CN109420496A - A kind of loaded nano platinum base alloy catalysis material Pt-M/N, preparation method and application - Google Patents
A kind of loaded nano platinum base alloy catalysis material Pt-M/N, preparation method and application Download PDFInfo
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- CN109420496A CN109420496A CN201710772229.0A CN201710772229A CN109420496A CN 109420496 A CN109420496 A CN 109420496A CN 201710772229 A CN201710772229 A CN 201710772229A CN 109420496 A CN109420496 A CN 109420496A
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- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 title claims abstract description 91
- 239000000463 material Substances 0.000 title claims abstract description 53
- 238000006555 catalytic reaction Methods 0.000 title claims abstract description 32
- 229910052697 platinum Inorganic materials 0.000 title claims abstract description 26
- 239000000956 alloy Substances 0.000 title claims abstract description 22
- 229910045601 alloy Inorganic materials 0.000 title claims abstract description 22
- 238000002360 preparation method Methods 0.000 title claims abstract description 20
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 claims abstract description 161
- 229910052751 metal Inorganic materials 0.000 claims abstract description 27
- 239000002184 metal Substances 0.000 claims abstract description 27
- 239000007864 aqueous solution Substances 0.000 claims abstract description 22
- 239000008139 complexing agent Substances 0.000 claims abstract description 18
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 15
- 238000003756 stirring Methods 0.000 claims abstract description 15
- 239000000243 solution Substances 0.000 claims abstract description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 13
- 238000003359 percent control normalization Methods 0.000 claims abstract description 12
- 239000002243 precursor Substances 0.000 claims abstract description 11
- 238000002604 ultrasonography Methods 0.000 claims abstract description 8
- 238000005406 washing Methods 0.000 claims abstract description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 30
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 9
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid group Chemical group C(CC(O)(C(=O)O)CC(=O)O)(=O)O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 9
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 8
- 229910052593 corundum Inorganic materials 0.000 claims description 8
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 claims description 8
- 239000000758 substrate Substances 0.000 claims description 8
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 8
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 claims description 6
- 229910019029 PtCl4 Inorganic materials 0.000 claims description 6
- 229910052741 iridium Inorganic materials 0.000 claims description 5
- 229910052707 ruthenium Inorganic materials 0.000 claims description 5
- 229910002651 NO3 Inorganic materials 0.000 claims description 3
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 3
- 235000010323 ascorbic acid Nutrition 0.000 claims description 3
- 229960005070 ascorbic acid Drugs 0.000 claims description 3
- 239000011668 ascorbic acid Substances 0.000 claims description 3
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052737 gold Inorganic materials 0.000 claims description 3
- 239000010931 gold Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 claims description 2
- 229910010084 LiAlH4 Inorganic materials 0.000 claims description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 2
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 claims description 2
- 239000004327 boric acid Substances 0.000 claims description 2
- 229960001484 edetic acid Drugs 0.000 claims description 2
- 239000012280 lithium aluminium hydride Substances 0.000 claims description 2
- 239000012279 sodium borohydride Substances 0.000 claims description 2
- 229910000033 sodium borohydride Inorganic materials 0.000 claims description 2
- 239000010970 precious metal Substances 0.000 abstract description 3
- 230000007704 transition Effects 0.000 abstract description 2
- 229910020427 K2PtCl4 Inorganic materials 0.000 abstract 1
- 235000019256 formaldehyde Nutrition 0.000 description 47
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 20
- 238000000034 method Methods 0.000 description 13
- 239000007789 gas Substances 0.000 description 12
- 239000002585 base Substances 0.000 description 11
- 229930040373 Paraformaldehyde Natural products 0.000 description 10
- 239000003054 catalyst Substances 0.000 description 10
- 229920002866 paraformaldehyde Polymers 0.000 description 10
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 8
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000012360 testing method Methods 0.000 description 8
- 230000003647 oxidation Effects 0.000 description 7
- 238000007254 oxidation reaction Methods 0.000 description 7
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 6
- 230000003197 catalytic effect Effects 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 238000010521 absorption reaction Methods 0.000 description 4
- 150000001450 anions Chemical class 0.000 description 4
- 239000001569 carbon dioxide Substances 0.000 description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 description 4
- 238000001514 detection method Methods 0.000 description 4
- 230000036541 health Effects 0.000 description 4
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 4
- 229910000510 noble metal Inorganic materials 0.000 description 4
- 230000001590 oxidative effect Effects 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 229910003244 Na2PdCl4 Inorganic materials 0.000 description 3
- 238000012512 characterization method Methods 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 238000002354 inductively-coupled plasma atomic emission spectroscopy Methods 0.000 description 3
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 3
- 229910052763 palladium Inorganic materials 0.000 description 3
- 229910021650 platinized titanium dioxide Inorganic materials 0.000 description 3
- 238000010189 synthetic method Methods 0.000 description 3
