CN114749151A - Formaldehyde adsorbent for air purification and preparation method and application thereof - Google Patents
Formaldehyde adsorbent for air purification and preparation method and application thereof Download PDFInfo
- Publication number
- CN114749151A CN114749151A CN202210484206.0A CN202210484206A CN114749151A CN 114749151 A CN114749151 A CN 114749151A CN 202210484206 A CN202210484206 A CN 202210484206A CN 114749151 A CN114749151 A CN 114749151A
- Authority
- CN
- China
- Prior art keywords
- formaldehyde
- air purification
- mesoporous carbon
- solution
- adsorbent
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 title claims abstract description 270
- 239000003463 adsorbent Substances 0.000 title claims abstract description 55
- 238000004887 air purification Methods 0.000 title claims abstract description 38
- 238000002360 preparation method Methods 0.000 title claims abstract description 28
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 66
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 52
- 238000003756 stirring Methods 0.000 claims abstract description 42
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims abstract description 39
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 claims abstract description 37
- 239000005011 phenolic resin Substances 0.000 claims abstract description 37
- 229920001568 phenolic resin Polymers 0.000 claims abstract description 37
- 239000000203 mixture Substances 0.000 claims abstract description 29
- 238000001914 filtration Methods 0.000 claims abstract description 25
- 238000005406 washing Methods 0.000 claims abstract description 23
- 238000001035 drying Methods 0.000 claims abstract description 18
- 238000012719 thermal polymerization Methods 0.000 claims abstract description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 17
- 230000003647 oxidation Effects 0.000 claims abstract description 16
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 16
- LXBGSDVWAMZHDD-UHFFFAOYSA-N 2-methyl-1h-imidazole Chemical compound CC1=NC=CN1 LXBGSDVWAMZHDD-UHFFFAOYSA-N 0.000 claims abstract description 15
- 239000008367 deionised water Substances 0.000 claims abstract description 13
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 13
- 229910017052 cobalt Inorganic materials 0.000 claims abstract description 12
- 239000010941 cobalt Substances 0.000 claims abstract description 12
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims abstract description 12
- 150000003751 zinc Chemical class 0.000 claims abstract description 8
- 239000012298 atmosphere Substances 0.000 claims abstract description 7
- 150000002505 iron Chemical class 0.000 claims abstract description 6
- 238000003763 carbonization Methods 0.000 claims abstract description 5
- 239000000243 solution Substances 0.000 claims description 68
- 238000000034 method Methods 0.000 claims description 36
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 30
- 238000010438 heat treatment Methods 0.000 claims description 28
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 22
- 239000002243 precursor Substances 0.000 claims description 22
- 239000003575 carbonaceous material Substances 0.000 claims description 20
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 18
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 16
- ONDPHDOFVYQSGI-UHFFFAOYSA-N zinc nitrate Chemical compound [Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ONDPHDOFVYQSGI-UHFFFAOYSA-N 0.000 claims description 16
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims description 15
- 239000001307 helium Substances 0.000 claims description 13
- 229910052734 helium Inorganic materials 0.000 claims description 13
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 claims description 13
- 239000012286 potassium permanganate Substances 0.000 claims description 12
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 11
- 238000010000 carbonizing Methods 0.000 claims description 11
- 238000001816 cooling Methods 0.000 claims description 11
- 238000001704 evaporation Methods 0.000 claims description 11
- 239000011259 mixed solution Substances 0.000 claims description 11
- 230000007935 neutral effect Effects 0.000 claims description 11
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 10
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 9
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 9
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 claims description 8
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims description 8
- 150000001879 copper Chemical class 0.000 claims description 6
- 150000002696 manganese Chemical class 0.000 claims description 6
- 230000001590 oxidative effect Effects 0.000 claims description 6
- 229920000428 triblock copolymer Polymers 0.000 claims description 6
- JIAARYAFYJHUJI-UHFFFAOYSA-L zinc dichloride Chemical compound [Cl-].[Cl-].[Zn+2] JIAARYAFYJHUJI-UHFFFAOYSA-L 0.000 claims description 6
- 229910052786 argon Inorganic materials 0.000 claims description 5
- 239000011261 inert gas Substances 0.000 claims description 5
- 239000007800 oxidant agent Substances 0.000 claims description 5
- 239000012670 alkaline solution Substances 0.000 claims description 4
- 229910021578 Iron(III) chloride Inorganic materials 0.000 claims description 3
- 229910021380 Manganese Chloride Inorganic materials 0.000 claims description 3
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 claims description 3
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 3
- ZOIORXHNWRGPMV-UHFFFAOYSA-N acetic acid;zinc Chemical compound [Zn].CC(O)=O.CC(O)=O ZOIORXHNWRGPMV-UHFFFAOYSA-N 0.000 claims description 3
- 229940011182 cobalt acetate Drugs 0.000 claims description 3
- GVPFVAHMJGGAJG-UHFFFAOYSA-L cobalt dichloride Chemical compound [Cl-].[Cl-].[Co+2] GVPFVAHMJGGAJG-UHFFFAOYSA-L 0.000 claims description 3
- QAHREYKOYSIQPH-UHFFFAOYSA-L cobalt(II) acetate Chemical compound [Co+2].CC([O-])=O.CC([O-])=O QAHREYKOYSIQPH-UHFFFAOYSA-L 0.000 claims description 3
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 claims description 3
