CN113842922A - Composite aerogel and preparation method and application thereof - Google Patents
Composite aerogel and preparation method and application thereof Download PDFInfo
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- CN113842922A CN113842922A CN202111049609.4A CN202111049609A CN113842922A CN 113842922 A CN113842922 A CN 113842922A CN 202111049609 A CN202111049609 A CN 202111049609A CN 113842922 A CN113842922 A CN 113842922A
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- 239000004964 aerogel Substances 0.000 title claims abstract description 51
- 239000002131 composite material Substances 0.000 title claims abstract description 43
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims abstract description 57
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 41
- PORQOHRXAJJKGK-UHFFFAOYSA-N 4,5-dichloro-2-n-octyl-3(2H)-isothiazolone Chemical compound CCCCCCCCN1SC(Cl)=C(Cl)C1=O PORQOHRXAJJKGK-UHFFFAOYSA-N 0.000 claims abstract description 24
- 238000001035 drying Methods 0.000 claims abstract description 20
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000011240 wet gel Substances 0.000 claims abstract description 14
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Inorganic materials O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 claims abstract description 13
- 239000000499 gel Substances 0.000 claims abstract description 12
- 238000003756 stirring Methods 0.000 claims abstract description 11
- 239000006228 supernatant Substances 0.000 claims abstract description 11
- 238000005303 weighing Methods 0.000 claims abstract description 11
- GOOHAUXETOMSMM-UHFFFAOYSA-N Propylene oxide Chemical compound CC1CO1 GOOHAUXETOMSMM-UHFFFAOYSA-N 0.000 claims abstract description 9
- 230000032683 aging Effects 0.000 claims abstract description 9
- 238000013329 compounding Methods 0.000 claims abstract description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 7
- 238000002791 soaking Methods 0.000 claims abstract description 3
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical group O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 claims description 69
- 239000000463 material Substances 0.000 claims description 17
- 230000001954 sterilising effect Effects 0.000 claims description 10
- 238000004659 sterilization and disinfection Methods 0.000 claims description 9
- 238000000034 method Methods 0.000 claims description 8
- 229910021380 Manganese Chloride Inorganic materials 0.000 claims description 5
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 claims description 5
- 239000011565 manganese chloride Substances 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 4
- 238000003421 catalytic decomposition reaction Methods 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims description 2
- 244000005700 microbiome Species 0.000 description 11
- 210000000170 cell membrane Anatomy 0.000 description 9
- 230000000694 effects Effects 0.000 description 9
- 229910021645 metal ion Inorganic materials 0.000 description 9
- 239000011572 manganese Substances 0.000 description 8
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 7
- 230000003197 catalytic effect Effects 0.000 description 7
- 239000000460 chlorine Substances 0.000 description 7
- 229910052801 chlorine Inorganic materials 0.000 description 7
- 229910052760 oxygen Inorganic materials 0.000 description 7
- 239000001301 oxygen Substances 0.000 description 7
- 238000006555 catalytic reaction Methods 0.000 description 5
- 241000894006 Bacteria Species 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 239000000411 inducer Substances 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- -1 oxygen ions Chemical class 0.000 description 4
- 239000002904 solvent Substances 0.000 description 4
- 238000007605 air drying Methods 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 3
- 210000002421 cell wall Anatomy 0.000 description 3
- XLJKHNWPARRRJB-UHFFFAOYSA-N cobalt(2+) Chemical compound [Co+2] XLJKHNWPARRRJB-UHFFFAOYSA-N 0.000 description 3
- 238000005034 decoration Methods 0.000 description 3
- 239000007769 metal material Substances 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 229910052761 rare earth metal Inorganic materials 0.000 description 3
- 150000002910 rare earth metals Chemical class 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 244000063299 Bacillus subtilis Species 0.000 description 2
- 235000014469 Bacillus subtilis Nutrition 0.000 description 2
- 102000004190 Enzymes Human genes 0.000 description 2
- 108090000790 Enzymes Proteins 0.000 description 2
- 241000588724 Escherichia coli Species 0.000 description 2
- 241000233866 Fungi Species 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 241000191967 Staphylococcus aureus Species 0.000 description 2
