by ambient pressure drying.《Journal of Non-Crystalline Solids》.2018,第505卷79-86. * |
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