- OPQARKPSCNTWTJ-UHFFFAOYSA-L copper(ii) acetate Chemical compound [Cu+2].CC([O-])=O.CC([O-])=O OPQARKPSCNTWTJ-UHFFFAOYSA-L 0.000 claims description 3
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 claims description 3
- PVFSDGKDKFSOTB-UHFFFAOYSA-K iron(3+);triacetate Chemical compound [Fe+3].CC([O-])=O.CC([O-])=O.CC([O-])=O PVFSDGKDKFSOTB-UHFFFAOYSA-K 0.000 claims description 3
- 229940071125 manganese acetate Drugs 0.000 claims description 3
- 239000011565 manganese chloride Substances 0.000 claims description 3
- 235000002867 manganese chloride Nutrition 0.000 claims description 3
- 229940099607 manganese chloride Drugs 0.000 claims description 3
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims description 3
- 239000004246 zinc acetate Substances 0.000 claims description 3
- 239000011592 zinc chloride Substances 0.000 claims description 3
- 235000005074 zinc chloride Nutrition 0.000 claims description 3
- 238000001354 calcination Methods 0.000 claims description 2
- 150000001868 cobalt Chemical class 0.000 claims description 2
- 150000003839 salts Chemical class 0.000 claims description 2
- 238000001179 sorption measurement Methods 0.000 abstract description 29
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 abstract description 7
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 abstract description 4
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 abstract description 4
- 229910052802 copper Inorganic materials 0.000 abstract description 4
- 239000010949 copper Substances 0.000 abstract description 4
- 229910052748 manganese Inorganic materials 0.000 abstract description 4
- 239000011572 manganese Substances 0.000 abstract description 4
- 238000005286 illumination Methods 0.000 abstract description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 28
- 239000007789 gas Substances 0.000 description 13
- 239000012855 volatile organic compound Substances 0.000 description 11
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 10
- 229910052799 carbon Inorganic materials 0.000 description 10
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 9
- 239000000463 material Substances 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 8
- 230000000694 effects Effects 0.000 description 7
- 230000001699 photocatalysis Effects 0.000 description 7
- 230000015556 catabolic process Effects 0.000 description 6
- 238000006731 degradation reaction Methods 0.000 description 6
- 239000002105 nanoparticle Substances 0.000 description 6
- 238000000746 purification Methods 0.000 description 6
- 238000010146 3D printing Methods 0.000 description 5
- 239000004408 titanium dioxide Substances 0.000 description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 4
- YRKCREAYFQTBPV-UHFFFAOYSA-N acetylacetone Chemical compound CC(=O)CC(C)=O YRKCREAYFQTBPV-UHFFFAOYSA-N 0.000 description 4
- 239000002775 capsule Substances 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 4
- 239000003344 environmental pollutant Substances 0.000 description 4
- 238000002156 mixing Methods 0.000 description 4
- 238000007146 photocatalysis Methods 0.000 description 4
- 231100000719 pollutant Toxicity 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 239000004964 aerogel Substances 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- -1 formaldehyde, benzene series Chemical class 0.000 description 3
- 239000011159 matrix material Substances 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 150000002894 organic compounds Chemical class 0.000 description 3
- 239000011148 porous material Substances 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- 239000004965 Silica aerogel Substances 0.000 description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 239000002156 adsorbate Substances 0.000 description 2
- 238000003915 air pollution Methods 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 230000000593 degrading effect Effects 0.000 description 2
- 125000000524 functional group Chemical group 0.000 description 2
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 238000005070 sampling Methods 0.000 description 2
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 description 2
- 238000007669 thermal treatment Methods 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- 239000011701 zinc Substances 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- 206010052613 Allergic bronchitis Diseases 0.000 description 1
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- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000000844 anti-bacterial effect Effects 0.000 description 1
- 208000006673 asthma Diseases 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000000498 ball milling Methods 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000005034 decoration Methods 0.000 description 1
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- 210000002249 digestive system Anatomy 0.000 description 1
- 239000004205 dimethyl polysiloxane Substances 0.000 description 1
- 201000010099 disease Diseases 0.000 description 1
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
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- 238000005469 granulation Methods 0.000 description 1
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- 230000036541 health Effects 0.000 description 1
- 238000003837 high-temperature calcination Methods 0.000 description 1
- 229920003088 hydroxypropyl methyl cellulose Polymers 0.000 description 1
- 239000001866 hydroxypropyl methyl cellulose Substances 0.000 description 1
- 235000010979 hydroxypropyl methyl cellulose Nutrition 0.000 description 1
- UFVKGYZPFZQRLF-UHFFFAOYSA-N hydroxypropyl methyl cellulose Chemical compound OC1C(O)C(OC)OC(CO)C1OC1C(O)C(O)C(OC2C(C(O)C(OC3C(C(O)C(O)C(CO)O3)O)C(CO)O2)O)C(CO)O1 UFVKGYZPFZQRLF-UHFFFAOYSA-N 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
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- 230000002045 lasting effect Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 210000004185 liver Anatomy 0.000 description 1