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 238000004887 air purification Methods 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000000969 carrier Substances 0.000 description 2
- 239000012876 carrier material Substances 0.000 description 2
- 210000004027 cell Anatomy 0.000 description 2
- 229910000420 cerium oxide Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 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
- 230000003993 interaction Effects 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 230000033116 oxidation-reduction process Effects 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 2
- 239000000741 silica gel Substances 0.000 description 2
- 229910002027 silica gel Inorganic materials 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- 239000011701 zinc Substances 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- SPOQSWFEPFFHCR-UHFFFAOYSA-N [Ce].[Mn].[Co] Chemical compound [Ce].[Mn].[Co] SPOQSWFEPFFHCR-UHFFFAOYSA-N 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- 230000003385 bacteriostatic effect Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 229910001429 cobalt ion Inorganic materials 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 1
- 230000000149 penetrating effect Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 102000004169 proteins and genes Human genes 0.000 description 1
- 108090000623 proteins and genes Proteins 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
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Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
-
- A—HUMAN NECESSITIES
- A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
- A01N—PRESERVATION OF BODIES OF HUMANS OR ANIMALS OR PLANTS OR PARTS THEREOF; BIOCIDES, e.g. AS DISINFECTANTS, AS PESTICIDES OR AS HERBICIDES; PEST REPELLANTS OR ATTRACTANTS; PLANT GROWTH REGULATORS
- A01N43/00—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds
- A01N43/72—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds having rings with nitrogen atoms and oxygen or sulfur atoms as ring hetero atoms
- A01N43/80—Biocides, pest repellants or attractants, or plant growth regulators containing heterocyclic compounds having rings with nitrogen atoms and oxygen or sulfur atoms as ring hetero atoms five-membered rings with one nitrogen atom and either one oxygen atom or one sulfur atom in positions 1,2
-
- A—HUMAN NECESSITIES
- A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
- A01N—PRESERVATION OF BODIES OF HUMANS OR ANIMALS OR PLANTS OR PARTS THEREOF; BIOCIDES, e.g. AS DISINFECTANTS, AS PESTICIDES OR AS HERBICIDES; PEST REPELLANTS OR ATTRACTANTS; PLANT GROWTH REGULATORS
- A01N59/00—Biocides, pest repellants or attractants, or plant growth regulators containing elements or inorganic compounds
- A01N59/16—Heavy metals; Compounds thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J13/00—Colloid chemistry, e.g. the production of colloidal materials or their solutions, not otherwise provided for; Making microcapsules or microballoons
- B01J13/0091—Preparation of aerogels, e.g. xerogels
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/889—Manganese, technetium or rhenium
- B01J23/8892—Manganese
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- B01J35/23—
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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
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
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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
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
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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
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
Composite aerogel, and preparation method and application thereof, wherein citric acid and MnCl with corresponding mass are weighed2·4H2O、Ce(NO3)2·6H2O、CO(NO3)2·6H2O and absolute ethyl alcohol are stirred untilClarifying for later use, and marking as a solution A; adding propylene oxide into the solution A in a water bath at 30 ℃, uniformly stirring, and standing to obtain wet gel; completely immersing the wet gel in absolute ethyl alcohol, aging for 24-72 h at 50 ℃, pouring out supernate, and replacing with isopropanol; drying the gel with the supernatant removed, and finally roasting at 500 ℃ for 3h to obtain Ce1‑xCoxOn‑MnO2Compounding aerogel; weighing dichlorooctyl isothiazolinone (DCOIT), dissolving in absolute ethyl alcohol, recording as solution B, soaking the roasted composite aerogel in the solution B for 24 hours, and finally drying to obtain the composite aerogel.
Description
Technical Field
The invention relates to the field of air purification, in particular to a composite aerogel with a sterilization function and a preparation method and application thereof for catalytic decomposition of formaldehyde at normal temperature.