- 206010028980 Neoplasm Diseases 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 239000003610 charcoal Substances 0.000 description 2
- 238000006731 degradation reaction Methods 0.000 description 2
- OSVXSBDYLRYLIG-UHFFFAOYSA-N dioxidochlorine(.) Chemical compound O=Cl=O OSVXSBDYLRYLIG-UHFFFAOYSA-N 0.000 description 2
- 125000002485 formyl group Chemical class [H]C(*)=O 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- NICDRCVJGXLKSF-UHFFFAOYSA-N nitric acid;trihydrochloride Chemical compound Cl.Cl.Cl.O[N+]([O-])=O NICDRCVJGXLKSF-UHFFFAOYSA-N 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000011941 photocatalyst Substances 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 210000002345 respiratory system Anatomy 0.000 description 2
- 239000011734 sodium Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- 235000017166 Bambusa arundinacea Nutrition 0.000 description 1
- 235000017491 Bambusa tulda Nutrition 0.000 description 1
- 239000004155 Chlorine dioxide Substances 0.000 description 1
- 201000004624 Dermatitis Diseases 0.000 description 1
- BDAGIHXWWSANSR-UHFFFAOYSA-M Formate Chemical compound [O-]C=O BDAGIHXWWSANSR-UHFFFAOYSA-M 0.000 description 1
- 206010019233 Headaches Diseases 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 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 description 1
- 206010028813 Nausea Diseases 0.000 description 1
- 208000012902 Nervous system disease Diseases 0.000 description 1
- 208000025966 Neurological disease Diseases 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 244000082204 Phyllostachys viridis Species 0.000 description 1
- 235000015334 Phyllostachys viridis Nutrition 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- 241000220317 Rosa Species 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 206010047700 Vomiting Diseases 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 238000005275 alloying Methods 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000003556 assay Methods 0.000 description 1
- 239000011425 bamboo Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 201000011510 cancer Diseases 0.000 description 1
- 239000003183 carcinogenic agent Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 235000019398 chlorine dioxide Nutrition 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 230000001627 detrimental effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 230000006870 function Effects 0.000 description 1
- 239000008246 gaseous mixture Substances 0.000 description 1
- 231100000869 headache Toxicity 0.000 description 1
- 239000008236 heating water Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000004615 ingredient Substances 0.000 description 1
- 238000011835 investigation Methods 0.000 description 1
- 230000000622 irritating effect Effects 0.000 description 1
- 208000032839 leukemia Diseases 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 210000002751 lymph Anatomy 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000002086 nanomaterial Substances 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 230000008693 nausea Effects 0.000 description 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 230000008520 organization Effects 0.000 description 1
- 238000006385 ozonation reaction Methods 0.000 description 1
- 150000003057 platinum Chemical class 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 239000012286 potassium permanganate Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011897 real-time detection Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000012216 screening Methods 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 230000000638 stimulation Effects 0.000 description 1
- 208000024891 symptom Diseases 0.000 description 1
- 229920002994 synthetic fiber Polymers 0.000 description 1
- 231100000462 teratogen Toxicity 0.000 description 1
- 239000003439 teratogenic agent Substances 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 239000004753 textile Substances 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 230000008673 vomiting Effects 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
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/44—Palladium
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/46—Ruthenium, rhodium, osmium or iridium
- B01J23/462—Ruthenium
-
- 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
- B01J35/20—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state
- B01J35/23—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state in a colloidal state
-
- 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
- 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
- B01J35/396—Distribution of the active metal ingredient
- B01J35/399—Distribution of the active metal ingredient homogeneously throughout the support particle
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/03—Precipitation; Co-precipitation
- B01J37/031—Precipitation
- B01J37/035—Precipitation on carriers
-
- 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
- B01J37/16—Reducing
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- Chemical Kinetics & Catalysis (AREA)
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- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
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Abstract
The invention discloses the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N a kind of, under normal temperature and pressure, by K2PtCl4Aqueous solution, M2+Precursor solution and complexing agent aqueous solution are stirred in a reservoir；The molar ratio of Pt:M controls between 0.1~10, and the mole of complexing agent is 1~5 times of total metal molar amount；PH value is adjusted to alkalinity；Carrier N is added, total metal ladings (Pt+M) wt% control is 0.1%~20%；Ultrasound stirs at normal temperature；Reducing agent aqueous solution is added dropwise, stirs, filters, a large amount of multiple water washings, 100-140 DEG C is dried overnight, and obtains powdered Pt-M/N.Additionally provide the application of the catalysis material and catalysis material in terms of removing formaldehyde.For the present invention with M transition elements instead of precious metal element, formaldehyde removal efficiency is high, effectively reduces the cost of removal formaldehyde.
