CN108654639A - Catalyst and its preparation method and application for formaldehyde normal temperature oxidation - Google Patents
Catalyst and its preparation method and application for formaldehyde normal temperature oxidation Download PDFInfo
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- CN108654639A CN108654639A CN201710209703.9A CN201710209703A CN108654639A CN 108654639 A CN108654639 A CN 108654639A CN 201710209703 A CN201710209703 A CN 201710209703A CN 108654639 A CN108654639 A CN 108654639A
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- metal source
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- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 title claims abstract description 149
- 239000003054 catalyst Substances 0.000 title claims abstract description 52
- 230000003647 oxidation Effects 0.000 title claims abstract description 24
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 24
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 43
- 229910000510 noble metal Inorganic materials 0.000 claims abstract description 17
- 239000000725 suspension Substances 0.000 claims abstract description 17
- 238000003756 stirring Methods 0.000 claims abstract description 14
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 13
- 150000003624 transition metals Chemical class 0.000 claims abstract description 13
- 230000032683 aging Effects 0.000 claims abstract description 10
- 239000002245 particle Substances 0.000 claims abstract description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 9
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 8
- 230000009467 reduction Effects 0.000 claims abstract description 8
- 239000007864 aqueous solution Substances 0.000 claims abstract description 7
- 239000008367 deionised water Substances 0.000 claims abstract description 7
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 7
- 239000011259 mixed solution Substances 0.000 claims abstract description 6
- 230000001376 precipitating effect Effects 0.000 claims abstract description 6
- 238000010438 heat treatment Methods 0.000 claims abstract description 5
- 238000001354 calcination Methods 0.000 claims abstract description 3
- 238000005406 washing Methods 0.000 claims abstract description 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 32
- 239000007789 gas Substances 0.000 claims description 24
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 20
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims description 20
- 229910052697 platinum Inorganic materials 0.000 claims description 14
- 229910052751 metal Inorganic materials 0.000 claims description 13
- 239000002184 metal Substances 0.000 claims description 13
- 230000000694 effects Effects 0.000 claims description 10
- 229910000029 sodium carbonate Inorganic materials 0.000 claims description 10
- 229910052742 iron Inorganic materials 0.000 claims description 8
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 7
- 229910052799 carbon Inorganic materials 0.000 claims description 7
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 6
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 6
- WQYVRQLZKVEZGA-UHFFFAOYSA-N hypochlorite Chemical compound Cl[O-] WQYVRQLZKVEZGA-UHFFFAOYSA-N 0.000 claims description 6
- 238000001035 drying Methods 0.000 claims description 5
- ATRRKUHOCOJYRX-UHFFFAOYSA-N Ammonium bicarbonate Chemical compound [NH4+].OC([O-])=O ATRRKUHOCOJYRX-UHFFFAOYSA-N 0.000 claims description 4
- 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-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 4
- 229910002651 NO3 Inorganic materials 0.000 claims description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 4
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 4
- 239000001099 ammonium carbonate Substances 0.000 claims description 4
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 4
- 229910052737 gold Inorganic materials 0.000 claims description 4
- 239000010931 gold Substances 0.000 claims description 4
- 239000011261 inert gas Substances 0.000 claims description 4
- 150000003891 oxalate salts Chemical class 0.000 claims description 4
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 claims description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 3
- 229910052739 hydrogen Inorganic materials 0.000 claims description 3
- 239000001257 hydrogen Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 229910052763 palladium Inorganic materials 0.000 claims description 3
- 238000011084 recovery Methods 0.000 claims description 3
- 229910000013 Ammonium bicarbonate Inorganic materials 0.000 claims description 2
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 2
- 229910052684 Cerium Inorganic materials 0.000 claims description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical group [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 2
- UIIMBOGNXHQVGW-UHFFFAOYSA-M Sodium bicarbonate Chemical compound [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 2
- 235000012538 ammonium bicarbonate Nutrition 0.000 claims description 2
- 235000012501 ammonium carbonate Nutrition 0.000 claims description 2
- 239000000908 ammonium hydroxide Substances 0.000 claims description 2
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 239000004202 carbamide Substances 0.000 claims description 2
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- 229910052802 copper Inorganic materials 0.000 claims description 2
- 239000010949 copper Substances 0.000 claims description 2
- 239000001307 helium Substances 0.000 claims description 2
- 229910052734 helium Inorganic materials 0.000 claims description 2
