CN102836712A - Catalyst for completely removing formaldehyde in indoor air at room temperature - Google Patents
Catalyst for completely removing formaldehyde in indoor air at room temperature Download PDFInfo
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- CN102836712A CN102836712A CN 201110174299 CN201110174299A CN102836712A CN 102836712 A CN102836712 A CN 102836712A CN 201110174299 CN201110174299 CN 201110174299 CN 201110174299 A CN201110174299 A CN 201110174299A CN 102836712 A CN102836712 A CN 102836712A
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Abstract
The invention provides a high-efficiency and humidity-resisting catalysis technology for removing formaldehyde at room temperature and relates to the field of catalysis and environmental protection. The catalysis technology is characterized in that honeycomb ceramic is used as a carrier, preloading mesoporous cerium dioxide (CeO2) is used as a basal body, and a back loading platinum (Pt) is used as an active component. The mesoporous CeO2 is characterized in that the diameter of every meso pore is 0.5-3nm. The weight ratio of the Pt to the CeO2 is 0-5 percent. The integral catalyst provided by the invention is high in efficiency and stability and has no side effects under a real environment with room temperature and normal humidity, and can be widely used for removing formaldehyde pollutants in various microenvironments.
Description
Technical field
The present invention is the catalysis technique that a kind of efficient moisture-resistant room temperature is removed formaldehyde, relates to fields such as environmental protection, air pollutants improvement and environmental protection.It is characterized in that adopting ceramic honey comb is carrier, with the loaded mesoporous ceria CeO of elder generation
2Be matrix, later platinum (Pt) is an active component.Meso-pore Ce O
2Matrix is characterised in that mesoporous aperture is 0.5-3nm.Pt and CeO
2Weight ratio be 0～5%.
The invention still further relates to above-mentioned mesoporous material preparation method.
The invention still further relates to above-mentioned mesoporous material and be applied to the improvement of various environmental protection and air formaldehyde pollutant.
Background technology
International cancer research institution of the World Health Organization (IARC) tissue is pointed out: formaldehyde can cause human carcinogenic.Research shows that formaldehyde is the higher material of a kind of toxicity, and short term contact formaldehyde can stimulate eyes, nasal cavity and respiratory tract and cause allergic reaction; Long-term contact low dosage formaldehyde can increase nasopharyngeal carcinoma, leukaemia and dead possibility.Therefore, China " IAQ standard " (GB/T18883-2002) in the regulation formaldehyde in indoor air sanitary standard (maximum permissible concentration) be respectively 0.10mg/m
3Simultaneously, along with steadily improving of China's rapid development of economy and living standards of the people, the repairs profession that is driven by real estate and building industry has obtained unprecedented development.Therefore, the air formaldehyde pollution problem that is caused by finishing or ornament materials is very serious, has caused that the whole world pays close attention to greatly, and the formaldehyde of removing in the room air is extremely urgent.
The method that purifies formaldehyde comprises absorption method, chemical reaction method, photocatalytic oxidation and heat catalytic oxidation method.The short-term effective method is a chemical reaction method at present; Promptly through chemical reagent and formolite reaction to reach the purpose of removing formaldehyde in the air; Its major defect is that chemical reagent is sometimes dangerous, cost is high, can only once uses, and may cause secondary pollution etc.Common chemical reaction method: formaldehyde generates water and carbon dioxide after being loaded in the filter that aluminium oxide or activated carbon make through the potassium permanganate load.But in case the potassium permanganate full consumption, filter will lose efficacy.Spray chemical reagent in the air or contaminated air is fed chemical reagent solution, generate other chemical substance by chemical reagent (like organic amine etc.) and formaldehyde complexing.Except the cost height, more very be that the material itself that it generated has certain toxicity, usually with the form suspended of aerosol particle in air, can directly get into human respiratory tract and lung, bigger to human harm.
