CN105107524A - Nano-composite material for catalytically decomposing formaldehyde at normal temperature and method for preparing nano-composite material - Google Patents
Nano-composite material for catalytically decomposing formaldehyde at normal temperature and method for preparing nano-composite material Download PDFInfo
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Abstract
The invention relates to a nano-composite material for catalytically decomposing formaldehyde at the normal temperature and a method for preparing the nano-composite material. The method includes a preparing step for mixed liquor of metal salt and silicon sources, a precipitating step and a calcining step. The nano-composite material and the method have the advantages that the nano-composite material comprises silicon dioxide carriers with nano-scale ordered mesopore structures and accordingly has huge specific surface areas; large quantities of mixed metal oxide catalysts with high-activity manganese oxide, copper oxide and cerium oxide are supported inside mesopores and on the surfaces of the nano-composite material, mixed catalyst particles are dispersed in channels of the silicon dioxide carriers with the ordered mesopores, accordingly, excellent dispersing effects can be realized, the nano-composite material is high in catalytic activity, and a large quantity of gas can be adsorbed in sufficient spaces to carry out catalytic reaction.
Description
Technical field
The present invention relates to purification of air application Material Field, be specifically related to a kind of nano composite material for constant temperature catalyzing Formaldehyde decomposition and preparation method thereof, this nano material is applicable to the equipment such as filtering element for air purifier.
Background technology
Formaldehyde (HCHO) is a kind of common indoor air pollutants, and it is mainly derived from the adhesive in indoor hardware fitting and furniture material.Particularly in newly-decorated room, indoor a large amount of finishing material can give out a large amount of formaldehyde, causes the content of formaldehyde in indoor air seriously to exceed national standard.Formaldehyde is the material that a kind of toxicity is higher, can the skin of intense stimulus human body, eyes and respiratory tract, also has anesthetic effect to human central nervous.The formaldehyde of low concentration can damage human respiratory tract, and Long Term Contact can insulting respiratory health.
The administering method of current use can be divided into absorption method, photocatalytic oxidation, Ozonation and metal oxide oxidation catalyst method roughly.Wherein absorption method has the features such as simple to operate, energy consumption is low.The people such as Lin Peng adopt loading available nitrogen composition obtained except formaldehyde activity charcoal, and formaldehyde of its absorption is all fixed on except formaldehyde activity charcoal is inner, not easily flies away and causes secondary pollution (Lin Peng, Lin Kai; Publication No.: CN104607151A).But rely on simple physical absorption, be difficult to thoroughly remove formaldehyde; And its disposal ability is limited, when reaching, its absorption is in limited time upper, just can not reprocessing formaldehyde.In photocatalytic oxidation, the photochemical catalyst of better performances is titanium dioxide, and it PARA FORMALDEHYDE PRILLS(91,95) and organic matter etc. can carry out catalytic degradation, but the problem being easy to reunite and causing catalytic efficiency low.Kan Bin etc. utilize carbon material supported titanium dioxide to obtain formaldehyde catalysis material, because titanium dioxide is difficult to dispersion, so can only disperse in the solution, to be not easy to practical application (Kan Bin, Cheng Henglin; Application publication number: CN104096465A).Ozonation utilizes the strong oxidizing property of ozone to carry out catalysis Formaldehyde decomposition, but ozone itself has toxicity, people is will produce headache in the ozone of 0.1-1ppm in concentration, and eyes are scorching hot, and respiratory tract meeting irriate, be difficult to be applied to remove the formaldehyde in room air.Metal oxide oxidation catalyst method utilizes metal oxide catalysis Formaldehyde decomposition under normal temperature condition with catalytic action, has fast reaction and the loss-free feature of use procedure.
