CN111013574A - Preparation method of noble metal/carbon sphere composite catalytic material for removing formaldehyde from air - Google Patents
Preparation method of noble metal/carbon sphere composite catalytic material for removing formaldehyde from air Download PDFInfo
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- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 title claims abstract description 81
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 57
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 56
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 53
- 239000000463 material Substances 0.000 title claims abstract description 41
- 239000002131 composite material Substances 0.000 title claims abstract description 40
- 229910000510 noble metal Inorganic materials 0.000 title claims abstract description 39
- 238000002360 preparation method Methods 0.000 title claims abstract description 7
- 239000002243 precursor Substances 0.000 claims abstract description 42
- 238000000034 method Methods 0.000 claims abstract description 34
- 239000002253 acid Substances 0.000 claims abstract description 14
- 238000002791 soaking Methods 0.000 claims abstract description 10
- 239000000243 solution Substances 0.000 claims description 40
- 238000005470 impregnation Methods 0.000 claims description 20
- 238000001035 drying Methods 0.000 claims description 18
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 claims description 14
- 238000010438 heat treatment Methods 0.000 claims description 13
- CQLFBEKRDQMJLZ-UHFFFAOYSA-M silver acetate Chemical compound [Ag+].CC([O-])=O CQLFBEKRDQMJLZ-UHFFFAOYSA-M 0.000 claims description 12
- 229940071536 silver acetate Drugs 0.000 claims description 12
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 11
- 238000004108 freeze drying Methods 0.000 claims description 11
- 239000001257 hydrogen Substances 0.000 claims description 11
- 229910052739 hydrogen Inorganic materials 0.000 claims description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 10
- 238000007710 freezing Methods 0.000 claims description 9
- 230000008014 freezing Effects 0.000 claims description 9
- PIBWKRNGBLPSSY-UHFFFAOYSA-L palladium(II) chloride Chemical compound Cl[Pd]Cl PIBWKRNGBLPSSY-UHFFFAOYSA-L 0.000 claims description 9
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 8
- 239000003929 acidic solution Substances 0.000 claims description 7
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 6
- 239000012266 salt solution Substances 0.000 claims description 6
- 150000002500 ions Chemical class 0.000 claims description 5
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 4
- 230000008569 process Effects 0.000 claims description 4
- 150000003839 salts Chemical class 0.000 claims description 4
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 2
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 239000012298 atmosphere Substances 0.000 claims description 2
- 150000001721 carbon Chemical class 0.000 claims description 2
- 238000001816 cooling Methods 0.000 claims description 2
- 229910017604 nitric acid Inorganic materials 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 238000005406 washing Methods 0.000 claims description 2
- 229910021604 Rhodium(III) chloride Inorganic materials 0.000 claims 1
- 239000011259 mixed solution Substances 0.000 claims 1
- 239000011148 porous material Substances 0.000 claims 1
- SONJTKJMTWTJCT-UHFFFAOYSA-K rhodium(iii) chloride Chemical compound [Cl-].[Cl-].[Cl-].[Rh+3] SONJTKJMTWTJCT-UHFFFAOYSA-K 0.000 claims 1
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 abstract description 12
- 239000002245 particle Substances 0.000 abstract description 12
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 abstract description 9
- 239000002082 metal nanoparticle Substances 0.000 abstract description 8
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 abstract description 6
- 229910052763 palladium Inorganic materials 0.000 abstract description 5
- 230000007613 environmental effect Effects 0.000 abstract description 4
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 abstract description 4
- 229910052737 gold Inorganic materials 0.000 abstract description 4
- 239000010931 gold Substances 0.000 abstract description 4
- 230000004048 modification Effects 0.000 abstract description 4
- 238000012986 modification Methods 0.000 abstract description 4
- 229910052697 platinum Inorganic materials 0.000 abstract description 4
- SWELZOZIOHGSPA-UHFFFAOYSA-N palladium silver Chemical compound [Pd].[Ag] SWELZOZIOHGSPA-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052703 rhodium Inorganic materials 0.000 abstract description 3
- 239000010948 rhodium Substances 0.000 abstract description 3
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052709 silver Inorganic materials 0.000 abstract description 3
- 239000004332 silver Substances 0.000 abstract description 3
- IHWJXGQYRBHUIF-UHFFFAOYSA-N [Ag].[Pt] Chemical compound [Ag].[Pt] IHWJXGQYRBHUIF-UHFFFAOYSA-N 0.000 abstract description 2
- 238000004887 air purification Methods 0.000 abstract description 2
- 239000000956 alloy Substances 0.000 abstract description 2
- 229910045601 alloy Inorganic materials 0.000 abstract description 2
- 239000006185 dispersion Substances 0.000 abstract description 2
- 238000011068 loading method Methods 0.000 abstract description 2
- 230000003647 oxidation Effects 0.000 description 11
- 238000007254 oxidation reaction Methods 0.000 description 11
- 239000003054 catalyst Substances 0.000 description 8
- 239000012300 argon atmosphere Substances 0.000 description 7
- 239000012153 distilled water Substances 0.000 description 7