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 244000005700 microbiome Species 0.000 description 1
- 210000004877 mucosa Anatomy 0.000 description 1
- 210000000653 nervous system Anatomy 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
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- 238000011056 performance test Methods 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 1
- 239000006187 pill Substances 0.000 description 1
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- 229910001961 silver nitrate Inorganic materials 0.000 description 1
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- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 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
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
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- 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
- B01J23/70—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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- 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
- B01J35/39—Photocatalytic properties
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
- B01J37/084—Decomposition of carbon-containing compounds into carbon
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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
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
- B01J37/086—Decomposition of an organometallic compound, a metal complex or a metal salt of a carboxylic acid
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2255/00—Catalysts
- B01D2255/80—Type of catalytic reaction
- B01D2255/802—Photocatalytic
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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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Abstract
The invention belongs to the technical field of air purification, and particularly relates to a formaldehyde adsorbent for air purification and a preparation method and application thereof. The preparation method comprises the following steps: preparing phenolic resin ethanol solution, carrying out thermal polymerization and carbonization to obtain mesoporous carbon containing manganese and copper, and then carrying out oxidation treatment to obtain oxidation-treated mesoporous carbon; dissolving a cobalt source in deionized water, adding oxidized mesoporous carbon, uniformly stirring to obtain a mixture solution, adding 2-methylimidazole, iron salt and zinc salt into the mixture solution, stirring, filtering, washing, drying, and roasting in an inert atmosphere to obtain the methanol adsorbent. The formaldehyde adsorbent prepared by the invention has excellent adsorption and removal capacity on formaldehyde, and can oxidize the formaldehyde under the illumination condition, so that the formaldehyde in the air is effectively removed.
Description
Technical Field
The invention belongs to the technical field of air purification. More particularly, relates to a formaldehyde adsorbent for air purification and a preparation method and application thereof.
Background
Air pollution, especially indoor air pollution, poses serious harm to human bodies, and 60% of human diseases are reported to be caused by air pollution. The use of interior decoration, daily chemicals and human activities produce a large amount of pollutants, such as formaldehyde, benzene series, ammonia, etc. Formaldehyde is one of volatile organic compounds, and has strong stimulating effects on eye mucosa, nose and upper respiratory tract, and can cause allergic asthma and bronchitis, and in addition, formaldehyde has toxicity on the nervous system, liver, kidney and digestive system of human body. Eliminating formaldehyde pollution, purifying indoor air and being very important to human health.
The existing indoor air purification mainly adopts filtration and adsorption. The filtration mainly removes suspended matters in the air, such as dust, smoke and the like. Volatile Organic Compounds (VOC) in the air can be removed only by adsorption, but the adsorption only transfers the organic compounds in the air to the adsorbent and does not eliminate the organic compounds, and the adsorption performance is reduced along with the increase of the adsorption quantity, and finally the volatile organic compounds tend to be saturated and lose the air purification capacity. The photocatalysis can eliminate pollutants in the air, particularly can effectively degrade volatile organic compounds in the air, is a new air purification method developed in recent years, and the reaction is carried out at normal temperature and normal pressure, so that the organic compounds can be degraded into water and carbon dioxide, and secondary pollution can not be generated.
The activated carbon has the characteristics of large specific surface area, high adsorption rate, moderate pore size distribution and the like, and has remarkable advantages in the aspects of adsorbing and separating formaldehyde pollutants. According to different adsorption modes, activated carbon adsorption is divided into physical adsorption and chemical adsorption. In the physical adsorption process, the gradient distribution of the pore diameters determines the adsorption capacity and the adsorption rate, the macropores and the mesopores play a role in conveying formaldehyde molecules, the micropores have huge specific surface area and can provide enough stay places for pollutants, and the surfaces of the activated carbon adsorb the formaldehyde molecules by utilizing Van der Waals force generated under the action of asymmetric dipole moment. The chemical adsorption is that functional groups such as carboxyl, phenolic hydroxyl and the like of the activated carbon and formaldehyde adsorbate molecules are subjected to chemical reaction, so that the adsorption is stable and irreversible. As known from the physical adsorption and chemical adsorption processes of activated carbon, the pore size distribution and surface functional groups of activated carbon are very important for the adsorbate adsorption process.