In metal oxide oxidation catalyst method, the more catalyst of research mainly contains noble metal, rare-earth oxide, transition-metals and their oxides etc. at present.Wherein noble metal has good catalytic performance, but due to expensive, limits its application.Du Bin etc. adopt composite noble metal alloy as activated centre, with a kind of composite noble metal alloy formaldehyde through catalytic oxidation agent for carrier obtains of compound crystal type nano TiO 2, reduce the consumption of noble metal, but be difficult to accomplish to substitute noble metal (Du Bin application publication number: CN103357409A) completely.Rare earth metal and transition metal become the alternative materials of noble metal because relative price is cheap, catalytic activity is higher.Due to d layer electronics instability, easily there is the situation of receiving and losing electrons, form multiple variable valence in transition metal; In addition in structure containing having vacant position and defect, both increase the quantity of active oxygen, so have stronger redox property.Wherein the oxide of manganese and copper at normal temperatures PARA FORMALDEHYDE PRILLS(91,95) there is stronger catalytic decomposition activity.Therefore Mn oxide is a kind of catalyst having higher catalytic activity.In rare earth element, cerium also has multiple variable valence, and when oxygen excess, cerium becomes tetravalence from trivalent, and play the effect storing oxygen, when hypoxgia, cerium becomes trivalent again by tetravalence, discharges oxygen in lattice, adds the quantity of active oxygen in system.When catalytic reaction is carried out in the oxide of manganese, copper and the oxide mixing of cerium, cerium plays the synergy storing and discharge oxygen, improves overall catalytic activity; , due to the difference of above a few metal ion species radius, when molecular level mixes, can plug the gap mutually meanwhile, strengthen the mechanical strength of catalyst.In recent years also there is the report about several metal oxide catalytic composite material, but due to the technical process more complicated of preparation method, be difficult to realize practical application widely.
In the catalytic reaction that normal temperature is spontaneous, be the reaction of pernicious gas in pressed powder and air, so contact surface directly has influence on the effect of catalytic reaction.The specific area of catalyst is larger, and the contact area of itself and air is larger, and the catalytic reaction of carrying out in the unit interval is more, and its catalytic activity is stronger.But present catalyst material major part is micron order packed particle, specific area is little, and in catalytic reaction process, only have the particle on surface in action, the very difficult of inside uses, and greatly limit the catalytic activity of material.
Summary of the invention
Based on above-mentioned mentioned problem, one object of the present invention is nano composite material providing a kind of constant temperature catalyzing Formaldehyde decomposition and preparation method thereof, this Nano-composite materials process is simple, and can formaldehyde at room temperature rapidly and efficiently in catalytic decomposition room air.
The invention provides a kind of nano composite material of constant temperature catalyzing Formaldehyde decomposition, described nano composite material comprises silica supports, and described silica supports has nano ordered meso-hole structure; Further, the mesoporous inner dispersion of described silica supports carries metal oxide catalyst.
Preferably, described metal oxide catalyst is Mn oxide, Cu oxide and cerium oxide particle mixture.
Preferably, the mesoporous aperture in described silica supports is 1-20nm.
Preferably, in described nano composite material, the mol ratio of metal oxide catalyst and silica is 1: (1.0-40).It is further preferred that the mol ratio of metal oxide catalyst and silica is 1: (1.7-20).
Preferably, in described nano composite material, described Mn oxide has divalent manganesetion (MnII), described Cu oxide has bivalent cupric ion (CuII), described cerium oxide has trivalent cerium ion (CeIII).
Preferably, in described nano composite material, the mol ratio of described MnII, CuII and CeIII is (0.67-0.87): (0.1-0.3): (0.03-0.15).It is further preferred that the mol ratio of MnII, CuII and CeIII is (0.67-0.87): (0.12-0.25): (0.06-0.15).
The nano composite material of this catalyst is nano ordered meso-hole structure, has huge specific area (specific area 500-1000cm
2/ g); Its mesoporous inside and area load have the mixed metal oxide catalyst of highly active Mn oxide, Cu oxide and cerium oxide in a large number, the catalyst granules of mixing is scattered in the duct of mesoporous silicon oxide, there is good peptizaiton, there is higher catalytic activity; Mesoporous silicon oxide is inner a large amount of order mesoporously not only can disperse the catalyst granules carrying dispersion, and enough spaces can be provided to adsorb a large amount of gas carry out catalytic reaction.
When the catalytic reaction of PARA FORMALDEHYDE PRILLS(91,95) is carried out in the oxide of manganese, copper and the oxide mixing of cerium, cerium plays the synergy storing and discharge oxygen, improves overall catalytic activity., due to the difference of above several metal (manganese, copper and cerium) ionic radius, when molecular level mixes, can plug the gap mutually meanwhile, strengthen the mechanical strength of catalyst.Therefore manganese, copper and cerium three kinds of oxides are used in combination, in catalytic reaction, due to mutual synergy, enhance the mechanical strength of nano composite material.
In order to prepare above-mentioned nano composite material, present invention also offers a kind of preparation method of constant temperature catalyzing Formaldehyde decomposition nano composite material, the method generates has order mesoporous silica supports, and in the process of synthesis, the mixed metal oxide catalyst comprising Mn oxide, Cu oxide and cerium oxide is carried on the avtive spot of this support material internal dispersedly.