- 230000000877 morphologic effect Effects 0.000 description 7
- 238000001291 vacuum drying Methods 0.000 description 7
- 239000003344 environmental pollutant Substances 0.000 description 5
- 238000003760 magnetic stirring Methods 0.000 description 5
- 231100000719 pollutant Toxicity 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 4
- 238000004090 dissolution Methods 0.000 description 4
- 241000282414 Homo sapiens Species 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 230000006872 improvement Effects 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 239000000809 air pollutant Substances 0.000 description 2
- 239000000969 carrier Substances 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 239000010970 precious metal Substances 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 230000010718 Oxidation Activity Effects 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 231100001243 air pollutant Toxicity 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000005034 decoration Methods 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 230000003203 everyday effect Effects 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 231100000171 higher toxicity Toxicity 0.000 description 1
- 238000003905 indoor air pollution Methods 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 244000005700 microbiome Species 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000010815 organic waste Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000006385 ozonation reaction Methods 0.000 description 1
- 230000020477 pH reduction Effects 0.000 description 1
- 238000010422 painting Methods 0.000 description 1
- 230000029058 respiratory gaseous exchange Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 239000012855 volatile organic compound Substances 0.000 description 1
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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0201—Impregnation
- B01J37/0207—Pretreatment of the support
-
- 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
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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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/42—Platinum
-
- 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/44—Palladium
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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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/48—Silver or gold
- B01J23/50—Silver
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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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/48—Silver or gold
- B01J23/52—Gold
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/391—Physical properties of the active metal ingredient
- B01J35/393—Metal or metal oxide crystallite size
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/51—Spheres
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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
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
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Abstract
The invention relates to a preparation method of a noble metal/carbon sphere composite catalytic material for removing formaldehyde from air, belonging to the technical field of indoor air purification. The method comprises the following steps: soaking the porous carbon spheres in an acid solution for modification treatment to obtain modified porous carbon spheres as a carrier; the composite catalytic material is dipped in a noble metal precursor solution with a certain concentration, and is dried and thermally treated after being taken out to obtain the composite catalytic material with noble metal nano-particles loaded on the surface of a porous carbon sphere. The noble metal nano particles comprise silver, gold, platinum, palladium, rhodium, silver palladium, silver platinum palladium and other alloys, and the loading amount of the noble metal nano particles is 1-20 wt%. The noble metals exist in a zero-valent form, and the particle size range of the particles is 5nm-50 nm. The composite catalytic material prepared by the method can keep the unique form of the carbon spheres, has high dispersion degree of the metal nanoparticles, excellent catalytic performance and environmental protection, and has important application potential and value.
Description
Technical Field
The invention relates to a preparation method of a noble metal/carbon sphere composite catalytic material for removing formaldehyde from air, belonging to the technical field of indoor air purification.
Background
Human breathing needs to exchange a large amount of air with the surrounding environment every day, and the quality of the air directly influences the physical health and the comfort of the human. At present, China is in the rapid development stage of industrialization, and industrial waste gas, automobile exhaust, photochemical smog and the like generated every year cause pollution to air (such as pollution of volatile organic compounds such as formaldehyde and the like) to a certain extent. Nowadays, with the improvement of the quality of life of human beings, novel indoor air pollution caused by indoor decoration, furniture painting and the like also becomes an environmental problem which is a hot concern of urban residents in China, wherein formaldehyde is taken as a typical representative, has wide sources and higher toxicity, and is one of serious indoor air pollutants. Therefore, how to scientifically and effectively remove formaldehyde in the air has become an important issue to be solved.