CN114315236A discloses a method for preparing porous block aerogel for adsorbing and degrading VOCs gas by 3D printing technology. Uniformly mixing isopropanol, polydimethylsiloxane and hydroxypropyl methyl cellulose, adding silicon dioxide aerogel powder and titanium dioxide photocatalytic powder, and preparing 3D printing slurry by ball milling and mixing; then preparing the material into a macroscopic porous 3D printing aerogel sample with a specific structure by using a direct-writing 3D printer; then aging at normal temperature, and drying at proper temperature to remove organic solvent and further crosslink and solidify the binder to provide certain mechanical strength; and finally, carrying out heat treatment on the mixture in an electric furnace to obtain the 3D printing silica aerogel for absorbing and degrading the VOCs. The adsorption performance of the 3D printing silica aerogel on VOCs represented by formaldehyde and toluene is higher than that of commercial activated carbon by more than 20%, the absorption rate can reach 100%, and the degradation rate can reach more than 25%.
CN113181767A discloses a capsule type slow-release formaldehyde scavenger and a preparation process thereof, belonging to the technical field of formaldehyde scavenging, comprising a slow-release carrier pill core and a coating capsule, which are prepared from the following raw materials in parts by mass: 40-70 parts of active carbon base material, 30-60 parts of titanium dioxide base material, 5-10 parts of forming material, 2-20 parts of slow release material, 1-5 parts of plasticizer and 0.5-1.5 parts of anti-sticking agent, wherein the capsule coated with the thin coat is a polytetrafluoroethylene breathable waterproof thin coat, and the preparation process comprises the steps of matrix preparation, material mixing, granulation, slow release liquid preparation and coating. Through mixing titanium dioxide oxide in the active carbon matrix, fuse the back with active carbon and forming material and slow release material, the slow release capsule can carry out lasting absorption purification to formaldehyde under photocatalysis, and the surface film can completely cut off outside steam and soak, improves slowly-releasing efficiency, is showing extension coating standing time, satisfies the continuous purification ability to formaldehyde.
CN113101961A discloses a load Ag/C3N4Active carbon composite material of nano particles, melamine and silver nitrate are mixed and pyrolyzed to prepare Ag/g-C3N4Nanoparticles and thenCompounding with porous active carbon material to obtain Ag/C load 3N4The active carbon composite material of nano particles takes porous active carbon as a carrier and uniformly loads Ag/g-C3N4Nanoparticles of Ag/g-C3N4The nanoparticles have excellent photochemical activity, can generate more photogenerated carriers under light irradiation, and g-C3N4The Ag doped with the matrix has excellent conductivity, and can promote the transfer of photogenerated electrons, promote the separation of the photogenerated electrons and holes and ensure that Ag/g-C3N4The nano particles show better photocatalytic activity, and have good functions of adsorbing and photodegrading formaldehyde and excellent photocatalytic antibacterial activity on bacteria and microorganisms such as escherichia coli by being combined with the porous activated carbon.
CN111514883A discloses a carbon-based catalyst for decomposing indoor formaldehyde at room temperature and a preparation method thereof, which takes molded active carbon as a carrier, uses equal volume of impregnation to load a catalytic component, and obtains a formaldehyde elimination catalyst after high-temperature calcination. The carbon-based catalyst can efficiently purify formaldehyde at room temperature, the prepared titanium dioxide-containing catalyst has the performance of removing formaldehyde by photocatalysis and catalytic oxidation, and the formaldehyde purification efficiency is improved by combining the adsorption effect of activated carbon, the oxidation effect of manganese oxide and the photocatalysis effect of titanium dioxide. And the preparation process does not use noble metals, has the characteristics of high efficiency and environmental protection, and simultaneously uses the molded active carbon to purify formaldehyde, thereby being convenient for recycling and having no secondary pollution.
In view of the above, although the prior art can effectively remove formaldehyde by combining an adsorbent with an oxidant or a photocatalyst, the above adsorbent is still not strong enough in treatment capacity and has a long removal period for low-concentration formaldehyde, and thus there is an urgent need to develop a new formaldehyde adsorbent having excellent removal capacity for formaldehyde.
Disclosure of Invention
The invention aims to solve the technical problems of overcoming the defects and shortcomings in the prior art and provides a formaldehyde adsorbent for air purification and a preparation method and application thereof. The preparation method comprises the following steps: preparing phenolic resin ethanol solution, carrying out thermal polymerization and carbonization to obtain mesoporous carbon containing manganese and copper, and then carrying out oxidation treatment to obtain oxidized mesoporous carbon; dissolving a cobalt source in deionized water, adding oxidized mesoporous carbon, uniformly stirring to obtain a mixture solution, adding 2-methylimidazole, iron salt and zinc salt into the mixture solution, stirring, filtering, washing, drying, and roasting in an inert atmosphere to obtain the methanol adsorbent. The formaldehyde adsorbent prepared by the invention has excellent adsorption and removal capacity on formaldehyde, and can oxidize the formaldehyde under the illumination condition, thereby effectively removing the formaldehyde in the air.
The invention aims to provide a preparation method of a formaldehyde adsorbent for air purification.
The invention also aims to provide a formaldehyde adsorbent for air purification and application thereof.