The preparation method of this constant temperature catalyzing Formaldehyde decomposition nano composite material comprises the following steps: the preparation steps of slaine and silicon source mixed solution, settling step and calcining step; Wherein, the preparation steps of slaine and silicon source mixed solution is specific as follows: be dissolved in water by MnII salt, CuII salt and CeIII salt, fully stirs the mixing salt solution forming clarification; Silicon source and surfactant mixed dissolution are obtained silicon source solution; In the solution of above-mentioned silicon source, first add alkali lye regulate pH value, then add mixing salt solution, form slaine and silicon source mixed solution, and in the above-mentioned process added vigorous stirring; Settling step specifically comprises: after reaction certain hour, slaine described in suction filtration and silicon source mixed solution, and oven dry obtains powder; By obtained powder dispersion in the ethanolic solution of uniform temperature after certain hour, suction filtration, oven dry, obtain the powder after dispersion treatment; Calcining step specifically comprises: obtain powdered substance after the powder after above-mentioned dispersion treatment is calcined certain hour under certain calcining heat, is the nano material with nano ordered mesoporous silica O composite metallic oxide catalyst.
As preferably, described silicon source is the one in sodium metasilicate, ethyl orthosilicate.
As preferably, described surfactant is the one in Cetyltrimethylammonium bromide, softex kw, dodecyl sodium sulfate, neopelex.It is further preferred that the concentration of described surfactant is 0.02-1g/100mL.Further preferably, the concentration of described surfactant is 0.05-0.8g/100mL.The amount of the Cetyltrimethylammonium bromide such as, dropped in every 1000mL water in reaction system controls within the scope of 0.2-10g, and preferred dosage is 0.5-8g.
As preferably, described MnII salt is the one in manganese sulfate, manganese nitrate.
As preferably, described CuII salt is the one in copper sulphate, copper nitrate.
As preferably, described CeIII salt is cerous nitrate.
As preferably, described alkali lye is the one in NaOH, ammoniacal liquor.
As preferably, the molar ratio of described MnII, CuII and CeIII salt is (0.67-0.87): (0.1-0.3): (0.03-0.15).It is further preferred that the molar ratio of MnII, CuII and CeIII salt is (0.67-0.87): (0.12-0.25): (0.06-0.15).
As preferably, described silicon source solution is being heated to 30-90 DEG C with alkali lye, mixing salt solution before reacting.Preferably, described silicon source solution is being heated to 40-85 DEG C with alkali lye, mixing salt solution before reacting.
As preferably, successively add in the step of alkali lye and mixing salt solution in the solution of silicon source, the pH of slaine and silicon source mixed solution remains on 8-11.It is further preferred that the pH of slaine and silicon source mixed solution remains on 8.5-10.
As preferably, the reaction time range of silicon source solution and mixing salt solution and alkali lye is 0.5-10h.Preferably, described reaction time range is 0.5-5h.
As preferably, powder dispersion described in settling step is 3-40h in the time of ethanolic solution.It is further preferred that described powder dispersion is 5-30h in the time of ethanolic solution.
As preferably, the temperature of ethanolic solution described in settling step is 30-70 DEG C.It is further preferred that the temperature of described ethanolic solution is 40-68 DEG C.
As preferably, in calcining step, described calcining heat is 300-800 DEG C.It is further preferred that described calcining heat is 350-700 DEG C.
As preferably, in calcining step, the time range of described powder calcining is 0.5-5h.It is further preferred that the time range of described powder calcining is 1-5h.
The process forming nano ordered meso-hole structure in above-mentioned course of reaction is: due to the build-in attribute of surfactant, and when it reaches finite concentration in the solution, its hydrophobic side can condense together, and water-wet side then, can form the micella of definite shape outwardly.In the process of reaction, the precursor of the outermost water-wet side of micella and silicon source or metal oxide combines, and is in the outer field silicon source of micella and also can combines with the precursor of metal oxide; In the process of calcining, remove the surfactant of micella inside, inner hollow structure part just just defines the mesoporous part of composite.Further, in course of reaction, catalyst precursor combines with hydrolysis silicon source compound and a small amount of surfactant, is dispersed among mesoporous material uniformly, serves the effect of nature dispersed catalyst; In addition, after prepared by precursor, carry out dispersion treatment with ethanol, material has also been served to the effect of dispersion, thus course of reaction improves the dispersiveness of catalyst in the middle of mesoporous SiO 2 structure.