At present, there are many methods for removing formaldehyde pollution in air, such as adsorption method, absorption method, negative ion oxidation method, ozone catalytic oxidation method, biological filtration and plant purification method, low temperature plasma method, catalytic oxidation method, etc. In the above method, the activated carbon adsorption method has a problem that the pollutants are not degraded after desorption. The solution absorption method has certain selectivity to pollutants and also has the problem of secondary pollution. The negative ion oxidation method can effectively decompose formaldehyde, but the generation of negative ions is very unstable and the reaction efficiency is slow. The catalytic ozonation method has simple flow, no secondary pollution problem, low utilization rate and slow reaction efficiency. The biofiltration method is one of the main methods for purifying organic waste gases and malodorous substances. Although the formaldehyde removal effect is good, once the harm caused by the leakage of microorganisms is larger, the safety of the formaldehyde removal agent is not sufficiently studied. Plant purification methods can degrade formaldehyde to some extent, but have limited absorption capacity for formaldehyde. The low-temperature plasma method utilizes the action of active particle pollutants such as high-energy electrons, free radicals and the like to decompose pollutant molecules in a very short time, and various subsequent reactions are carried out to achieve the purpose of decomposing pollutants. But it has high requirements for equipment and a very complicated process. The catalytic oxidation method is to catalyze oxygen in the air and organic pollutants to perform chemical reactions such as oxidation decomposition and the like, so as to decompose the organic pollutants such as formaldehyde and the like. The catalytic oxidation method has attracted extensive attention of researchers due to the advantages of simple operation method, good treatment effect, environmental protection, no pollution and the like.
The key point of removing formaldehyde by the catalytic oxidation method is the selection of a catalyst, and the catalyst for the catalytic oxidation method can be divided into a noble metal catalyst and a transition metal catalyst. The noble metal catalyst can be loaded on different types of carriers to carry out formaldehyde catalytic oxidation at low temperature even at room temperature. The carbon spheres are a porous excellent carrier with large specific surface area, and can be used as a noble metal carrier by increasing the surface activity of the carbon spheres through acidification treatment.
In conclusion, the invention provides a precious metal/carbon sphere composite catalytic material for removing formaldehyde from air, which is obtained by pretreating porous carbon spheres, taking the porous carbon spheres as a carrier, and carrying out vacuum impregnation, drying and heat treatment on the porous carbon spheres by using a precious metal salt solution. The noble metal nano particles comprise silver, gold, platinum, palladium, rhodium, silver palladium, silver platinum palladium and other alloys, and the loading amount of the noble metal nano particles is adjustable within the range of 1-20 wt%. The noble metals exist in a zero-valent form, and the particle size range of the particles is 5nm-50 nm. The composite catalytic material prepared by the method can keep the unique form of the carbon spheres, has high dispersion degree of the metal nanoparticles, excellent catalytic performance and environmental protection, and has important application potential and value.
Disclosure of Invention
The invention discloses a preparation method of a noble metal/carbon sphere composite catalytic material for removing formaldehyde from air, and aims to provide a simple and efficient catalytic material aiming at the prior art so as to solve the problems of low formaldehyde pollution decomposition efficiency, complex catalytic process and the like in the prior air.
In order to realize the purpose, the invention provides that the porous carbon spheres are dipped in an acid solution for modification treatment, and the modified porous carbon spheres are used as carriers; the composite catalytic material is dipped in a noble metal precursor solution with a certain concentration, and is dried and thermally treated after being taken out to obtain the composite catalytic material with noble metal nano-particles loaded on the surface of a porous carbon sphere. The obtained composite material has excellent catalytic performance, is environment-friendly and has wide application prospect.
The preparation method of the air formaldehyde-removing noble metal/carbon sphere composite catalytic material mainly comprises the steps of preparing an acidic solution, modifying porous carbon spheres, preparing a noble metal aqueous solution, vacuum impregnation and freeze drying to obtain a noble metal precursor, heat treatment and the like, and is characterized in that:
(1) preparing an acidic solution with the concentration of 1-10 mol/L, wherein the acidic solution is any one of hydrochloric acid, sulfuric acid, nitric acid, hydrofluoric acid and acetic acid, placing the porous carbon spheres in the acidic solution for soaking for 0.5-10 hours, and washing and drying to obtain modified porous carbon spheres;
(2) preparing a metal salt solution with the concentration of 1mg/mL-30mg/mL by using noble metal salt and water, wherein the noble metal salt is a compound of any one of silver, gold, platinum, palladium and rhodium, placing the modified carbon sphere obtained in the step (1) in a certain noble metal salt solution, further processing a sample by adopting a vacuum impregnation process, taking out the sample, and freeze-drying the sample to obtain a noble metal ion/porous carbon sphere precursor material;
(3) and (3) placing the precursor material obtained in the step (2) in a tubular furnace with the initial temperature of room temperature, carrying out heat treatment for 0.5-4 hours in the atmosphere of hydrogen/argon or hydrogen/nitrogen, cooling to room temperature, and taking out to obtain the noble metal/carbon sphere composite catalytic material.