Absorption method and photocatalytic method also are the methods of the removal formaldehyde in indoor air pollutant used always.Adsorbent commonly used is porous material such as active carbon, the molecular sieve etc. of high-ratio surface in the absorption method.Because boiling point of formaldehyde lower (20 ℃) and molecule have stronger polarity; So at room temperature gaseous formaldehyde the surface be nonpolar or material such as low pole active carbon on absorption generally a little less than; Therefore in practical application, need carry out modification to these porous masses usually, to improve its adsorption capacity.Yet physical absorption still is that chemisorbed all can not obtain satisfied effect, because when absorption and desorption reach balance when saturated (adsorb), adsorbent will lose efficacy maybe to be needed to regenerate.Catalyst commonly used in the photochemical catalytic oxidation formaldehyde technology is TiO
2Yet, the lower formaldehyde of full-scale condition remove efficiency limitations, among others photocatalysis use widely.Also have, make the migration of its electronics occur in problem such as visible region through modification and remain problem demanding prompt solution in photocatalytic degradation formaldehyde and even the overall optical catalytic field photochemical catalyst.
The catalytic oxidation airborne formaldehyde of degrading is a kind of long-acting method, and the most key is catalyst.U.S. Pat 5585083 has been invented a kind of Pt/SnO
2Catalyst is removed the method for formaldehyde in the air, and catalyst uses airborne oxygen will perfect as oxidant and is degraded into carbon dioxide and water fully under extra energy input and-5～25 ℃ of conditions not having.But Pt content (12%) high in the catalyst causes costing an arm and a leg of catalyst, and therefore this catalyst can only be used special occasions such as some military projects or aerospace.Chinese patent CN1698932A perhaps adsorbs composite oxide catalysts with the rare earth oxide of load gold, under 80-100 ℃ of temperature, can obtain effect preferably, and still, the input of high humility and heat energy is the biggest obstacle of this catalyst extensive use.
The purpose of this invention is to provide a kind of honeycomb ceramic catalyze material of under the condition of room temperature and high humility, efficiently removing formaldehyde, be about to airborne formaldehyde and be completely oxidized to carbon dioxide (CO
2) and water (H
2O), be applicable to the removal of airborne formaldehyde pollutant.The airborne formaldehyde of environment protection catalytic oxidation removal has caused the attention in the world, because catalyst does not need extra light or electric energy just can airborne formaldehyde be converted into harmless H
2O and CO
2, its advantage is: it is high to handle formaldehyde efficient, does not have secondary pollution and do not exist to adsorb problems such as saturated.
Summary of the invention
The object of the invention 1: provide a kind of efficient room temperature to remove the mesoporous material of formaldehyde.
The object of the invention 2: provide a kind of efficient room temperature to remove the preparation method of the mesoporous material of formaldehyde.
The objective of the invention is to realize through following scheme:
Efficient room temperature provided by the invention is removed formaldehyde, adopts following scheme implementation:
1. the preparation of mesoporous ceria nano material
The P123 of 10g is added the Ce (NO that contains 0.01mol
3)
4The 250ml aqueous solution in, at continuous stirring condition adding 40ml trioctylamine down, obtain colloidal sol; To seal then and behind crystallization 24h under 50 ℃ of conditions; Colloidal sol is transferred to has in the teflon-lined still, in 100 ℃ of following hydro-thermal 24h, products therefrom is behind deionized water and ethanol cyclic washing; Put into the electric vacunm drying case in 100 ℃ of following vacuum drying 24h: put into Muffle furnace at last in 500 ℃ of calcining 6h removed template methods down, the gained powder is the mesoporous cerium oxide sample.
2. the preparation of the loaded mesoporous cerium dioxide nano material of honeycomb ceramic carrier
(1) takes by weighing the mesoporous ceria nano material of a certain amount of doping, add a certain proportion of deionized water and adhesive.According to the requirement of viscosity and particle diameter, adhesive is mixed suspended emulsion high-speed stirred 1～24h with the mesoporous ceria nano material, obtain certain density mesoporous ceria nano material slurries.
(2) adopt the vacuum-negative pressure extraction technique that above-mentioned mesoporous ceria nano material slurries are coated on the ceramic honey comb of anticipating,, obtain carried with doped mesoporous ceria nano material at 200～800 ℃ of roasting 1～36h.