Compared with prior art, tool of the present invention has the following advantages: 1, the synthesis step of catalyst is simple; 2, reactive metal oxides catalyst distribution is in the duct of ordered mesoporous silica dioxide, has good dispersion, active high feature; 3, carrier material has huge specific area, is the space that catalytic reaction provides, ensure that the high efficiency of catalyst; 4, three kinds of active materials mix at molecular level, play concerted catalysis effect, improve overall catalytic activity.
Accompanying drawing explanation
Accompanying drawing 1 is the SEM structural representation of nano composite material sample prepared by embodiment 1;
Accompanying drawing 2 is the SEM structural representation of nano composite material sample prepared by embodiment 2;
Accompanying drawing 3 is the SEM structural representation of nano composite material sample prepared by embodiment 3;
Accompanying drawing 4 is the SEM structural representation of nano composite material sample prepared by embodiment 4;
Accompanying drawing 5 is the SEM structural representation of nano composite material sample prepared by embodiment 5.
Detailed description of the invention
Below by embodiment, and by reference to the accompanying drawings, technical scheme of the present invention is done more specifically bright.
Embodiment 1
14.71g manganese sulfate monohydrate, 2.50g cupric sulfate pentahydrate and 1.33g six water cerous nitrate are dissolved in 200mL pure water, fully stir the mixing salt solution forming clarification; 28.42g nine water sodium metasilicate and 2.00g Cetyltrimethylammonium bromide mixed dissolution are obtained silicon source solution in 1000mL pure water, adds the pH to 9.0 of the sodium hydrate regulator solution of 14mL1mol/L, and be heated to 30 DEG C; Above-mentioned mixing salt solution is added fast in the solution of above-mentioned silicon source, and vigorous stirring; After reaction 2h, suction filtration slaine and silicon source mixed solution, be scattered in constant temperature stirring 30h in 50 DEG C of ethanolic solutions and carry out dispersion treatment, then suction filtration by obtained filter residue powder; Obtain powdered substance after filter residue powder after above-mentioned dispersion treatment is calcined 0.5h at 800 DEG C, be the nano composite material with nano ordered mesoporous silicon oxide complex copper manganese cerium catalyst.
Through SEM test (as shown in Figure 1 the present embodiment prepare the SEM structural representation of nano composite material sample), show that the skeleton of synthesized catalyst nano composite is ordered mesopore structure, its aperture is between 1-20nm.
The composite nano materials getting the above-mentioned preparation of 1.00g is placed in glass tube that diameter is 5mm and core carries out catalytic decomposition activity assessment.The bottom of glass tube is connected with formaldehyde generator, and top is connected with gas chromatograph on-line detector.Pump air to be blasted in formaldehyde generator and formaldehyde to be mixed to get containing concentration of formaldehyde be the air of 120ppm, to enter from bottom containing the air of formaldehyde and be equipped with the glass tube of composite catalyst, then enter into through glass tube top the content that chromatography of gases detects formaldehyde.Testing result shows, it is 99% that the composite catalyst prepared in the present embodiment carries out catalytic decomposition efficiency once to the formaldehyde of 120ppm at ambient temperature.
Embodiment 2
0.42g tetra-water manganese nitrate, 0.19g cupric sulfate pentahydrate and 0.03g six water cerous nitrate are dissolved in 200mL pure water, fully stir the mixing salt solution forming clarification; 28.42g nine water sodium metasilicate and 0.20g Cetyltrimethylammonium bromide mixed dissolution are obtained silicon source solution in 1000mL pure water, adds the pH to 8.0 of the sodium hydrate regulator solution of 10mL1mol/L, and be heated to 30 DEG C; Above-mentioned mixing salt solution is added fast in the solution of above-mentioned silicon source, and vigorous stirring; After reaction 0.5h, suction filtration slaine and silicon source mixed solution, be scattered in constant temperature stirring 5h in 70 DEG C of ethanolic solutions and carry out dispersion treatment, then suction filtration by obtained filter residue powder; Obtain powdered substance after filter residue powder after above-mentioned dispersion treatment is calcined 5h at 300 DEG C, be the nano composite material (as shown in Figure 2 the present embodiment prepare the SEM structural representation of nano composite material sample) with nano ordered mesoporous silicon oxide complex copper manganese cerium catalyst.