The above purpose of the invention is realized by the following technical scheme:
a method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving phenol and formaldehyde in an alkaline solution, stirring uniformly at a certain temperature, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture at a certain temperature under a vacuum condition, and dissolving the obtained phenolic resin in ethanol to prepare a phenolic resin ethanol solution; dissolving the triblock copolymer, manganese salt and copper salt in a phenolic resin mixed solution, evaporating at room temperature, and performing thermal polymerization to obtain a precursor; roasting and carbonizing the precursor to obtain a mesoporous carbon material;
(2) adding the mesoporous carbon obtained in the step (1) into an oxidant solution for oxidation treatment, and then filtering and washing to obtain oxidized mesoporous carbon;
(3) dissolving a cobalt source in deionized water, adding the mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, adding 2-methylimidazole, iron salt and zinc salt into the mixture solution, stirring, filtering, washing, drying, and roasting in an inert atmosphere to obtain the methanol adsorbent.
Preferably, in the step (1), the stirring temperature is 50-70 ℃; the temperature of the vacuum is 80-100 ℃, and the concentration of the phenolic resin ethanol solution is 20-30 wt%.
Preferably, in the step (1), the temperature of the thermal polymerization is 70-90 ℃, and the time of the thermal polymerization is 16-24 h; the roasting condition is that the temperature is raised to 750-850 ℃ at the heating rate of 4-8 ℃/min under inert gas for roasting carbonization, and the temperature is kept for 2-5 h.
Preferably, in step (1), the triblock copolymer is at least one of P123, F127; the alkaline solution is at least one of sodium hydroxide solution and potassium hydroxide solution; the inert gas is one of helium and argon; the manganese salt is at least one of manganese nitrate, manganese acetate and manganese chloride, and the copper salt is at least one of copper nitrate, copper acetate and copper chloride.
Preferably, in step (1), the molar ratio of phenol to formaldehyde is 1: 2-4; the ratio of the phenol to the triblock copolymer to the manganese salt to the copper salt is 10-14 mmol: 1 g: 0.2-0.4 mmol: 0.2 to 0.4 mmol.
Preferably, in the step (2), the oxidant is potassium permanganate or hydrogen peroxide, and the oxidation treatment condition is that the potassium permanganate or hydrogen peroxide is treated in 2mol/L potassium permanganate or hydrogen peroxide for 0.5-1.5 h.
Preferably, in the step (3), the stirring condition is that the mixture is stirred for 16-22 hours at the temperature of 20-30 ℃; the drying is drying treatment at 80-120 ℃ for 10-14 h; the calcination temperature is 450-550 ℃, and the treatment is carried out for 2-4 h; the ratio of the mesoporous carbon to the cobalt source is 1 g: 0.01-0.03 mol, wherein the molar ratio of the cobalt source to the 2-methylimidazole is 1: 4-8; the molar ratio of the cobalt source to the iron salt to the zinc salt is 1: 0.02-0.06.
Preferably, in the step (3), the inert atmosphere is one of nitrogen, argon and helium; the cobalt salt is at least one of cobalt nitrate, cobalt acetate and cobalt chloride, the ferric salt is at least one of ferric nitrate, ferric acetate and ferric chloride, and the zinc salt is at least one of zinc acetate, zinc chloride and zinc nitrate.
The formaldehyde adsorbent for air purification is prepared based on the preparation method of the formaldehyde adsorbent for air purification.
The application of the formaldehyde adsorbent for air purification is characterized in that the formaldehyde adsorbent is used for purifying formaldehyde in air.
The invention has the following beneficial effects:
(1) the modified mesoporous carbon material has excellent adsorption capacity on formaldehyde, can effectively remove the adsorbed formaldehyde due to the existence of metal, and further has excellent purification capacity on formaldehyde.
(2) The mesoporous carbon modified by manganese and copper can obviously modify the adsorption capacity of the mesoporous carbon, and has excellent catalytic oxidation capacity on formaldehyde due to the existence of manganese and copper.
(3) By oxidizing the mesoporous carbon, oxygen-containing groups on the surface of the mesoporous carbon can be increased, which is beneficial to the adsorption of cobalt, and further improves the dispersibility of the cobalt and the purification capacity of formaldehyde.
(4) Iron and zinc are added in the prepared metal framework, and the generated metal oxide formaldehyde has excellent photocatalytic degradation capability after modification and carbonization of the iron and the zinc, so that the formaldehyde purification capability is further improved.
Detailed Description
The present invention will be further described with reference to the following specific examples, which are not intended to limit the invention in any manner. The reagents, methods and apparatus employed in the present invention are conventional in the art, except as otherwise indicated.
Unless otherwise indicated, reagents and materials used in the following examples are commercially available.