Background
In recent years, with the improvement of living standard and the enhancement of health consciousness of people, people pay more attention to indoor air quality of buildings. The formaldehyde in the indoor air is from a variety of sources, is limited by indoor decoration technology, material production process and cost, and currently, home decoration materials without formaldehyde cannot be prepared, so that the formaldehyde exists in the home decoration materials and part of daily necessities, except formaldehyde harm, air pollution caused by propagation of microorganisms such as bacteria and fungi in the room, and indoor sterilization becomes a concern of people. At present, a plurality of methods for purifying formaldehyde are available, an important and commonly applied method is to purify formaldehyde by using an air purifier, a formaldehyde filter screen used by the air purifier is to load a catalytic material on the surface of a porous carrier particle material, and then the particle material is filled into a honeycomb-shaped framework material, in order to ensure that the wind resistance is small and the wind resistance cannot fall off, the used porous carrier material needs to be larger particles, so that the purification effect is influenced, meanwhile, the material only purifies formaldehyde and cannot sterilize, and another layer of sterilization material is compounded when sterilization is needed, so that the resistance of the filter screen is increased, and the cost is increased. According to the traditional method, porous adsorption materials such as zeolite, silica gel, alumina and activated carbon are taken as carriers, noble metal materials and rare earth metal materials with formaldehyde catalytic oxidation functions and silver, zinc or copper-containing substances with sterilization functions are loaded on the carrier materials according to a certain proportion, the carriers such as zeolite, silica gel, alumina and activated carbon only reach adsorption saturation in a short time, and the cost of the noble metal materials is high, so that the design and development of a novel composite functional catalysis material are key to solve the defects, and have great practical significance for realizing formaldehyde degradation and bacteriostasis.
Disclosure of Invention
The technical problem to be solved is as follows: aiming at the problems of saturated adsorption, low utilization rate, high price and the like of catalysts in the market, the invention provides the composite aerogel, the preparation method and the application thereof. The gel has large specific surface area and high porosity, improves catalytic oxidation performance, achieves extremely high dispersity of manganese and cobalt on a cerium oxide carrier, and greatly increases the activity of oxygen species on the surface of the catalyst due to the interaction of rare earth metal-antibacterial metal-carrier, which is two important reasons that the composite aerogel has the activity of catalyzing and oxidizing formaldehyde at room temperature. Metal ion Co2+When (Zn, Ni, Cu) contacts with the cell membrane of the microorganism, the cell membrane is negatively charged and is subjected to coulomb attraction with metal ions, so that the metal ions penetrate through the cell membrane, enter the microorganism body and react with sulfydryl on protein in the microorganism body to destroy enzyme in the microorganism body and interfere the formation of microorganism DNA, thereby achieving the purpose of killing the microorganism. The manganese-cobalt-cerium catalytic center generates hydroxyl radicals and active oxygen ions, and sterilization and bacteriostasis are performed through the strong oxidation reduction capability of the hydroxyl radicals and the active oxygen ions. Finally, the problem that metal ions only act on cell membranes is solved through organic chlorine modification, and the problem of cell structureFungi have one more cell wall than bacteria. Cobalt ions can enter the mould body to play a role in sterilization only by penetrating through two-layer structures of cell walls and cell membranes to achieve the mould-proof effect, so that the combination of inorganic bacteriostatic metal and organic chloride is more extensive in air purification.
The technical scheme is as follows: a preparation method of composite aerogel comprises the following preparation steps: (1) according to the mol ratio of n (citric acid), n (Mn), n (Ce), n (Co), n (EtOH) = 1:1, (0.5-0.8), (0.2-0.5) and (45-55), weighing citric acid and MnCl with corresponding mass2·4H2O、Ce(NO3)2·6H2O、CO(NO3)2·6H2Stirring O and absolute ethyl alcohol until the mixture is clear for later use, and marking the mixture as a solution A; (2) adding 1, 2-epoxypropane with the molar ratio of 1 to (12-15) to citric acid into the solution A in a water bath at 30 ℃, uniformly stirring, and standing to obtain wet gel; (3) completely immersing the wet gel in absolute ethyl alcohol, aging for 24-72 h at 50 ℃, pouring out supernate, and replacing with isopropanol for at least 3 times; (4) drying the gel with the supernatant removed, and finally roasting at 500 ℃ for 3h to obtain Ce1-xCoxOn-MnO2Compounding aerogel; (5) weighing dichlorooctyl isothiazolinone (DCOIT), dissolving in absolute ethyl alcohol, recording as solution B, and soaking the roasted composite aerogel in the solution B for 24 hours, wherein the Ce is1-xCoxOn-MnO2The mass ratio of the composite aerogel to the dichlorooctyl isothiazolinone (DCOIT) to the absolute ethyl alcohol is 1 (0.45-1.8) to (5-6), and finally, the composite aerogel is obtained by drying.