3. the method for mesoporous ceria nano material supporting Pt is characterized in that adopting the preparation of gas phase reduction process or liquid phase reduction:
(1) gas phase reduction process: above-mentioned loaded mesoporous cerium dioxide nano material (claim 6 preparation) is immersed in the nitroso diamines closes platinum (Pt (NH
3)
2(NO
2)
2) or chloroplatinic acid (H
2PtCl
6) in the mixed solution, dry back is at 200～400 ℃ of roasting 1～36h, then at H
2At 200～400 ℃ of reduction 1～36h, or adopt the UV of certain wavelength and light intensity to shine 1～72h in the atmosphere.
(2) liquid phase reduction: loaded mesoporous ceria monolithic devices material is immersed in finite concentration Pt (NH
3)
2(NO
2)
2Or H
2PtCl
6In the mixed solution, add reducing agent then, like NaBH
4, formaldehyde, ethylene glycol, glucose or have the organic matter of reducing property, react 1～6h at a certain temperature, dry back is at 200～400 ℃ of roasting 1～36h.
Technique effect of the present invention
Technique effect of the present invention is the characteristic that a kind of room temperature can thoroughly be removed airborne formaldehyde technology: in the presence of unglazed under the often wet condition of room temperature with oxidation air in concentration be 0.010～50mg/m
3Formaldehyde change into nontoxic CO
2And H
2O.
Advantage of the present invention
1. high efficiency and broad spectrum activity
Efficient room temperature of the present invention is removed the formaldehyde catalysis technique, adopts the method for catalysis, and PARA FORMALDEHYDE PRILLS(91,95) has good removal ability.
2. high stability and long-lasting
Anti-biotic material of the present invention has been abandoned adsorption technology, adopts catalytic activation oxygen mechanism, and catalyst did not consume when formaldehyde was removed, and has well long-lasting, very high stability and good economy, and human body is not had any adverse side effect.
Avirulence with have no side effect
Efficient room temperature of the present invention is removed the catalysis technique of formaldehyde, and when being applied to air clearing product, avirulence does not have accessory substance carbon monoxide (CO) and formic acid and produces.
The specific embodiment
Embodiment one
The preparation of mesoporous ceria nano material
The P123 of 10g is added the Ce (NO that contains 0.01mol
3)
4The 250ml aqueous solution in, at continuous stirring condition adding 40ml trioctylamine down, obtain colloidal sol; To seal then and behind crystallization 24h under 50 ℃ of conditions; Colloidal sol is transferred to has in the teflon-lined still, in 100 ℃ of following hydro-thermal 24h, products therefrom is behind deionized water and ethanol cyclic washing; Put into the electric vacunm drying case in 100 ℃ of following vacuum drying 24h: put into Muffle furnace at last in 500 ℃ of calcining 6h removed template methods down, the gained powder is the mesoporous cerium oxide sample.Little angle XRD and HRTEM analytical proof CeO
2The aperture be 2nm.
The preparation of the loaded mesoporous cerium dioxide nano material of honeycomb ceramic carrier takes by weighing the mesoporous ceria nano material of a certain amount of doping, adds a certain proportion of deionized water and adhesive.According to the requirement of viscosity and particle diameter, adhesive is mixed suspended emulsion high-speed stirred 1～24h with the mesoporous ceria nano material, obtain certain density mesoporous ceria nano material slurries.Adopt the vacuum-negative pressure extraction technique that above-mentioned mesoporous ceria nano material slurries are coated on the ceramic honey comb of anticipating,, obtain carried with doped mesoporous ceria nano material at 200～800 ℃ of roasting 1～36h.
The method of mesoporous ceria nano material supporting Pt is characterized in that adopting gas phase reduction process.Above-mentioned loaded mesoporous cerium dioxide nano material (claim 6 preparation) is immersed in the nitroso diamines closes platinum (Pt (NH
3)
2(NO
2)
2) or chloroplatinic acid (H
2PtCl
6) in the mixed solution, dry back is at 200～400 ℃ of roasting 1～36h, then at H
2At 200～400 ℃ of reduction 1～36h, or adopt the UV of certain wavelength and light intensity to shine 1～72h in the atmosphere.