Description
Technical field
The present invention relates to formaldehyde treated fields, and in particular to a kind of formaldehyde treated material, with and preparation method thereof.
Background technique
Under normal temperature and pressure, formaldehyde is a kind of colourless gas for having intense stimulus taste.Formaldehyde in room air comes mostly
From in furniture, finishing material and textile.Respiratory tract and skin irritating effect of the formaldehyde to people, Yi Yinqi throat are swollen
Bitterly, headache, nausea, vomiting, the symptoms such as dermatitis.If people is chronically exposed in formaldehyde, it is possible that neurological disorders, memory
Power decline, it is serious can also afflicted with leukemia, the cancers such as lymph cancer.Formaldehyde is classified as by the World Health Organization can carcinogenic substance and can
Teratogen.
Concern further with people to indoor air quality and own health, people increasingly pay attention to first in room air
The measurement and removal of aldehyde.People's Republic of China's Code for design of dwelling houses (GB50096-2011) provides free formaldehyde in room air
Limit value be≤0.08mg/m3(that is: 65ppb).Since often to there is volatile formaldehyde exceeded for some furniture and finishing material
Phenomenon, the topic how to be concerned about using effective method reduction indoor formaldehyde content at many people.
It is existing on the market to be divided into following several classes: 1. physisorphtions by its working principle except formaldehyde products.Using work
Property the porous materials such as charcoal, bamboo charcoal, physical absorption is carried out to the formaldehyde in air, to play the effect for reducing concentration of formaldehyde.It should
Method low efficiency, generally can only achieve 3.3~28.6%.Simultaneously as physical absorption is reversible, when indoor formaldehyde content is lower
When, then the porous material for being adsorbed with higher concentration formaldehyde may become the source of release of formaldehyde, cause secondary pollution.2. Strong oxdiative
Agent oxidizing process.The chemicals sprinkling of potassium permanganate, the strong oxidizing properties such as chlorine dioxide is applied to household surface, is oxidized the formaldehyde into
For carbon dioxide and water, to play the effect of removal formaldehyde.The chemicals oxidisability that the method uses is stronger, has corruption mostly
Corrosion, when use, need significant care, otherwise may corrode skin, stimulation respiratory tract etc..3. anion purifier.Anion is net
Anion can be generated by changing device, convert water and carbon dioxide for the formaldehyde in air.But the method low efficiency (18.5~
30.8%) ozone can be generated while, generating anion, to will cause ozone concentration exceeded as being used for a long time, and is detrimental to health.
4. photocatalyst method.The fado uses titanic oxide material, and under ultraviolet irradiation, in titanium dioxide surface light can occur for formaldehyde
Catalytic oxidation generates carbon dioxide and water.Since the uitraviolet intensity in daylight is weak, the Degradation Formaldehyde of photocatalyst method
Inefficient (18.7~56.0%).5. Ozonation.The method generates a certain amount of ozone using ozone generator, is discharged into
In air.It since ozone has strong oxidizing property, can oxidize the formaldehyde into as carbon dioxide and water, to play the function of removal formaldehyde
Effect.The method is inefficient (18.2~44.2%), while ozone has certain toxicity, then can be to human body if concentration control is improper
Health generates harm.
Other than the method for numerous removal indoor formaldehydes that appeal discusses, precious metal catalyst oxidizing process is efficient, clear because of it
The features such as clean, receives more and more attention.Existing research shows that the platinum of support type or palladium catalyst can at room temperature efficiently
Catalysis oxidation formaldehyde.Due to expensive (about every gram of the $230) of noble metal, especially metal platinum, therefore, how further to mention
The activity of high catalyst reduces the dosage of noble metal, at the problem for needing to capture.