Preferably, in step (1), the molar ratio n (citric acid) n (Mn) n (Ce) n (Co) n (EtOH) = 1: 1: 0.8: 0.2: 51.
Preferably, the molar ratio of the citric acid to the 1, 2-propylene oxide in the step (2) is 1:14, and the standing and gelling time is 5-30 min.
Preferably, the aging time of the step (3) is 48 hours; the time for replacing isopropanol with three times is not less than 12 h.
Preferably, the drying temperature in the step (4) is 80 ℃, and the drying time is 12 h.
Preferably, Ce is used in the step (5)1-xCoxOn-MnO2The mass ratio of the composite aerogel to the dichlorooctyl isothiazolinone (DCOIT) to the absolute ethyl alcohol is 1: 0.6: 5.79.
Preferably, the drying temperature in the step (5) is 60 ℃, and the drying time is 20 h.
The composite aerogel prepared by the preparation method.
The composite aerogel is applied to the preparation of materials with the functions of catalyzing and decomposing formaldehyde and sterilizing at normal temperature.
Has the advantages that: 1. the composite aerogel of the invention is different from the traditional adsorbing material, the manganese and the cobalt obtain extremely high dispersion degree on the cerium oxide carrier, and meanwhile, the interaction of the rare earth metal-bacteriostatic metal-carrier greatly increases the activity of oxygen species on the surface of the catalyst, thereby better catalyzing and oxidizing the formaldehyde. 2. Metal ion Co2+When contacting with the cell membrane of the microorganism, the cell membrane is negatively charged and generates coulomb attraction with metal ions, so that the metal ions penetrate through the cell membrane, destroy enzymes in the microorganism body and interfere the formation of microorganism DNA. 3. The aerogel active oxygen is a metal ion catalytic microorganism active center, generates hydroxyl radicals and active oxygen ions, and performs sterilization and bacteriostasis and better catalytic oxidation of formaldehyde through the strong oxidation reduction capacity of the hydroxyl radicals and the active oxygen ions. 4. According to the invention, the problem that Co metal ions only act on cell membranes is solved by modifying the surface chlorine of the material, and fungi have a layer of cell walls more than bacteria on the cell structure.
Drawings
FIG. 1 is a schematic diagram of activity detection of composite aerogels in example 1, example 2, example 3 and example 4, and the influence of catalytic oxidation of formaldehyde by using chlorine modified aerogel is explored;
FIG. 2 is a graph showing the inhibitory effects of modified composite aerogels of examples 1, 2, 3 and 4 on Escherichia coli, Staphylococcus aureus and Bacillus subtilis.
Detailed Description
The present invention will be described in more detail with reference to specific examples, but the present invention is not limited thereto.
Example 1
(1) Weighing MnCl2•4H2O，Ce(NO3)2•6H2O，CO(NO3)2•6H2Dissolving citric acid in 30mL of absolute ethyl alcohol, wherein the molar ratio n (citric acid) n (Mn) n (Ce) n (Co) n (EtOH) = 1: 1: 0.8: 0.2: 51, stirring uniformly for later use, and marking as solution A;
(2) adding 10mL of propylene oxide inducer into the solution A at the temperature of 30 ℃ in a water bath, and standing to obtain wet gel;
(3) adding 20mL of absolute ethanol into the wet gel to completely immerse the gel in the solvent, aging at 50 ℃ for 48h, pouring out the supernatant, and then performing at least three times of replacement with isopropanol;
(4) placing the gel with the supernatant removed in a forced air drying oven, drying, and roasting at 500 ℃ for 3h to obtain Ce1-xCoxOn-MnO2Compounding aerogel;
(5) 0.9g of dichlorooctyl isothiazolinone (DCOIT) and 2.0g of composite aerogel are weighed and dissolved in 20mL of absolute ethyl alcohol, stirred to be fully soaked, and then dried at 60 ℃ to obtain the chlorine modified composite aerogel.