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 2
- 229910052759 nickel Inorganic materials 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 239000011148 porous material Substances 0.000 claims description 2
- 229910000027 potassium carbonate Inorganic materials 0.000 claims description 2
- 229910052709 silver Inorganic materials 0.000 claims description 2
- 239000004332 silver Substances 0.000 claims description 2
- 229910052719 titanium Inorganic materials 0.000 claims description 2
- 239000010936 titanium Substances 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052725 zinc Inorganic materials 0.000 claims description 2
- 239000011701 zinc Substances 0.000 claims description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims 1
- 229910002091 carbon monoxide Inorganic materials 0.000 claims 1
- 239000003610 charcoal Substances 0.000 claims 1
- 150000002431 hydrogen Chemical class 0.000 claims 1
- 238000004062 sedimentation Methods 0.000 claims 1
- 239000011734 sodium Substances 0.000 claims 1
- 229910052708 sodium Inorganic materials 0.000 claims 1
- 235000015424 sodium Nutrition 0.000 claims 1
- 239000000052 vinegar Substances 0.000 claims 1
- 235000021419 vinegar Nutrition 0.000 claims 1
- 230000003197 catalytic effect Effects 0.000 abstract description 8
- 239000000463 material Substances 0.000 abstract description 4
- 239000010953 base metal Substances 0.000 abstract description 2
- 235000019256 formaldehyde Nutrition 0.000 description 41
- 239000002253 acid Substances 0.000 description 17
- 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 description 16
- 238000006243 chemical reaction Methods 0.000 description 15
- 229930040373 Paraformaldehyde Natural products 0.000 description 12
- 238000000034 method Methods 0.000 description 12
- 229920002866 paraformaldehyde Polymers 0.000 description 12
- 238000004458 analytical method Methods 0.000 description 7
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- 230000008859 change Effects 0.000 description 6
- 239000002994 raw material Substances 0.000 description 5
- 239000008236 heating water Substances 0.000 description 4
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 4
- 239000007787 solid Substances 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- 239000001569 carbon dioxide Substances 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- 238000011156 evaluation Methods 0.000 description 3
- 231100000597 Sick building syndrome Toxicity 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 125000002485 formyl group Chemical class [H]C(*)=O 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- 239000013528 metallic particle Substances 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 230000001699 photocatalysis Effects 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 208000008842 sick building syndrome Diseases 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- UIIMBOGNXHQVGW-DEQYMQKBSA-M Sodium bicarbonate-14C Chemical compound [Na+].O[14C]([O-])=O UIIMBOGNXHQVGW-DEQYMQKBSA-M 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 231100000481 chemical toxicant Toxicity 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 201000010099 disease Diseases 0.000 description 1
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 description 1
- 235000013399 edible fruits Nutrition 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000008187 granular material Substances 0.000 description 1
- 231100000171 higher toxicity Toxicity 0.000 description 1
- QWPPOHNGKGFGJK-UHFFFAOYSA-N hypochlorous acid Chemical compound ClO QWPPOHNGKGFGJK-UHFFFAOYSA-N 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000001802 infusion Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 230000008520 organization Effects 0.000 description 1
- 238000006213 oxygenation reaction Methods 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 208000011580 syndromic disease Diseases 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
Classifications
-
- 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
- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
- B01J23/8906—Iron and noble metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2259/00—Type of treatment
- B01D2259/45—Gas separation or purification devices adapted for specific applications
- B01D2259/4508—Gas separation or purification devices adapted for specific applications for cleaning air in buildings
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Catalysts (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
Abstract
The present invention relates to a kind of preparation methods of the catalyst for formaldehyde normal temperature oxidation, which is characterized in that includes the following steps：A. excessive deionized water is added, noble metal source is fully dissolved with transition metal source, heating stirring within the temperature range of 40 DEG C 90 DEG C obtains mixed solution；B. 1 30 times of the activated carbon that addition is the noble metal source and transition metal source quality is added in the mixed solution, continues to stir, obtains suspension；C. the aqueous solution of alkaline precipitating agent is added drop-wise to constant rate of speed in the suspension, and aging；D. the suspension obtained by step c is filtered, washing to neutrality, and dry, obtains particle；E. at a temperature of 200 DEG C 400 DEG C, the particle is placed in calcining reduction under reducibility gas atmosphere.The present invention greatly reduces cost of material, while keeping preferable catalytic activity by adding base metal.