Size in addition to reducing precious metal material, is improved outside the utilization rate of noble metal, alloying is a kind of common metal
Modified means.He Hong of Ecological Environment Research Center, Chinese Academy of Sciences et al. has found in 1%wt Pt/TiO2Middle addition 2%
The alkali metal such as sodium or potassium can greatly improve the catalysis oxidation ability of catalyst PARA FORMALDEHYDE PRILLS(91,95).Correlative study obtains related awards,
And have been commercialized, but later investigation discovery, the formaldehyde removal rate of Related product are up to standard far away.Simultaneously as Pt-Na/
TiO2The preparation of material is needed using hydrogen high temperature reduction, and condition is more harsh, is not energy-saving and environment-friendly.It would therefore be desirable to seek
New synthetic method is looked for, new catalyst is synthesized, commercially eliminates the demand of formaldehyde to better meet us.
Summary of the invention
Therefore, the technical problem to be solved in the present invention is to provide the catalysis materials that one kind can effectively remove formaldehyde, simultaneously
The preparation method of the catalysis material is provided, and provides the application of the catalysis material.
The technical scheme is that a kind of preparation method of loaded nano platinum base alloy catalysis material Pt-M/N,
A. under normal temperature and pressure, by the 0.1-5g/100ml K of 0.1~10ml2PtCl4Aqueous solution, 0.1~10ml concentration are
The M of 0.01~0.1mol/L2+The complexing agent aqueous solution of 0.01~0.1mol/L of precursor solution and 0.1~20ml is in a reservoir
It is stirred；The molar ratio of Pt:M controls between 0.1~10, and the mole of complexing agent is 1~5 times of total metal molar amount；M
For Pd, Ru, Ir, either element in Au, Rh；The N is active supporting substrate, is selected from TiO2,MnO2, Al2O3, one of C；
B. pH value is adjusted to alkalinity；Be added the carrier N of 0.5~5g, total metal ladings (Pt+M) wt% control 0.1%~
Between 20%；
C. it after ultrasound 5-40min, stirs at normal temperature；Reducing agent aqueous solution is added dropwise, stirs, filters, a large amount of repeatedly washings
It washs, 100-140 DEG C is dried overnight, and obtains powdered Pt-M/N.
The ingredients such as the metals such as Pd, Ru, Ir, Rh PARA FORMALDEHYDE PRILLS(91,95) itself or the intermediate formic acid of Degradation Formaldehyde, formate, methanol
Has catalytic activity.But the excessively high too low catalytic activity that can all reduce Pt of numerical value, the attainable removal rate of the program is herein
Experiment table/chart in have detailed numerical value (> 90%).
Total metal ladings refer to: the gross mass of Pt element and M element accounts for the percentage of material gross mass, it may be assumed that (Pt+M) wt%
=[m (Pt)+m (M)]/[m (Pt)+m (M)+m (carrier)] x 100%.
Preferably, step c is water washing more than three times.
The preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to the present invention, it is preferred that described
M2+Precursor solution is the nitrate of M, one of villaumite or sulfate solution.
These types of precursor species are the chemical reagent for being easier to obtain.Meanwhile the dissolution of these types of salt in water
Degree is good, is conducive to reaction and carries out.
The preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to the present invention, it is preferred that described
Complexing agent is selected from citric acid, one of boric acid or ethylenediamine tetra-acetic acid.
These types of complexing agent is relatively common and is easy to get.
The preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to the present invention, it is preferred that described
Reducing agent is ascorbic acid, NaBH4Or LiAlH4One of or more than one.
These types of complexing agent is relatively common and is easy to get, therefore as preferred.
Preferably, total metal ladings (Pt+M) wt% control described in step b is in 0.5%-2%.
The preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to the present invention, it is preferred that step c
The mixing time is 1h or more.
It is further preferred that mixing time described in step c is 2 hours or more.
Preferably, in step c, reducing agent is 2~10 times excessive.
The preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to the present invention, it is preferred that use
NaOH aqueous solution adjusts pH value.
It is further preferred that with the NaOH aqueous solution of 0.1M.Other aqueous slkalis can also be used.Preferably, step b
PH value is adjusted to 8-10.
The present invention also provides above-mentioned loaded nano platinum base alloy catalysis material Pt-M/N, the M Pd being prepared,
Either element in Ru, Ir, Au, Rh；The N is active supporting substrate, is selected from TiO2,MnO2, Al2O3, one of C；Total gold
Belonging to carrying capacity (Pt+M) wt% is between 0.1%~20%.