Example 2
(1) Weighing MnCl2•4H2O，Ce(NO3)2•6H2O，CO(NO3)2•6H2Dissolving citric acid in 30mL of absolute ethyl alcohol, wherein the molar ratio n (citric acid) n (Mn) n (Ce) n (Co) n (EtOH) = 1: 1: 0.8: 0.2: 51, stirring uniformly for later use, and marking as solution A;
(2) adding 10mL of propylene oxide inducer into the solution A at the temperature of 30 ℃ in a water bath, and standing to obtain wet gel;
(3) adding 20mL of absolute ethanol into the wet gel to completely immerse the gel in the solvent, aging at 50 ℃ for 48h, pouring out the supernatant, and then performing at least three times of replacement with isopropanol;
(4) placing the gel with supernatant removed in an air blastDrying in a drying oven, and finally roasting for 3h at 500 ℃ to obtain Ce1-xCoxOn-MnO2Compounding aerogel;
(5) weighing 1.2g of dichlorooctyl isothiazolinone (DCOIT) and 2.0g of composite aerogel, dissolving in 20mL of absolute ethyl alcohol, stirring to fully soak the materials, and then drying at 60 ℃ to obtain the chlorine modified composite aerogel.
Example 3
(1) Weighing MnCl2•4H2O，Ce(NO3)2•6H2O，CO(NO3)2•6H2Dissolving citric acid in 30mL of absolute ethyl alcohol, wherein the molar ratio n (citric acid) n (Mn) n (Ce) n (Co) n (EtOH) = 1: 1: 0.8: 0.2: 51, stirring uniformly for later use, and marking as solution A;
(2) adding 10mL of propylene oxide inducer into the solution A at the temperature of 30 ℃ in a water bath, and standing to obtain wet gel;
(3) adding 20mL of absolute ethanol into the wet gel to completely immerse the gel in the solvent, aging at 50 ℃ for 48h, pouring out the supernatant, and then performing at least three times of replacement with isopropanol;
(4) placing the gel with the supernatant removed in a forced air drying oven, drying, and roasting at 500 ℃ for 3h to obtain Ce1-xCoxOn-MnO2Compounding aerogel;
(5) weighing 2.4g of dichlorooctyl isothiazolinone (DCOIT) and 2.0g of composite aerogel, dissolving in 20mL of absolute ethyl alcohol, stirring to fully soak the materials, and then drying at 60 ℃ to obtain the chlorine modified composite aerogel.
Example 4
(1) Weighing MnCl2•4H2O，Ce(NO3)2•6H2O，CO(NO3)2•6H2Dissolving citric acid in 30mL of absolute ethyl alcohol, wherein the molar ratio n (citric acid) n (Mn) n (Ce) n (Co) n (EtOH) = 1: 1: 0.8: 0.2: 51, stirring uniformly for later use, and marking as solution A;
(2) adding 10mL of propylene oxide inducer into the solution A at the temperature of 30 ℃ in a water bath, and standing to obtain wet gel;
(3) adding 20mL of absolute ethanol into the wet gel to completely immerse the gel in the solvent, aging at 50 ℃ for 48h, pouring out the supernatant, and then performing at least three times of replacement with isopropanol;
(4) placing the gel with the supernatant removed in a forced air drying oven, drying, and roasting at 500 ℃ for 3h to obtain Ce1-xCoxOn-MnO2Compounding aerogel;
(5) 3.6g of dichlorooctyl isothiazolinone (DCOIT) and 2.0g of composite aerogel are weighed and dissolved in 20mL of absolute ethyl alcohol, stirred to be fully soaked, and then dried at 60 ℃ to obtain the chlorine modified composite aerogel.