Description
Technical field
The present invention relates to catalyst fields, more particularly to are used for catalyst of formaldehyde normal temperature oxidation and preparation method thereof and answer
With.
Background technology
Formaldehyde is one of the pollutant of indoor most serious, has higher toxicity, in China's toxic chemical priority acccess control
It is in second on list, Ι class carcinogenic substances are determined as by the World Health Organization (WHO) and international cancer research institution (IARC).
According to statistics, after finishing in 1~6 month, up to 80% in formaldehyde rate room, even if finishing is after 3 years, exceeding standard rate is all still up to 50%
More than.The acquisition time of formaldehyde is 3~15 years in wood-based plate.As it can be seen that indoor formaldehyde will influence the health of people for a long time, such as
Sick Building syndrome (SBS), building association syndrome (BRI) etc..In addition, most human body diseases and room air
It pollutes related.
Currently, there are many kinds of the methods of removal formaldehyde, such as：Absorption method, plant purification method, air negative ion purifying skill
Art, chemical reaction method, photocatalytic method and catalytic oxidation.Wherein, plant purification processing formaldehyde is less efficient and time-consuming longer；
Chemical reagent consumption amount is big in chemical reaction method and can cause secondary pollution；Absorption method need to repeatedly replace sorbing material and presence
Phenomenon is desorbed；The modes such as photocatalysis, plasma technique need to provide additional luminous energy and electric energy.In comparison, it is catalyzed oxygen
Change method can convert formaldehyde to carbon dioxide and water, and removal efficiency is high, and without secondary pollution, and catalyst life is long, can weigh
Multiple to utilize, exploitation formaldehyde normal temperature oxidation catalyst is crucial.
Noble metal shows excellent low temperature active, especially metal platinum in PARA FORMALDEHYDE PRILLS(91,95) catalysis oxidation.Chinese patent
A kind of noble metal platinum is disclosed in CN104368335A or palladium is used for the method for preparing catalyst of catalysis oxidation formaldehyde, by your gold
Category loads on active carbon fiber felt, which can be by the formaldehyde through catalytic oxidation of low concentration at carbon dioxide and water, removal effect
Fruit is 89% or more.A kind of using titanium dioxide as carrier, platinum and Jin Shuan noble metals are disclosed in Chinese patent CN103586022A
For active component, using infusion process Supported Pt Nanoparticles component, deposition-precipitation method gold-supported component, which can be catalyzed oxygen at normal temperatures
Change formaldehyde, oxygenation efficiency is 95% or more.The bullion content of the above patent load is relatively high, and preparation method is more multiple
It is miscellaneous, limit the practical application of catalyst.
In addition, at present in the research of most formaldehyde normal temperature oxidation catalyst, the evaluation of catalyst activity is usually used
Be higher concentration formaldehyde, generally in 100ppm or more, but in real life, the content of formaldehyde in room air is then in
Lower level, generally in 1ppm or less.The formaldehyde removal difficulty of low concentration is larger, and steam, carbon dioxide in air
It is higher Deng in contrast concentration, also have an impact to catalyst activity.
Invention content
In order to overcome, the cost of material of existing formaldehyde catalyst is high, preparation process is complicated, room-temperature catalytic oxidation low concentration first
The low defect of aldehyde efficiency, the present invention provide a kind of preparation method of the catalyst for formaldehyde normal temperature oxidation, include the following steps：
A. excessive deionized water is added, noble metal source is fully dissolved with transition metal source, in 40 DEG C -90 DEG C of temperature model
Interior heating stirring is enclosed, mixed solution is obtained；
B. 1-30 times of the quality that addition is the noble metal source and transition metal source is added in the mixed solution
Activated carbon, continue to stir, obtain suspension；
C. the aqueous solution of alkaline precipitating agent is added drop-wise to constant rate of speed in the suspension, and aging；
D. the suspension obtained by step c is filtered, washing to neutrality, and dry, obtains particle；
E. at a temperature of 200 DEG C -400 DEG C, the particle is placed in calcining reduction under reducibility gas atmosphere.