Example 1
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL0.6mol/L sodium hydroxide solution, uniformly stirring at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture under the vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% phenolic resin ethanol solution; dissolving 1g P123, 0.3mmol of manganese nitrate and 0.3mmol of copper nitrate in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out heat treatment at the temperature for 20 hours to obtain a precursor; heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas for roasting and carbonizing, and preserving heat for 4 hours to obtain a mesoporous carbon material;
(2) Adding the mesoporous carbon material obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution for treatment for 1 h; then filtering and washing to obtain oxidation-treated mesoporous carbon;
(3) dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, then adding 0.12mol of 2-methylimidazole, 0.6mmol of ferric nitrate and 0.6mmol of zinc nitrate into the mixture solution, stirring for 20h at 25 ℃, filtering, washing, drying for 12h at 100 ℃, and then roasting for 3h at 500 ℃ under nitrogen to obtain the methanol adsorbent.
Example 2
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 14mmol of phenol and 56mmol of formaldehyde in 10ml of 0.7mol/L potassium hydroxide solution, stirring uniformly at 70 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing water under the vacuum condition of 100 ℃, dissolving the obtained phenolic resin in ethanol to prepare 30 wt% phenolic resin ethanol solution; dissolving 1g F127, 0.4mmol of manganese chloride and 0.2mmol of copper acetate in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 90 ℃, and carrying out heat treatment at the temperature for 16h to obtain a precursor; and heating the precursor to 850 ℃ at the heating rate of 8 ℃/min under inert gas, roasting, carbonizing, and preserving heat for 2 hours to obtain the mesoporous carbon material.
(2) Adding the mesoporous carbon obtained in the step (1) into 50mL of 2mol/L hydrogen peroxide solution for treatment for 1.5 h; then filtering and washing to obtain oxidized mesoporous carbon;
(3) dissolving 0.03mol of cobalt chloride in 10mL of deionized water, adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, adding 0.24mol of 2-methylimidazole, 1.8mmol of ferric chloride and 0.6mmol of zinc acetate into the mixture solution, stirring at 30 ℃ for 16h, filtering, washing, drying at 120 ℃ for 10h, and roasting at 550 ℃ under argon for 2h to obtain the methanol adsorbent.
Example 3
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 10mmol of phenol and 20mmol of formaldehyde in 10mL0.5mol/L sodium hydroxide solution, stirring uniformly at 50 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing water under the vacuum condition of 80 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 20 wt% phenolic resin ethanol solution; dissolving 1g P123, 0.2mmol of manganese acetate and 0.4mmol of copper chloride in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 70 ℃, and carrying out heat treatment at the temperature for 24 hours to obtain a precursor; and heating the precursor to 750 ℃ at the heating rate of 4 ℃/min under helium gas, roasting, carbonizing, and preserving heat for 5 hours to obtain the mesoporous carbon material.
(2) Adding the mesoporous carbon obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution, and treating for 0.5-1.5 h; then filtering and washing to obtain oxidized mesoporous carbon;
(3) dissolving 0.01mol of cobalt acetate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, then adding 0.04mol of 2-methylimidazole, 0.2mmol of iron acetate and 0.6mmol of zinc chloride into the mixture solution, stirring at 20 ℃ for 22h, filtering, washing, drying at 80 ℃ for 14h, and then roasting at 450 ℃ for 4h under the atmosphere of helium gas to obtain the methanol adsorbent.
Comparative example 1
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL0.6mol/L sodium hydroxide solution, uniformly stirring at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture under the vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% phenolic resin ethanol solution; dissolving 1g P123 and 0.6mmol of manganese nitrate in the phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out thermal treatment at the temperature for 20h to obtain a precursor; heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas for roasting and carbonizing, and preserving heat for 4 hours to obtain a mesoporous carbon material;
(2) Adding the mesoporous carbon material obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution for treatment for 1 h; then filtering and washing to obtain oxidized mesoporous carbon;
(3) dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, then adding 0.12mol of 2-methylimidazole, 0.6mmol of ferric nitrate and 0.6mmol of zinc nitrate into the mixture solution, stirring for 20h at 25 ℃, filtering, washing, drying for 12h at 100 ℃, and then roasting for 3h at 500 ℃ under nitrogen to obtain the methanol adsorbent.
Comparative example 2
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL0.6mol/L sodium hydroxide solution, uniformly stirring at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture under the vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% phenolic resin ethanol solution; dissolving 1g P123 and 0.6mmol of copper nitrate in the phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out thermal treatment at the temperature for 20h to obtain a precursor; heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas for roasting and carbonizing, and preserving heat for 4 hours to obtain a mesoporous carbon material;
(2) Adding the mesoporous carbon material obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution for treatment for 1 h; then filtering and washing to obtain oxidation-treated mesoporous carbon;
(3) dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, then adding 0.12mol of 2-methylimidazole, 0.6mmol of ferric nitrate and 0.6mmol of zinc nitrate into the mixture solution, stirring for 20h at 25 ℃, filtering, washing, drying for 12h at 100 ℃, and then roasting for 3h at 500 ℃ under nitrogen to obtain the methanol adsorbent.