Performance testing, composite aerogels prepared in all the above examples as test objects
All of the dichlorooctyl isothiazolinone modified Ce1-xCoxOn-MnO2The composite aerogel is applied to room-temperature formaldehyde catalysis and bacteriostasis experiments, wherein the concentration of formaldehyde under the test condition is 1.2 +/-0.1 mg/m3The concentration range of the diluted bacteria (Escherichia coli, Staphylococcus aureus and Bacillus subtilis) is about 105-106cfu/mL, and 0.2g of example sample is weighed, and the formaldehyde catalyzing performance and the bacteriostasis effect are tested, and the data are shown in attached figures 1 and 2. From the obtained product, the modification of dichlorooctyl isothiazolinone is to Ce1-xCoxOn-MnO2The composite aerogel has remarkable influence on the formaldehyde catalysis and bacteriostasis performance, and has the advantages of improved formaldehyde catalysis performance and better bacteriostasis effect when being doped in a proper amount, but the bacteriostasis and the formaldehyde catalysis effect show obvious reduction trend after being introduced excessively. The above examples are only for the purpose of analyzing and understanding the preparation method and the application range of the present invention, but the present invention is not limited to the above examples. If persons skilled in the art should appreciate that they can directly make changes, substitutions, modifications and the like to the invention, they should fall within the scope of the invention.
Claims (9)
1. The preparation method of the composite aerogel is characterized by comprising the following preparation steps: (1) according to the molar ratio n (citric acid): n: (Mn (n), (Ce) n (EtOH) = 1:1 (0.5-0.8) 0.2-0.5 (45-55), weighing citric acid and MnCl2·4H2O、Ce(NO3)2·6H2O、CO(NO3)2·6H2Stirring O and absolute ethyl alcohol until the mixture is clear for later use, and marking the mixture as a solution A; (2) adding 1, 2-epoxypropane with the molar ratio of 1 to (12-15) to citric acid into the solution A in a water bath at 30 ℃, uniformly stirring, and standing to obtain wet gel; (3) completely immersing the wet gel in absolute ethyl alcohol, aging for 24-72 h at 50 ℃, pouring out supernate, and replacing with isopropanol for at least 3 times; (4) drying the gel with the supernatant removed, and finally roasting at 500 ℃ for 3h to obtain Ce1-xCoxOn-MnO2Compounding aerogel; (5) weighing dichlorooctyl isothiazolinone (DCOIT), dissolving in absolute ethyl alcohol, recording as solution B, and soaking the roasted composite aerogel in the solution B for 24 hours, wherein the Ce is1-xCoxOn-MnO2The mass ratio of the composite aerogel to the dichlorooctyl isothiazolinone (DCOIT) to the absolute ethyl alcohol is 1 (0.45-1.8) to (5-6), and finally, the composite aerogel is obtained by drying.
2. The method for preparing composite aerogel according to claim 1, wherein the molar ratio n (citric acid) n (Mn) n (Ce) n (Co) n (EtOH) = 1: 1: 0.8: 0.2: 51 in step (1).
3. The preparation method of the composite aerogel according to claim 1, wherein the molar ratio of the citric acid to the 1, 2-propylene oxide in the step (2) is 1:14, and the standing and gelling time is 5-30 min.
4. The method for preparing composite aerogel according to claim 1, wherein the aging time in step (3) is 48 h; the time for replacing isopropanol with three times is not less than 12 h.
5. The method for preparing composite aerogel according to claim 1, wherein the drying temperature in step (4) is 80 ℃ and the drying time is 12 h.
6. The method for preparing composite aerogel according to claim 1, wherein the Ce of step (5)1-xCoxOn-MnO2The mass ratio of the composite aerogel to the dichlorooctyl isothiazolinone (DCOIT) to the absolute ethyl alcohol is 1: 0.6: 5.79.
7. The method for preparing composite aerogel according to claim 1, wherein the drying temperature in step (5) is 60 ℃ and the drying time is 20 h.
8. A composite aerogel obtained by the production method according to any one of claims 1 to 7.
9. The use of the composite aerogel as claimed in claim 8 in the preparation of materials with normal temperature catalytic decomposition of formaldehyde and sterilization functions.
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