Preferably, the noble metal source in step a can be the nitrate, chloride, hypochlorous acid of palladium, platinum, gold, silver etc.
Salt, acetate, oxalates or sulfate, concentration of aqueous solution are 1x 10-4-1x 10-3mol/L；The transition metal source can be with
For the nitrate of copper, iron, manganese, nickel, cobalt, cerium, titanium, zinc, vanadium etc., chloride, hypochlorite, acetate, oxalates or sulfate,
Its concentration of aqueous solution is 0.003-0.01mol/L.
Preferably, activated carbon described in step b is granular activated carbon, has pore structure, the mixing time of step b is 1-
12h。
Preferably, alkaline precipitating agent described in step c be sodium carbonate, sodium bicarbonate, potassium carbonate, saleratus, ammonium carbonate,
Ammonium hydrogen carbonate, sodium hydroxide, potassium hydroxide, ammonium hydroxide or urea；Alkaline precipitating agent and the noble metal source and the transition metal
The molar ratio of metal contained by source is 2:1~10:1, ageing time 0.5-3h.
Preferably, drying temperature described in step d is 60 DEG C -120 DEG C, drying time 1-24h.
Preferably, reducibility gas atmosphere described in step e includes that volume fraction is aoxidized in the hydrogen of 1-10% or one
Carbon, and the inert gas as balanced gas；In step e, recovery time 0.5-10h.
Preferably, the inert gas is helium, argon gas or nitrogen.
According to another aspect of the present invention, it is normal for formaldehyde according to the preparation of above-mentioned preparation method that the present invention also provides a kind of
The catalyst of temperature oxidation.
Preferably, the catalyst includes the activated carbon as carrier, and the noble metal as active component and transition gold
Belong to, wherein the grain size of the active component is 5-10nm.
According to another aspect of the present invention, the present invention also provides answering in the catalyst at normal temperatures oxidation of formaldehyde
With wherein a concentration of 0.1-1.0mg/m of the formaldehyde3, room temperature is 15 DEG C -25 DEG C.
Compared with prior art, the technical advantage of catalyst for formaldehyde normal temperature oxidation of the invention and preparation method thereof
It is mainly reflected in：
(1) by adding base metal, cost of material is greatly reduced, while keeping preferable catalytic activity；
(2) it is used in the embodiment of the present invention when carrying out activity rating to gained catalyst closer to actual conditions
Evaluation condition, the data obtained have more directive significance to the practical application of catalyst of the present invention.
Description of the drawings
Fig. 1 is the transmission electron microscope photo (TEM figures) of activated carbon supported platinum obtained and iron double metal catalyst.
Fig. 2 is activated carbon supported platinum obtained and iron double metal catalyst (Pt:Fe:AC=1:40:82) formaldehyde room temperature
Conversion rate curve.
Fig. 3 is activated carbon supported platinum obtained and iron double metal catalyst (Pt:Fe:AC=1:20:42) formaldehyde room temperature
Conversion rate curve.
Fig. 4 is activated carbon supported platinum obtained and iron double metal catalyst (Pt:Fe:AC=1:10:22) formaldehyde room temperature
Conversion rate curve.
Fig. 5 is the formaldehyde room temperature conversion rate curve of activated carbon supported platinum catalyst obtained.
Specific implementation mode
With reference to specific embodiment to the catalyst and preparation method thereof of the present invention for formaldehyde normal temperature oxidation
It is described further.Specific embodiment is that present invention be described in more detail, unrestricted protection scope of the present invention.It is all without departing substantially from
The change of present inventive concept or equivalent substitute are within the scope of the present invention.Unless stated otherwise, the embodiment of the present invention is adopted
Raw material is this field conventional selection.
Embodiment 1
(1) in deionized water by chloroplatinic acid (analysis is pure) and ferric nitrate (analysis is pure) dissolving, 70 DEG C of heating water baths, stirring
Uniformly, it is respectively 3.0x 10 to make the concentration of chloroplatinic acid and ferric nitrate-4mol·L-1With 1.2x 10-2mol·L-1；
(2) granular active carbon is added into above-mentioned solution, activated carbon addition is 5 times of above-mentioned chloroplatinic acid quality, after
Continuous stirring 1h；
(3) sodium carbonate liquor is gradually added dropwise to above-mentioned suspension, sodium carbonate is 2 with chloroplatinic acid molar ratio:1, it is added dropwise to complete
Aging 0.5h afterwards；
(4) above-mentioned suspension is filtered and is washed with deionized to neutrality, be placed in 60 DEG C of baking ovens dry 18h；
(5) by the dry solid particle completed in 5%H21h, 300 DEG C of reduction temperature are restored under/He atmosphere, TEM schemes such as
Shown in Fig. 1.Black spheric granules is metallic particles in figure, and cake mass is carrier active carbon, and metallic particles is distributed on carrier
Uniformly.