Preferably, in catalysis material of the invention, total metal ladings (Pt+M) wt% control is in 0.5%-
2%.It is further preferred that total metal ladings (Pt+M) wt% control is 1%.
The present invention also provides above-mentioned loaded nano platinum base alloy catalysis material Pt-M/N answering in terms of formaldehyde removal
With.
The beneficial effects of the present invention are:
For present invention transition elements instead of Pt, formaldehyde removal efficiency is high, reduces manufacturing cost, removes first in high efficiency
Aldehyde technical field has biggish dissemination.
Detailed description of the invention
Fig. 1 is the TEM figure of Pt-M/N catalyst.
Fig. 2 is test device schematic diagram.
Fig. 3 is the catalytic oxidation activity of each material PARA FORMALDEHYDE PRILLS(91,95).
Fig. 4 is the conversion ratio of each material PARA FORMALDEHYDE PRILLS(91,95).
Specific embodiment
Embodiment 1
A. under normal temperature and pressure, by the 1g/100ml K of 0.365ml2PtCl4Aqueous solution, 1.58ml concentration are 0.05mol/L's
Na2PdCl4The complexing agent aqueous citric acid solution of precursor solution and 1ml 0.1mol/L are stirred in flask；Pt:M's rubs
, than control in 1:9, the mole of complexing agent is equal with total metal molar amount for you；M is Pd element；The N is active supporting substrate,
Selected from TiO2；
B. pH value is adjusted to alkalinity；The carrier N of 1g is added, total metal ladings (Pt+M) wt% control is 1%；
C. it after ultrasound 20min, stirs at normal temperature；Reducing agent aqueous ascorbic acid is added dropwise, reducing agent is 3 times excessive, stirs
It mixes, filters, a large amount of multiple water washings, 100-140 DEG C is dried overnight, and obtains powdered Pd9Pt1/TiO2.Metal index number
Indicate molar ratio.
Embodiment 2
A. under normal temperature and pressure, by the 1g/100ml K of 0.83ml2PtCl4Aqueous solution, 1.2ml concentration are 0.05mol/L's
Na2PdCl4The complexing agent aqueous solution of precursor solution and 0.8ml 0.1mol/L are stirred in flask；The molar ratio of Pt:M
In 1:3, the mole of complexing agent is equal with total metal molar amount for control；M is Pd element；The N is active supporting substrate, is selected from
Al2O3；
B. pH value is adjusted to alkalinity；The carrier Al of 1.12g is added2O3, total metal ladings (Pt+M) wt% control is 1%；
C. it after ultrasound 20min, stirs at normal temperature；Reducing agent aqueous solution is added dropwise, reducing agent is 3 times excessive, stirs, it filters,
A large amount of multiple water washings, 100-140 DEG C is dried overnight, and obtains powdered Pd3Pt1/Al2O3。
Embodiment 3
A. under normal temperature and pressure, by the 1g/100ml K of 1.56ml2PtCl4Aqueous solution, 0.75ml concentration are 0.05mol/L's
Na2PdCl4The complexing agent aqueous solution of precursor solution and 0.75ml 0.1mol/L are stirred in flask；The molar ratio of Pt:M
In 1:1, the mole of complexing agent is equal with total metal molar amount for control；M is Pd element；The N is active supporting substrate, is selected from
C；
B. pH value is adjusted to alkalinity；The carrier N of 1g is added, total metal ladings (Pt+M) wt% control is 1%；
C. it after ultrasound 20min, stirs at normal temperature；Reducing agent aqueous solution is added dropwise, reducing agent is 3 times excessive, stirs, it filters,
A large amount of multiple water washings, 100-140 DEG C is dried overnight, and obtains powdered Pd1Pt1/C。
Embodiment 4
A. under normal temperature and pressure, by the 2g/100ml K of 0.208ml2PtCl4Aqueous solution, 1.00ml concentration are 0.08mol/L's
Ru(NO3)3The complexing agent aqueous solution of precursor solution and 2.7ml 0.1mol/L are stirred in flask；The molar ratio of Pt:M
In 1:8, the mole of complexing agent is 3 times of total metal molar amount for control；N is active supporting substrate, is selected from Al2O3；
B. pH value is adjusted to alkalinity；The carrier N of 1g is added, total metal ladings (Pt+M) wt% control is 1%；
C. it after ultrasound 20min, stirs at normal temperature；Reducing agent aqueous solution is added dropwise, reducing agent is 5 times excessive, stirs, it filters,
A large amount of multiple water washings, 100-140 DEG C is dried overnight, and obtains powdered Pt1Ru8/Al2O3。
1. the preparation and test of sample
10~20mg Pt-M/N is placed in 10ml small beaker, the chloroazotic acid of addition 4ml Fresh, sealing ultrasound 2~
3min, until solid is well dispersed in chloroazotic acid.Heating water bath to solution boils 2~3 times.Cooled and filtered is simultaneously settled to 10
In ml/25ml volumetric flask.The solution matched is surveyed using inductively coupled plasma atomic emission spectrometry (ICP-AES)
Examination, is calculated the content of noble metal in raw material.