The noble metal/carbon sphere composite catalytic material for removing formaldehyde from air has the following advantages: the noble metal/carbon sphere composite catalyst has stable morphology, can stably exist in indoor and other environments, and cannot form secondary pollution; the composite catalyst shows excellent formaldehyde catalytic oxidation activity, high catalytic selectivity and good catalytic stability, and products of formaldehyde catalytic oxidation are carbon dioxide and water, so that the composite catalyst has no environmental pollution.
Detailed Description
The following examples are intended to illustrate the invention but are not intended to limit the scope of the invention.
Example 1
(1) 3g of commercially available carbon spheres having a particle size of 3mm were immersed in 50ml of a 3M hydrofluoric acid solution, and the solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken, 0.01mol of palladium chloride is added to be dissolved, and the solution is magnetically stirred for 1 hour to obtain precursor solution.
(3) And (3) taking out the carrier in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 1 hour at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain the precursor of the palladium chloride/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 800 ℃ for 2 hours to obtain the nano palladium/carbon sphere composite catalytic material with stable morphological structure.
Example 2
(1) 3g of commercially available carbon spheres having a particle size of 3mm were immersed in 100ml of a 3M hydrofluoric acid solution, and the solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken, 0.02mol of chloroplatinic acid is added for dissolution, and the precursor solution is obtained after magnetic stirring for 1 hour.
(3) And (3) taking out the carrier in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 360min at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain the precursor of the chloroplatinic acid/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 800 ℃ for 2 hours to obtain the nano platinum/carbon sphere composite catalytic material with stable morphological structure.
Example 3
(1) Commercially available carbon spheres having a particle size of 3mm (2 g) were immersed in 50ml of a 5M sulfuric acid solution, which was passed through the carbon spheres, and the resultant solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken, 0.02mol of silver acetate is added for dissolution, and the precursor solution is obtained after magnetic stirring for 1 hour.
(3) And (2) taking out the carrier in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 2 hours at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain the precursor of the silver acetate/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 500 ℃ for 2 hours to obtain the nano silver/carbon sphere composite catalytic material with stable morphological structure.
Example 4
(1) A commercially available carbon sphere 5g having a particle size of 3mm was immersed in 50ml of a 5M sulfuric acid solution, and the solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken and added with 0.05mol of chloroauric acid for dissolution, and the precursor solution is obtained after magnetic stirring for 1 hour.
(3) And (3) taking out the carrier in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 0.5 hour at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain the precursor of the chloroauric acid/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 600 ℃ for 3 hours to obtain the nano gold/carbon sphere composite catalytic material with stable morphological structure.
Example 5
(1) 3g of commercially available carbon spheres having a particle size of 3mm were immersed in 100ml of a 5M hydrofluoric acid solution, and the solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken, 0.02mol of silver acetate and chloroplatinic acid are respectively added for dissolution, and the precursor solution is obtained after magnetic stirring for 1 hour.
(3) And (2) taking out the carrier in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 2 hours at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain the precursor of the silver acetate and chloroplatinic acid/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 500 ℃ for 2h to obtain the nano silver platinum/carbon sphere composite catalytic material with stable morphological structure.
Example 6
(1) 3g of commercially available carbon spheres having a particle size of 3mm were immersed in 100ml of a 5M hydrofluoric acid solution, and the solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken, 0.02mol of silver acetate and palladium chloride are respectively added to dissolve, and the mixture is magnetically stirred for 1 hour to obtain a precursor solution.
(3) And (3) taking out the carrier in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 1 hour at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain the precursor of the silver acetate and palladium chloride/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 600 ℃ for 1h to obtain the nano silver-palladium/carbon sphere composite catalytic material with stable morphological structure.