The activity rating of catalyst carries out in U-shaped reaction tube, and raw material formaldehyde gas is generated by gas generator, uses two
Platform methylene oxide detecting instrument detects the concentration of formaldehyde in entrance and exit gas respectively.The evaluation condition of catalyst is as follows：Catalyst sample
Product 100mg, gas flow 90mL/min, 20 DEG C, mass space velocity 54000mL/gh of temperature, formaldehyde inlet concentration 0.5ppm.Catalysis
The room-temperature catalytic oxidation performance of agent PARA FORMALDEHYDE PRILLS(91,95) is as shown in Figure 2.Chloroplatinic acid and ferric nitrate under the ratio catalyst obtained to first
Aldehyde conversion ratio is very low and unstable, average out to 25% or so.
Embodiment 2
(1) in deionized water by chloroplatinic acid (analysis is pure) and ferric nitrate (analysis is pure) dissolving, 70 DEG C of heating water baths, stirring
Uniformly, it is respectively 3.0x 10 to make the concentration of chloroplatinic acid and ferric nitrate-4mol·L-1With 6x 10-3mol·L-1；
(2) granular active carbon is added into above-mentioned solution, activated carbon addition is 5 times of above-mentioned source metal quality, after
Continuous stirring 1h；
(3) sodium carbonate liquor is gradually added dropwise to above-mentioned suspension, sodium carbonate is 2 with source metal molar ratio:1, it is added dropwise to complete
Aging 0.5h afterwards；
(4) above-mentioned suspension is filtered and is washed with deionized to neutrality, be placed in 60 DEG C of baking ovens dry 18h；
(5) by the dry solid particle completed in 5%H21h, 300 DEG C of reduction temperature are restored under/He atmosphere.
The activity rating of catalyst carries out in U-shaped reaction tube, and raw material formaldehyde gas is generated by gas generator, uses two
Platform methylene oxide detecting instrument detects the concentration of formaldehyde in entrance and exit gas respectively.Catalyst sample dosage 100mg, gas flow
90mL/min, 20 DEG C, mass space velocity 54000mL/gh of temperature, formaldehyde inlet concentration 0.5ppm.The room temperature of catalyst PARA FORMALDEHYDE PRILLS(91,95) is urged
Change oxidation susceptibility as shown in figure 3, chloroplatinic acid and ferric nitrate the catalyst PARA FORMALDEHYDE PRILLS(91,95) conversion ratio obtained under the ratio it is higher and compared with
Stablize, average out to 82% or so.
Embodiment 3
(1) in deionized water by chloroplatinic acid (analysis is pure) and ferric nitrate (analysis is pure) dissolving, 70 DEG C of heating water baths, stirring
Uniformly, it is respectively 3.0x 10 to make the concentration of chloroplatinic acid and ferric nitrate-4mol·L-1With 3x 10-3mol·L-1；
(2) granular active carbon is added into above-mentioned solution, activated carbon addition is 5 times of above-mentioned source metal quality, after
Continuous stirring 1h；
(3) sodium carbonate liquor is gradually added dropwise to above-mentioned suspension, sodium carbonate is 2 with source metal molar ratio:1, it is added dropwise to complete
Aging 0.5h afterwards；
(4) above-mentioned suspension is filtered and is washed with deionized to neutrality, be placed in 60 DEG C of baking ovens dry 18h；
(5) by the dry solid particle completed in 5%H21h, 300 DEG C of reduction temperature are restored under/He atmosphere.