B.ICP-AES test result
The carrying capacity and molar ratio and its inventory of each metal are almost the same, it was demonstrated that the synthetic method of use can effectively will be expensive
Metal precursor is reducing loaded in carrier surface.Meanwhile material can simply and effectively be controlled by the inventory of presoma
In each metal molar ratio, greatly facilitate later period screening of catalyst.
2. the morphology characterization of nano material
Morphology characterization (Fig. 1) has been carried out to material sample using transmission electron microscope.As can be seen that your gold from photo
Belong to nanoparticle and be dispersed in carrier surface, partial size concentrates between 3-4nm.This proof, can using our synthetic method
Easily and effectively to prepare the support type platinum base Nanoalloy material that partial size is small, is evenly distributed.
The test of synthetic material PARA FORMALDEHYDE PRILLS(91,95) catalytic oxidation performance
1. test device (Fig. 2) and articles:
U-shaped glass tube (φ=6mm).
Catalyst (tabletting is simultaneously sieved, 20-40 mesh)
Formaldehyde gas steel cylinder (16ppm is nitrogen with gas), 100% oxygen bottle
Formaldehyde gas detector
Mass flowmenter, triple valve, water bath thermostat
2. test method:
The flow velocity of formaldehyde gas is 10ml/min, and the flow velocity of oxygen is 90ml/min, and total gas flow rate is controlled in 100ml/
min.Triple valve is got into Shang Lu, detector is placed on corresponding gas outlet, under room temperature after (about 15-30 minutes) stabilization of a period of time
Record formaldehyde and TVOC concentration initial value.In this experiment, the reading of formaldehyde and TVOC are generally in 2.5ppm and 9.5ppm or so.
0.1 gram of catalyst is placed on the left of U-shaped glass tube, constant temperature is to 25 DEG C (about 15 minutes) in water-bath.Rotate threeway
Valve makes mixed gas by catalyst, in the concentration of corresponding gas outlet formaldehyde and TVOC in detector real-time detection gas circuit.Often
A sample persistently records 4 hours.
3. test result and analysis
By theoretical calculation, initial concentration of formaldehyde should be 16*0.9=14.4ppm, and TVOC should be equal thereto.But it surveys
Value formaldehyde is initially between 2.3-2.6ppm, and TVOC is initially at 8.8-9.99 (i.e. upper limit of detection), or the detection machine with detector
It manages related.Conversion ratio calculating is averaged (formaldehyde 2.5ppm, TVOC 9.5ppm).
Fig. 3 is the concentration of formaldehyde measured value of each material different time points.In pure carrier TiO2In blank test, with when
Between increase, U-tube end point detection to concentration of formaldehyde also gradually increase.Concentration of formaldehyde and time at approximate linear relationship,
This explanation is since formaldehyde is in TiO2There is absorption in material surface.It is worth noting that, for PdxPty/TiO2(x=1, y=0；x
=1,3,9, y=1；X=0, y=1) material, concentration of formaldehyde first rises rapidly, then tends towards stability, and class plateau occurs.It is right
In Pd/TiO2Material, concentration of formaldehyde rose very rapidly up to 0.9ppm or so in one hour, much higher than the N blank at same time point
Experiment value (~0.3ppm).It is believed that the addition of Pd may change TiO2Surface sex character, cause formaldehyde on its surface
Absorption can be rapidly achieved balance.The addition of Pt can greatly improve the activity of material PARA FORMALDEHYDE PRILLS(91,95) catalysis oxidation.With material
The catalysis oxidation ability of the increase of Pt content in material, PARA FORMALDEHYDE PRILLS(91,95) is gradually promoted.After four hours, Pd9Pt1/TiO2, Pd3Pt1/
TiO2And Pd1Pt1/ TiO2The concentration of formaldehyde of rear end detection is respectively 0.35ppm, 0.27ppm and 0.17ppm, is TiO2Material
The 35%, 27% and 17% of blank assay value (~1ppm).Pd1Pt1/TiO2With Pt/TiO2Catalytic activity it is very close.