Catalytic performance test is with embodiment 1, and it is 97.5% that testing result shows that the composite catalyst prepared in the present embodiment carries out catalytic decomposition efficiency once to the formaldehyde of 120ppm at ambient temperature.
Embodiment 3
0.87g tetra-water manganese nitrate, 0.20g cupric sulfate pentahydrate and 0.33g six water cerous nitrate are dissolved in 200mL pure water, fully stir the mixing salt solution forming clarification; 28.42g nine water sodium metasilicate and 10.00g Cetyltrimethylammonium bromide mixed dissolution are obtained silicon source solution in 1000mL pure water, adds the pH to 11.0 of the sodium hydrate regulator solution of 23mL1mol/L, and be heated to 30 DEG C; Above-mentioned mixing salt solution is added fast in the solution of above-mentioned silicon source, and vigorous stirring; After reaction 5h, suction filtration slaine and silicon source mixed solution, be scattered in 30 DEG C of ethanolic solutions after constant temperature stirring 20h, then suction filtration by obtained filter residue powder; Obtain powdered substance after filter residue powder after above-mentioned dispersion treatment is calcined 3h at 400 DEG C, be the nano composite material (as shown in Figure 3 the present embodiment prepare the SEM structural representation of nano composite material sample) with nano ordered mesoporous silicon oxide complex copper manganese cerium catalyst.
Catalytic performance test is with embodiment 1, and it is 97.5% that testing result shows that the composite catalyst prepared in the present embodiment carries out catalytic decomposition efficiency once to the formaldehyde of 120ppm at ambient temperature.
Embodiment 4
1.76g tetra-water manganese nitrate, 0.41g copper nitrate and 0.35g six water cerous nitrate are dissolved in 200mL pure water, fully stir the mixing salt solution forming clarification; 28.42g nine water sodium metasilicate and 4.00g Cetyltrimethylammonium bromide mixed dissolution are obtained silicon source solution in 1000mL pure water, adds the pH to 10.0 of the sodium hydrate regulator solution of 19mL1mol/L, and be heated to 30 DEG C; Above-mentioned mixing salt solution is added fast in the solution of above-mentioned silicon source, and vigorous stirring; After reaction 4h, suction filtration slaine and silicon source mixed solution, be scattered in 40 DEG C of ethanolic solutions after constant temperature stirring 25h, then suction filtration by obtained filter residue powder; Obtain powdered substance after filter residue powder after above-mentioned dispersion treatment is calcined 2h at 500 DEG C, be the nano composite material (as shown in Figure 4 the present embodiment prepare the SEM structural representation of nano composite material sample) with nano ordered mesoporous silicon oxide complex copper manganese cerium catalyst.
Catalytic performance test is with embodiment 1, and it is 98.5% that testing result shows that the composite catalyst prepared in the present embodiment carries out catalytic decomposition efficiency once to the formaldehyde of 120ppm at ambient temperature.
Embodiment 5
6.93g manganese sulfate monohydrate, 2.25g cupric sulfate pentahydrate and 2.17g six water cerous nitrate are dissolved in 200mL pure water, fully stir the mixing salt solution forming clarification; 28.42g nine water sodium metasilicate and 7.00g Cetyltrimethylammonium bromide mixed dissolution are obtained silicon source solution in 1000mL pure water, adds the pH to 9.5 of the sodium hydrate regulator solution of 17.3mL1mol/L, and be heated to 30 DEG C; Above-mentioned mixing salt solution is added fast in the solution of above-mentioned silicon source, and vigorous stirring; After reaction 3h, suction filtration slaine and silicon source mixed solution, be scattered in constant temperature stirring 40h in 60 DEG C of ethanolic solutions and carry out dispersion treatment, then suction filtration by obtained filter residue powder; Obtain powdered substance after filter residue powder after above-mentioned dispersion treatment is calcined 2.5h at 600 DEG C, be the nano composite material (as shown in Figure 5 the present embodiment prepare the SEM structural representation of nano composite material sample) with nano ordered mesoporous silicon oxide complex copper manganese cerium catalyst.
Catalytic performance test is with embodiment 1, and it is 98% that testing result shows that the composite catalyst prepared in the present embodiment carries out catalytic decomposition efficiency once to the formaldehyde of 120ppm at ambient temperature.
Above embodiment is only for illustration of the present invention; and be not limitation of the present invention; the those of ordinary skill of relevant technical field; without departing from the spirit and scope of the present invention; can also make a variety of changes and modification; therefore all equivalent technical schemes also belong to category of the present invention, and scope of patent protection of the present invention should be defined by the claims.