The activity rating of catalyst carries out in U-shaped reaction tube, and raw material formaldehyde gas is generated by gas generator, uses two
Platform methylene oxide detecting instrument detects the concentration of formaldehyde in entrance and exit gas respectively.Catalyst sample dosage 100mg, gas flow
90mL/min, 20 DEG C, mass space velocity 54000mL/gh of temperature, formaldehyde inlet concentration 0.5ppm.The room temperature of catalyst PARA FORMALDEHYDE PRILLS(91,95) is urged
Change oxidation susceptibility as shown in figure 4, chloroplatinic acid and ferric nitrate the catalyst PARA FORMALDEHYDE PRILLS(91,95) conversion ratio obtained under the ratio are relatively low and not
Stablize, average out to 40% or so.
Embodiment 1,2 and 3 shows that the conversion ratio than regular meeting PARA FORMALDEHYDE PRILLS(91,95) of chloroplatinic acid and ferric nitrate has larger impact, specifically
For：With the reduction of Fe contents, the transformation efficiency of catalyst PARA FORMALDEHYDE PRILLS(91,95) first increases to be reduced afterwards, in the concentration of chloroplatinic acid and ferric nitrate
Respectively 3.0x 10-4mol·L-1With 6x 10-3mol·L-1When, the performance of catalyst is best.That is Fe and Pt has intermetallic
Synergistic effect：Suitable ratio is selected, catalyst PARA FORMALDEHYDE PRILLS(91,95) changing effect can be made best.
Embodiment 4
(1) in deionized water by chloroplatinic acid (analysis is pure) dissolving, 70 DEG C of heating water baths stir evenly, make chloroplatinic acid
A concentration of 3.0x 10-4mol·L-1；
(2) granular active carbon is added into above-mentioned solution, activated carbon addition is 5 times of above-mentioned chloroplatinic acid quality, after
Continuous stirring 1h；
(3) sodium carbonate liquor is gradually added dropwise to above-mentioned suspension, sodium carbonate is 2 with chloroplatinic acid molar ratio:1, it is added dropwise to complete
Aging 0.5h afterwards；
(4) above-mentioned suspension is filtered and is washed with deionized to neutrality, be placed in 60 DEG C of baking ovens dry 18h；
(5) by the dry solid particle completed in 5%H2Restore 1h under/He atmosphere, 300 DEG C of reduction temperature, formaldehyde
Room-temperature catalytic oxidation performance is as shown in Figure 5.
The activity rating of catalyst carries out in U-shaped reaction tube, and raw material formaldehyde gas is generated by gas generator, uses two
Platform methylene oxide detecting instrument detects the concentration of formaldehyde in entrance and exit gas respectively.Catalyst sample dosage 100mg, gas flow
90mL/min, 20 DEG C, mass space velocity 54000mL/gh of temperature, formaldehyde inlet concentration 0.5ppm.The room temperature of catalyst PARA FORMALDEHYDE PRILLS(91,95) is urged
Change oxidation susceptibility as shown in figure 5, the catalyst PARA FORMALDEHYDE PRILLS(91,95) conversion ratio made from monometallic platinum it is higher and relatively stablize, average out to 80%
Left and right.
Embodiment 4 is the contrast experiment carried out with embodiment 1,2,3, the results showed that, platinum and iron double metal catalyst can be with
Obtain PARA FORMALDEHYDE PRILLS(91,95) catalytic effect identical with monometallic platinum, you can with the expensive Pt of more cheap Fe substitutions, to reduce catalyst
Manufacturing cost.
It should be appreciated by those skilled in the art that above example step 1) can also use other suitable mode of heatings,
Heating temperature, such as selected in 40-90 DEG C.The additive amount of activated carbon can also be selected as in above example step 2)
Other multiples in 1-30 times of noble metal source and transition metal source, mixing time can be other suitable periods, such as 1-
It is arbitrarily selected in 12h.The molar ratio of noble metal source and the metal contained by transition metal source can be in above example step 3)
Other values, such as 2:1~10:1 is selected, and ageing time can be, such as 0.5-3h.It is done in above example step 4)
Dry temperature can select between such as 60-120 DEG C, and drying time can be selected between such as 1-24h.It is above to implement
Recovery time in example step 5) can select between 0.5-10h.
Several embodiments of the invention above described embodiment only expresses, the description thereof is more specific and detailed, but simultaneously
Cannot the limitation to the scope of the claims of the present invention therefore be interpreted as.It should be pointed out that for those of ordinary skill in the art
For, without departing from the inventive concept of the premise, various modifications and improvements can be made, these belong to the guarantor of the present invention
Protect range.Therefore, the protection domain of patent of the present invention should be determined by the appended claims.