The performance test of catalyst is carried out on the fixed bed reactors of continuous-flow.Before the catalyst performance test, catalyst is not done any processing; Fine catalyst is pulverized the granular of processing 0.25～0.50mm through compressing tablet, then the 0.2g granular is loaded in the glass tube; Be under 50% the condition in room temperature (20 ℃) and relative humidity, feed and contain 5.0mg/m
3The air of formaldehyde, wind speed are 2.5m/s.Reactor outlet gas detects with FTIR infrared spectrum analyser, trace gas analysis mass spectrograph and Aglient 7890A gas chromatographicanalyzer simultaneously simultaneously.The result sees table 1.
The test result of table 1. mesoporous ceria nano material supporting Pt.
Embodiment two
The preparation of mesoporous ceria nano material.The P123 of 10g is added the Ce (NO that contains 0.01mol
3)
4The 250ml aqueous solution in, at continuous stirring condition adding 40ml trioctylamine down, obtain colloidal sol; To seal then and behind crystallization 24h under 50 ℃ of conditions; Colloidal sol is transferred to has in the teflon-lined still, in 100 ℃ of following hydro-thermal 24h, products therefrom is behind deionized water and ethanol cyclic washing; Put into vacuum drying chamber in 100 ℃ of following vacuum drying 24h: put into Muffle furnace at last in 500 ℃ of calcining 6h removed template methods down, the gained powder is the mesoporous cerium oxide sample.Little angle XRD and HRTEM analytical proof CeO
2The aperture be 2nm.
The preparation of the loaded mesoporous cerium dioxide nano material of honeycomb ceramic carrier takes by weighing the mesoporous ceria nano material of a certain amount of doping, adds a certain proportion of deionized water and adhesive.According to the requirement of viscosity and particle diameter, adhesive is mixed suspended emulsion high-speed stirred 1～24h with the mesoporous ceria nano material, obtain certain density mesoporous ceria nano material slurries.Adopt the vacuum-negative pressure extraction technique that above-mentioned mesoporous ceria nano material slurries are coated on the ceramic honey comb of anticipating,, obtain carried with doped mesoporous ceria nano material at 200～800 ℃ of roasting 1～36h.
The method of mesoporous ceria nano material supporting Pt is characterized in that adopting liquid phase reduction: loaded mesoporous ceria monolithic devices material is immersed in finite concentration Pt (NH
3)
2(NO
2)
2Or H
2PtCl
6In the mixed solution, add reducing agent then, like NaBH
4, formaldehyde, ethylene glycol, glucose or have the organic matter of reducing property, mainly select NaBH
4, react 1～6h at a certain temperature, dry back is at 200～400 ℃ of roasting 1～36h.The performance test of catalyst is carried out on the fixed bed reactors of continuous-flow.
Before the catalyst performance test, catalyst is not done any processing; Fine catalyst is pulverized the granular of processing 0.25～0.50mm through compressing tablet, then the 0.2g granular is loaded in the glass tube; Be under 50% the condition in room temperature (20 ℃) and relative humidity, feed and contain 5.0mg/m
3The air of formaldehyde, wind speed are 2.5m/s.Reactor outlet gas detects with FTIR infrared spectrum analyser, trace gas analysis mass spectrograph and Aglient7890A gas chromatographicanalyzer simultaneously simultaneously.The result sees table 2.
The test result of table 2. mesoporous ceria nano material supporting Pt.
Embodiment three
The preparation of the mesoporous ceria nano material of supporting Pt is identical with embodiment two.
The performance test of catalyst stability experiment is with embodiment one, and 120 days follow-on test time, the formaldehyde of inlet is 5mg/m
3, the formaldehyde exit concentration is respectively 0.001mg/m
3
Claims (10)
1. the present invention is the catalysis technique that a kind of efficient moisture-resistant room temperature is removed formaldehyde, and it is characterized in that adopting ceramic honey comb is carrier, with the loaded mesoporous ceria CeO of elder generation
2Be matrix, later platinum (Pt) is an active component.
2. a kind of efficient moisture-resistant room temperature in the claim 1 is removed the catalysis technique of formaldehyde, and its characteristic catalyst is its preparation as follows:
(1) preparation of mesoporous ceria nano material.