The concentration of formaldehyde value of each material different time points is calculated by the concentration of formaldehyde (2.5ppm) in gaseous mixture
Corresponding conversion ratio (Fig. 4 and table 1).Wherein, Pd1Pt1/TiO2With Pt/TiO2The conversion ratio of PARA FORMALDEHYDE PRILLS(91,95) is respectively 93% He
95%, very efficiently.Meanwhile catalytic performance is sufficiently stable, enters plateau, conversion ratio after 3 hours within about 1 hour or so
Almost without decaying, it was demonstrated that both materials can be with long-term stable operation.In view of the price of transition metal is generally than the valence of platinum
Lattice are more cheap, Pd1Pt1/TiO2There is stronger competitiveness in commercialization.
The conversion ratio of each material PARA FORMALDEHYDE PRILLS(91,95) of table 1.
We are co-deposited the precipitation method using mild liquid phase, have easily and efficiently synthesized a series of platinum base nanometer of support types
Alloy catalysis material, and more comprehensive characterization has been carried out to material, it tests them and trace formaldehyde gas is urged at normal temperature
Change oxidation susceptibility.Studies have shown that the conversion ratio of new material PARA FORMALDEHYDE PRILLS(91,95) gas is up to 90% or more, long-time stability are excellent.
Claims (10)
1. a kind of preparation method of loaded nano platinum base alloy catalysis material Pt-M/N, it is characterised in that:
A. under normal temperature and pressure, by the 0.1-5g/100ml K of 0.1~10ml2PtCl4Aqueous solution, 0.1~10ml concentration be 0.01~
The M of 0.1mol/L2+The complexing agent aqueous solution of 0.01~0.1mol/L of precursor solution and 0.1~20ml stirs mixed in a reservoir
It closes；The molar ratio of Pt:M controls between 0.1~10, and the mole of complexing agent is 1~5 times of total metal molar amount；M is Pd,
Either element in Ru, Ir, Au, Rh；The N is active supporting substrate, is selected from TiO2,MnO2, Al2O3, one of C；
B. pH value is adjusted to alkalinity；The carrier N of 0.5~5g is added, total metal ladings (Pt+M) wt% control is 0.1%~20%
Between；
C. it after ultrasound 5-40min, stirs at normal temperature；Reducing agent aqueous solution is added dropwise, stirs, filters, a large amount of multiple water washings,
100-140 DEG C is dried overnight, and obtains powdered Pt-M/N.
2. the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to claim 1, feature exist
In: the M2+Precursor solution is the nitrate of M, one of villaumite or sulfate solution.
3. the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to claim 1, feature exist
In: the complexing agent is selected from citric acid, one of boric acid or ethylenediamine tetra-acetic acid；The reducing agent is ascorbic acid, NaBH4
Or LiAlH4One of or more than one.
4. the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to claim 1, feature exist
In: total metal ladings (Pt+M) wt% control is in 0.5%-2% described in step b.
5. the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to claim 1, feature exist
In: mixing time described in step c is 1h or more.
6. the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to claim 1, feature exist
In: reducing agent described in step c is 2~10 times excessive.
7. the preparation method of loaded nano platinum base alloy catalysis material Pt-M/N according to claim 1, feature exist
In: pH value is adjusted with NaOH aqueous solution.
8. the loaded nano platinum base alloy catalysis material Pt-M/N that claim 1 is prepared, it is characterised in that: M Pd,
Either element in Ru, Ir, Au, Rh；The N is active supporting substrate, is selected from TiO2,MnO2, Al2O3, one of C；Total metal
Carrying capacity (Pt+M) wt% is between 0.1%~20%.
9. loaded nano platinum base alloy catalysis material Pt-M/N according to claim 8, it is characterised in that: total gold
Belong to carrying capacity (Pt+M) wt% control in 0.5%-2%.
10. application of the loaded nano platinum base alloy catalysis material Pt-M/N in terms of formaldehyde removal described in claim 8.
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