Comparative example 3
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL of 0.6mol/L sodium hydroxide solution, stirring uniformly at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture under a vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% of phenolic resin ethanol solution; dissolving 1g P123, 0.3mmol of manganese nitrate and 0.3mmol of copper nitrate in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out heat treatment at the temperature for 20 hours to obtain a precursor; heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas for roasting and carbonizing, and preserving heat for 4 hours to obtain a mesoporous carbon material;
(2) Adding the mesoporous carbon material obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution for treatment for 1 h; then filtering and washing to obtain oxidation-treated mesoporous carbon;
(3) dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, then adding 0.12mol of 2-methylimidazole and 1.2mmol of ferric nitrate into the mixture solution, stirring for 20h at 25 ℃, filtering, washing, drying for 12h at 100 ℃, and then roasting for 3h at 500 ℃ under nitrogen to obtain the methanol adsorbent.
Comparative example 4
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL of 0.6mol/L sodium hydroxide solution, stirring uniformly at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture under a vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% of phenolic resin ethanol solution; dissolving 1g P123, 0.3mmol of manganese nitrate and 0.3mmol of copper nitrate in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out heat treatment at the temperature for 20 hours to obtain a precursor; and heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas, roasting, carbonizing, and preserving heat for 4 hours to obtain the mesoporous carbon material.
(2) Adding the mesoporous carbon material obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution for treatment for 1 h; then filtering and washing to obtain oxidation-treated mesoporous carbon;
(3) dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, then adding 0.12mol of 2-methylimidazole and 1.2mmol of zinc nitrate into the mixture solution, stirring for 20h at 25 ℃, filtering, washing, drying for 12h at 100 ℃, and then roasting for 3h at 500 ℃ under nitrogen to obtain the methanol adsorbent.
Comparative example 5
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL of 0.6mol/L sodium hydroxide solution, uniformly stirring at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing water under the vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% of phenolic resin ethanol solution; dissolving 1g P123, 0.3mmol of manganese nitrate and 0.3mmol of copper nitrate in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out heat treatment at the temperature for 20 hours to obtain a precursor; heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas for roasting and carbonizing, and preserving heat for 4 hours to obtain a mesoporous carbon material;
(2) Dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, then adding 1g of mesoporous carbon obtained in the step (1), uniformly stirring to obtain a mixture solution, then adding 0.12mol of 2-methylimidazole, 0.6mmol of ferric nitrate and 0.6mmol of zinc nitrate into the mixture solution, stirring for 20h at 25 ℃, filtering, washing, drying for 12h at 100 ℃, and then roasting for 3h at 500 ℃ under nitrogen to obtain the methanol adsorbent.
Comparative example 6
A method for preparing a formaldehyde adsorbent for air purification, the method comprising the steps of:
(1) preparation of mesoporous carbon
Dissolving 12mmol of phenol and 36mmol of formaldehyde in 10mL of 0.6mol/L sodium hydroxide solution, stirring uniformly at 60 ℃, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture under a vacuum condition of 90 ℃, and dissolving the obtained phenolic resin in ethanol to prepare 35 wt% of phenolic resin ethanol solution; dissolving 1g P123, 0.3mmol of manganese nitrate and 0.3mmol of copper nitrate in a phenolic resin mixed solution, evaporating at room temperature, carrying out thermal polymerization at 80 ℃, and carrying out heat treatment at the temperature for 20 hours to obtain a precursor; heating the precursor to 800 ℃ at the heating rate of 6 ℃/min under helium gas for roasting and carbonizing, and preserving heat for 4 hours to obtain a mesoporous carbon material;
(2) Adding the mesoporous carbon material obtained in the step (1) into 50mL of 2mol/L potassium permanganate solution for treatment for 1 h; then filtering and washing to obtain oxidation-treated mesoporous carbon;
(3) dissolving 0.02mol of cobalt nitrate in 10mL of deionized water, uniformly stirring to obtain a mixture solution, adding 0.12mol of 2-methylimidazole, 0.6mmol of ferric nitrate and 0.6mmol of zinc nitrate into the mixture solution, stirring at 25 ℃ for 20 hours, then adding 1g of mesoporous carbon obtained in the step (2), continuing stirring for 0.5min, filtering, washing, drying at 100 ℃ for 12 hours, and then roasting at 500 ℃ under nitrogen for 3 hours to obtain the methanol adsorbent.
The formaldehyde adsorbents for air purification of examples 1 to 3 and comparative examples 1 to 6 were subjected to the adsorption and degradation experiments of formaldehyde, and the specific test results are shown in table 1.
Adsorption test of formaldehyde: and (3) putting 20g of sample into a closed container, wherein the volume of the container is 1000L, introducing 100ppm of formaldehyde as VOCs to be detected, extracting gas in the closed environment through a sampling needle, detecting the initial concentration of toluene in the container by using an acetylacetone method, and checking the removal rate at 60 min.
Degradation test of formaldehyde: putting 20g of sample into a closed container, wherein the volume of the container is 1000L, introducing 100ppm of formaldehyde as VOCs to be detected, extracting gas in the closed environment through a sampling needle, detecting the initial concentration of toluene in the container by using an acetylacetone method, then introducing 100ppm of formaldehyde gas into the closed environment for multiple times until the concentration of the VOCs in the closed environment is equal to the determined initial concentration and is still unchanged after 60min, opening 300W xenon lamp light for degradation performance test, and determining the formaldehyde degradation rate at 30 min.