Claims (10)
1. a kind of preparation method of catalyst for formaldehyde normal temperature oxidation, which is characterized in that include the following steps：
A. excessive deionized water is added, noble metal source is fully dissolved with transition metal source, within the temperature range of 40 DEG C -90 DEG C
Heating stirring obtains mixed solution；
B. the activity for 1-30 times of the quality that addition is the noble metal source and transition metal source is added in the mixed solution
Charcoal continues to stir, obtains suspension；
C. the aqueous solution of alkaline precipitating agent is added drop-wise to constant rate of speed in the suspension, and aging；
D. the suspension obtained by step c is filtered, washing to neutrality, and dry, obtains particle；
E. at a temperature of 200 DEG C -400 DEG C, the particle is placed in calcining reduction under reducibility gas atmosphere.
2. preparation method according to claim 1, which is characterized in that noble metal source described in step a be palladium, platinum, gold,
Nitrate, chloride, hypochlorite, acetate, oxalates or the sulfate of silver, concentration of aqueous solution 1x10-4-1x10- 3mol/L；The transition metal source is copper, iron, manganese, nickel, cobalt, cerium, titanium, zinc, the nitrate of vanadium, chloride, hypochlorite, vinegar
Hydrochlorate, oxalates or sulfate, concentration of aqueous solution 0.003-0.01mol/L.
3. preparation method according to claim 1, which is characterized in that activated carbon described in step b is granular activated carbon, tool
There is pore structure, the mixing time of step b is 1-12h.
4. preparation method according to claim 1, which is characterized in that alkaline precipitating agent described in step c is sodium carbonate, carbon
Sour hydrogen sodium, potassium carbonate, saleratus, ammonium carbonate, ammonium hydrogen carbonate, sodium hydroxide, potassium hydroxide, ammonium hydroxide or urea；Alkaline sedimentation
The molar ratio of agent and the metal contained by the noble metal source and the transition metal source is 2:1~10:1, the time of aging is
0.5-3h。
5. preparation method according to claim 1, which is characterized in that drying temperature described in step d is 60 DEG C -120 DEG C,
Drying time is 1-24h.
6. preparation method according to claim 1, which is characterized in that reducibility gas atmosphere described in step e includes body
Fraction is in the hydrogen or carbon monoxide of 1-10%, and the inert gas as balanced gas；In step e, the recovery time
For 0.5-10h.
7. preparation method according to claim 6, which is characterized in that the inert gas is helium, argon gas or nitrogen.
8. the catalyst for formaldehyde normal temperature oxidation prepared by the preparation method according to any one of claim 1-7.
9. catalyst according to claim 8, which is characterized in that the catalyst includes the activated carbon as carrier, and
As the noble metal and transition metal of active component, wherein the grain size of the active component is 5-10nm.
10. catalyst according to claim 8 application in oxidation of formaldehyde at normal temperatures, wherein the formaldehyde is a concentration of
0.1-1.0mg/m3, the room temperature is 15 DEG C -25 DEG C.
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| CN109603853A (en) * | 2019-02-25 | 2019-04-12 | 青岛华世洁环保科技有限公司 | Normal-temperature catalyst and composite screen and its application |
| CN109939703A (en) * | 2019-03-25 | 2019-06-28 | 福建绿航环保科技有限公司 | A kind of catalyst of the purification containing volatile organic compounds |
| CN110455977A (en) * | 2019-06-30 | 2019-11-15 | 北京联合大学 | A kind of low-temperature catalyzed luminous sensitive material of formaldehyde and ammonia |
| CN112264010A (en) * | 2020-10-26 | 2021-01-26 | 珠海格力电器股份有限公司 | Catalyst for normal-temperature decomposition of formaldehyde and preparation method thereof |
| CN113198488A (en) * | 2021-03-31 | 2021-08-03 | 浙江工业大学 | Activated carbon fiber loaded bimetallic catalyst for formaldehyde catalytic oxidation reaction and preparation and application thereof |
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| CN113198488A (en) * | 2021-03-31 | 2021-08-03 | 浙江工业大学 | Activated carbon fiber loaded bimetallic catalyst for formaldehyde catalytic oxidation reaction and preparation and application thereof |
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