Example 7
(1) 3g of commercially available carbon spheres having a particle size of 3mm were immersed in 100ml of a 5M hydrofluoric acid solution, and the solution was placed in a thermostat at a set temperature of 60 ℃ for 3 hours.
(2) 50ml of distilled water is taken, 0.01mol of silver acetate, palladium chloride and chloroplatinic acid are respectively added to dissolve, and the precursor solution is obtained after magnetic stirring for 1 hour.
(3) And (3) taking out the carrier obtained in the step (1), drying, soaking in the precursor solution obtained in the step (2) to ensure that the precursor solution overflows the carrier, putting in a vacuum drying oven for vacuum impregnation for 1 hour at the impregnation temperature of 60 ℃, taking out, freeze-drying at the freezing temperature of-40 ℃, the vacuum degree of 10Pa for 12 hours, and drying for 48 hours to obtain a precursor of the silver acetate, chloroplatinic acid and palladium chloride/carbon sphere composite catalytic material.
(4) And (4) placing the precursor sample obtained in the step (3) in a tubular furnace with the initial temperature of room temperature, introducing hydrogen and argon atmosphere, and carrying out heat treatment at the temperature of 600 ℃ for 2h to obtain the nano silver platinum palladium/carbon sphere composite catalytic material with stable morphological structure.
Although the invention has been described in detail above with reference to a general description and specific examples, it will be apparent to one skilled in the art that modifications or improvements may be made thereto based on the invention. Accordingly, such modifications and improvements are intended to be within the scope of the invention as claimed.
Claims (6)
1. A preparation method of a noble metal/carbon sphere composite catalytic material for removing formaldehyde from air is characterized by comprising the following steps:
(1) preparing an acidic solution with the concentration of 1-10 mol/L, wherein the acidic solution is any one of hydrochloric acid, sulfuric acid, nitric acid, hydrofluoric acid and acetic acid, placing the porous carbon spheres in the acidic solution for soaking for 0.5-10 hours, and washing and drying to obtain modified porous carbon spheres;
(2) preparing a metal salt solution with the concentration of 1mg/mL-30mg/mL by using noble metal salt and water, placing the modified carbon ball obtained in the step (1) in a certain noble metal salt solution, further processing a sample by adopting a vacuum impregnation process, taking out, and freeze-drying to obtain a noble metal ion/porous carbon ball precursor material;
(3) and (3) placing the precursor material obtained in the step (2) in a tubular furnace with the initial temperature of room temperature, carrying out heat treatment for 0.5-4 hours in the atmosphere of hydrogen/argon or hydrogen/nitrogen, cooling to room temperature, and taking out to obtain the noble metal/carbon sphere composite catalytic material.
2. The method for preparing the noble metal/carbon sphere composite catalytic material for removing formaldehyde from air as claimed in claim 1, wherein the diameter of the porous carbon sphere in step (1) is 2mm-6mm, and the pore diameter is in the range of 50nm-5 μm.
3. The method for preparing the noble metal/carbon sphere composite catalytic material for removing formaldehyde by air according to claim 1, wherein the noble metal salt solution in the step (2) is one of a solution of any one of silver acetate, chloroauric acid, chloroplatinic acid, palladium dichloride and rhodium trichloride or a mixed solution of multiple metal salts in silver acetate/palladium dichloride, silver acetate/chloroplatinic acid, silver acetate/palladium dichloride and chloroplatinic acid.
4. The method for preparing the noble metal/carbon sphere composite catalytic material for removing formaldehyde from air as claimed in claim 1, wherein the vacuum impregnation temperature in the step (2) is 20-90 ℃ and the impregnation time is 0.5-5 hours.
5. The method for preparing the noble metal/carbon sphere composite catalytic material for removing formaldehyde from air as claimed in claim 1, wherein the freezing temperature of the freeze-drying in the step (2) is-40 ℃ to-60 ℃, the vacuum degree is 1 to 100Pa, the freezing time is 12 to 24 hours, and the drying time is 24 to 72 hours.
6. The method for preparing the noble metal/carbon sphere composite catalytic material for removing formaldehyde from air as claimed in claim 1, wherein the heat treatment temperature in the step (3) is 300-1000 ℃ and the heat treatment time is 1-4 hours.
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