TABLE 1
As can be seen from Table 1, the formaldehyde adsorbent for air purification prepared in the present application has advantageous adsorption and removal ability to formaldehyde, and it can be confirmed by comparing examples 1 to 3 with comparative examples 1 to 6 that the components of the present invention have a mutual coordination effect and it is the mutual coordination effect between the components that promotes the improvement of the adsorption ability and the degradation ability of the formaldehyde adsorbent.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such modifications are intended to be included in the scope of the present invention.
Claims (10)
1. A preparation method of formaldehyde adsorbent for air purification is characterized in that: the preparation method comprises the following steps:
(1) preparation of mesoporous carbon
Dissolving phenol and formaldehyde in an alkaline solution, stirring uniformly at a certain temperature, cooling to room temperature, adjusting the solution to be neutral by hydrochloric acid, removing moisture at a certain temperature under a vacuum condition, and dissolving the obtained phenolic resin in ethanol to prepare a phenolic resin ethanol solution; dissolving the triblock copolymer, manganese salt and copper salt in a phenolic resin mixed solution, evaporating at room temperature, and performing thermal polymerization to obtain a precursor; roasting and carbonizing the precursor to obtain a mesoporous carbon material;
(2) Adding the mesoporous carbon material obtained in the step (1) into an oxidant solution for oxidation treatment, and then filtering and washing to obtain oxidation-treated mesoporous carbon;
(3) dissolving a cobalt source in deionized water, adding the mesoporous carbon obtained in the step (2), uniformly stirring to obtain a mixture solution, adding 2-methylimidazole, iron salt and zinc salt into the mixture solution, stirring, filtering, washing, drying, and roasting in an inert atmosphere to obtain the methanol adsorbent.
2. The method for preparing the formaldehyde adsorbent for air purification according to claim 1, wherein: in the step (1), the stirring temperature is 50-70 ℃; the temperature of the vacuum is 80-100 ℃, and the concentration of the phenolic resin ethanol solution is 20-30 wt%.
3. The method for preparing the formaldehyde adsorbent for air purification according to claim 1, wherein: in the step (1), the temperature of the thermal polymerization is 70-90 ℃, and the time of the thermal polymerization is 16-24 h; the roasting condition is that the temperature is raised to 750-850 ℃ at the heating rate of 4-8 ℃/min under inert gas for roasting carbonization, and the temperature is kept for 2-5 h.
4. The method for preparing the formaldehyde adsorbent for air purification according to claim 1, wherein: in the step (1), the triblock copolymer is at least one of P123 and F127; the alkaline solution is at least one of sodium hydroxide solution and potassium hydroxide solution; the inert gas is one of helium and argon; the manganese salt is at least one of manganese nitrate, manganese acetate and manganese chloride, and the copper salt is at least one of copper nitrate, copper acetate and copper chloride.
5. The method for preparing a formaldehyde adsorbent for air purification according to any one of claims 1 to 4, wherein: in step (1), the molar ratio of phenol to formaldehyde is 1: 2-4; the ratio of the phenol to the triblock copolymer to the manganese salt to the copper salt is 10-14 mmol: 1 g: 0.2-0.4 mmol: 0.2 to 0.4 mmol.
6. The method for preparing the formaldehyde adsorbent for air purification according to claim 1, wherein: in the step (2), the oxidant is potassium permanganate or hydrogen peroxide, and the oxidation treatment condition is to treat the mixture in 2mol/L potassium permanganate or hydrogen peroxide for 0.5-1.5 h.
7. The method for preparing the formaldehyde adsorbent for air purification according to claim 1, wherein: in the step (3), stirring for 16-22 h at 20-30 ℃; the drying is drying treatment at 80-120 ℃ for 10-14 h; the calcination temperature is 450-550 ℃, and the treatment is carried out for 2-4 h; the ratio of the mesoporous carbon to the cobalt source is 1 g: 0.01-0.03 mol, wherein the molar ratio of the cobalt source to the 2-methylimidazole is 1: 4-8; the molar ratio of the cobalt source to the ferric salt to the zinc salt is 1: 0.02-0.06.
8. The method for preparing the formaldehyde adsorbent for air purification according to claim 1, wherein: in the step (3), the inert atmosphere is one of nitrogen, argon and helium; the cobalt salt is at least one of cobalt nitrate, cobalt acetate and cobalt chloride, the iron salt is at least one of ferric nitrate, ferric acetate and ferric chloride, and the zinc salt is at least one of zinc acetate, zinc chloride and zinc nitrate.
9. A formaldehyde adsorbent for air purification prepared by the method for preparing a formaldehyde adsorbent for air purification according to any one of claims 1 to 8.
10. The use of the formaldehyde adsorbent for air purification according to claim 9, wherein the formaldehyde adsorbent is used for purifying formaldehyde in air.
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