(2) preparation of the loaded mesoporous cerium dioxide nano material of honeycomb ceramic carrier.
(3) method of mesoporous ceria nano material supporting Pt is characterized in that adopting the preparation of gas phase reduction process or liquid phase reduction.
3. the preparation method of mesoporous cerium dioxide nano material in the claim 2 (1) is characterized in that adopting hydrothermal method synthetic:
A certain amount of P123 is added the Ce (NO that contains 0.01mol
3)
4The 250ml aqueous solution in, at continuous stirring condition adding 40ml trioctylamine down, obtain colloidal sol; To seal then and behind 50 ℃ of crystallization 24h; Colloidal sol is transferred to has in the teflon-lined still, in 100 ℃ of following hydro-thermal 24h, products therefrom is behind deionized water and ethanol cyclic washing; Put into the electric vacunm drying case in 100 ℃ of following vacuum drying 24h: put into Muffle furnace at last in 500 ℃ of calcining 6h removed template methods down, the gained powder is the mesoporous cerium oxide sample.
4. the preparation of the loaded mesoporous cerium dioxide nano material of claim 2 (2) honeycomb ceramic carrier is characterized in that the condition for preparing is following:
(1) takes by weighing the mesoporous ceria nano material of a certain amount of doping, add a certain proportion of deionized water and adhesive.According to the requirement of viscosity and particle diameter, adhesive is mixed suspended emulsion high-speed stirred 1～24h with the mesoporous ceria nano material, obtain certain density mesoporous ceria nano material slurries.
(2) adopt the vacuum-negative pressure extraction technique that above-mentioned mesoporous ceria nano material slurries are coated on the ceramic honey comb of anticipating,, obtain carried with doped mesoporous ceria nano material at 200～800 ℃ of roasting 1～36h.
5. the method for the mesoporous ceria nano material supporting Pt in the claim 2 (3) is characterized in that adopting the gas phase reduction process preparation method:
Above-mentioned loaded mesoporous cerium dioxide nano material (claim 6 preparation) is immersed in the nitroso diamines closes platinum (Pt (NH
3)
2(NO
2)
2) or chloroplatinic acid (H
2PtCl
6) in the mixed solution, dry back is at 200～400 ℃ of roasting 1～36h, then at H
2At 200～400 ℃ of reduction 1～36h, or adopt the UV of certain wavelength and light intensity to shine 1～72h in the atmosphere.
6. the method for the mesoporous ceria nano material supporting Pt in the claim 2 (3) is characterized in that adopting the gas phase reduction process preparation method:
Loaded mesoporous ceria monolithic devices material is immersed in finite concentration Pt (NH
3)
2(NO
2)
2Or H
2PtCl
6In the mixed solution, add reducing agent then, react 1～6h at a certain temperature, dry back is at 200～400 ℃ of roasting 1～36h.
In the claim 6 (4) reducing agent be NaBH
4, formaldehyde, ethylene glycol, glucose or have the organic matter of reducing property, preferably adopt NaBH
4
8. the adhesive described in the claim 4 (1) is inorganic bonds such as silicate, aluminium oxide or zirconium carbonate ammonium, and the weight ratio of adhesive and mesoporous ceria nano material is between 1～50%.Pt described in the claim 7 and mesoporous ceria nano material matrix weight ratio are 0～5%.
9. the mesoporous material of purifying formaldehyde in the long-acting air at room temperature in the claim 1, the aperture that it is characterized in that is 0.5-3nm.Pt and CeO
2Weight ratio be 0～5%.
10. a kind of efficient moisture-resistant room temperature described in the claim 1 is removed the characteristic of the catalysis technique of formaldehyde: in the presence of unglazed under the often wet condition of room temperature with oxidation air in concentration be 0.010～50mg/m
3Formaldehyde change into nontoxic carbon dioxide and water.
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|---|---|---|---|
| CN 201110174299 CN102836712A (en) | 2011-06-24 | 2011-06-24 | Catalyst for completely removing formaldehyde in indoor air at room temperature |
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|---|---|---|---|
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Application publication date: 20121226 |