Claims (10)
1. a nano composite material for constant temperature catalyzing Formaldehyde decomposition, described nano composite material comprises silica supports, and described silica supports has nano ordered meso-hole structure; Further, the mesoporous inner dispersion of described silica supports carries metal oxide catalyst.
2. nano composite material according to claim 1, is characterized in that, described metal oxide catalyst is Mn oxide, Cu oxide and cerium oxide particle mixture.
3. nano composite material according to claim 1, is characterized in that, the mesoporous aperture in described silica supports is 1-20nm.
4. nano composite material according to claim 1, is characterized in that, in described nano composite material, the mol ratio of metal oxide catalyst and silica is 1: (1.0-40).
5. nano composite material according to claim 4, is characterized in that, the mol ratio of metal oxide catalyst and silica is 1: (1.7-20).
6. nano composite material according to claim 2, it is characterized in that, in described nano composite material, described Mn oxide has divalent manganesetion (MnII), described Cu oxide has bivalent cupric ion (CuII), described cerium oxide has trivalent cerium ion (CeIII).
7. nano composite material according to claim 6, is characterized in that, in described nano composite material, the mol ratio of described MnII, CuII and CeIII is (0.67-0.87): (0.1-0.3): (0.03-0.15).
8. nano composite material according to claim 7, is characterized in that, the mol ratio of MnII, CuII and CeIII is (0.67-0.87): (0.12-0.25): (0.06-0.15).
9. a preparation method for constant temperature catalyzing Formaldehyde decomposition nano composite material, is characterized in that, comprises the following steps: the preparation steps of slaine and silicon source mixed solution, settling step and calcining step; Wherein, the preparation steps of slaine and silicon source mixed solution is specific as follows: be dissolved in water by MnII salt, CuII salt and CeIII salt, fully stirs the mixing salt solution forming clarification; Silicon source and surfactant mixed dissolution are obtained silicon source solution; In the solution of above-mentioned silicon source, first add alkali lye regulate pH value, then add above-mentioned mixing salt solution, form slaine and silicon source mixed solution, and in the above-mentioned process added vigorous stirring; Settling step specifically comprises: after reaction certain hour, slaine described in suction filtration and silicon source mixed solution, and oven dry obtains powder; By obtained powder dispersion in the ethanolic solution of uniform temperature after certain hour, suction filtration, oven dry, obtain the powder after dispersion treatment; Calcining step specifically comprises: obtain powdered substance after the powder after above-mentioned dispersion treatment is calcined certain hour under certain calcining heat, is the nano material with nano ordered mesoporous silica O composite metallic oxide catalyst.
10. preparation method according to claim 9, is characterized in that, described silicon source is the one in sodium metasilicate, ethyl orthosilicate.
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| CN108654556A (en) * | 2018-05-28 | 2018-10-16 | 福建远翔新材料股份有限公司 | A kind of preparation method of nanometer of national standard method overlay film silica formaldehyde purifying agent |
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| CN109364942A (en) * | 2018-12-10 | 2019-02-22 | 广州立白企业集团有限公司 | A kind of support type charing PEI MOF catalyst of Mn-Cu-Ce high degree of dispersion and preparation method thereof |
| CN109364942B (en) * | 2018-12-10 | 2021-05-28 | 广州立白企业集团有限公司 | Mn-Cu-Ce highly-dispersed supported carbonized PEI @ MOF catalyst and preparation method thereof |
| CN110518213A (en) * | 2019-08-30 | 2019-11-29 | 深圳市德方纳米科技股份有限公司 | A kind of porous silicon-carbon nano tube compound material and its preparation method and application |
| CN110721579A (en) * | 2019-11-12 | 2020-01-24 | 庆泓技术(上海)有限公司 | Method for deodorizing and sterilizing refrigerator |
| CN110975853A (en) * | 2019-11-29 | 2020-04-10 | 扬州大学 | Transition metal doped micron-sized spherical silicon dioxide catalyst and preparation method thereof |
| CN112604693A (en) * | 2020-12-15 | 2021-04-06 | 南京工业大学 | Mesoporous manganese-based composite oxide and preparation method and application thereof |
| US11648329B1 (en) | 2021-11-24 | 2023-05-16 | Rht Limited | Air purifiers |
| WO2023093655A1 (en) * | 2021-11-24 | 2023-06-01 | Rht Limited | Catalyst compositions and methods for decomposing formaldehyde thereof |
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