CN103599793A - Supported copper-manganese composite oxide catalyst capable of removing formaldehyde at room temperature and preparation method - Google Patents
Supported copper-manganese composite oxide catalyst capable of removing formaldehyde at room temperature and preparation method Download PDFInfo
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Abstract
The invention discloses a supported copper-manganese composite oxide catalyst capable of removing formaldehyde at room temperature and a preparation method. The supported copper-manganese composite oxide catalyst is capable of completely oxidizing formaldehyde gas in the air into carbon dioxide and water under the conditions of room temperature and normal atmospheric humidity; the catalyst uses Cu and Mn as active components and employs TiO2 or active alumina as a carrier, the content of Cu and Mn accounts for 10 to 30% of the total mass of the catalyst, and a mol ratio of Cu to Mn is 1 1 to 1 4; evaluation of purification performance of the catalyst on formaldehyde is carried out in a self-made static catalytic oxidation formaldehyde reaction experimental apparatus and a minisized catalytic reaction experimental apparatus. According to the invention, the catalyst can highly efficiently, stably and thoroughly remove formaldehyde in the air in the actual environment of normal temperature and normal atmospheric humidity; the preparation method for the catalyst is simple and has low cost, input of any external energy is not needed in a catalytic reaction, and the catalyst is applicable to removal of formaldehyde pollution in closed and semiclosed space like an artificial board production workshop, a room and a building material and furniture market.
Description
Technical field
The carried copper Mn complex oxide catalyst and the preparation method that the present invention relates under the condition that in room temperature, often wets, airborne formaldehyde gas is completely oxidized to harmless carbon dioxide and water, belong to catalysis material, environmental catalysis and field of environment protection.It is characterized in that it is active component that catalyst be take Cu and Mn, adopts TiO
2or activated alumina is carrier.
Background technology
Along with the accelerated development of Chinese Urbanization, the room air pollution that house decoration brings is day by day serious, has become and has affected population health, socially harmonious major issue.Formaldehyde is one of pollutant typical, the most serious in indoor environment, has higher toxicity , China toxic chemical and preferentially controls and on list, be in second, and by the World Health Organization, be defined as carcinogenic and cause deformed material.In the < < IAQ standard > > (GB/T18883-2002) of China, the sanitary standard (maximum permissible concentration) of regulation formaldehyde in indoor air is 0.10mg/m
3.According to statistics, after finishing, in 1~6 month, formaldehyde rate reaches 80% in room, in meeting room and office, approaches 100%; Fit up after 3 years, exceeding standard rate all still reaches more than 50%.The research of Japan Yokohama national university shows, the release time limit of the formaldehyde pollution that interior decoration or ornament materials bring is generally 8~15 years, and modern has and surpasses time of 80% and spend indoor, and indoor formaldehyde is healthy to people by the Long-term Effect.Therefore the formaldehyde that, adopts effective method to remove in room air has great importance to the mankind's life and health.
At present, the method for removal Formaldehyde Pollution of Indoor Air mainly comprises absorption method, anion method, green plants absorption process, low temperature plasma method, photocatalytic oxidation and heat catalytic oxidation method etc.Wherein, the restriction of the easy sorbent suspension inactivation of absorption method and regeneration and adsorbent capacity; Anion method is had relatively high expectations to transmitter, and easily secondary fly-up occurs; Green plants disposal ability limited and ageing need textual criticism; Lower temperature plasma technology exists that power consumption is large, secondary pollution problems; The problems such as photocatalytic oxidation can at room temperature be processed formaldehyde, but it is inadequate to process the formaldehyde degree of depth, and disposal ability is low, and must have the support of ultraviolet light, therefore exists light source on the high side, and the life-span is short are difficult to use in indoor improvement; Heat catalytic oxidation method can be under the condition of gauge without light source to air in formaldehyde carry out oxidation Decomposition, to formaldehyde in indoor air clearance up to 100%, but the operating temperature of course of reaction, far above room temperature, is difficult to meet the requirement of the required normal-temperature operation of indoor air purification, low energy consumption.
Catalyze oxidation of formaldehyde is a kind of method of effectively removing indoor formaldehyde at ambient temperature, get the attention in recent years, but the catalyst of current room temperature catalyze oxidation of formaldehyde application all comprises at least one noble metal.The Pt/SnO of US Patent No. 5585083 inventions
2catalyst is not having the input of extra energy and can become carbon dioxide and water by airborne formaldehyde is degradable under-5~25 ℃ of conditions, but there is mass fraction in this catalyst, is 12% Pt.Chinese patent CN102139234A adopts low temperature liquid phase reducing process to prepare a kind of support type reduced precious metal catalyst at ambient temperature airborne formaldehyde with high removal efficiency, its active component is one or more in reduction-state noble metal platinum, palladium, gold and silver, and bullion content accounts for the 0.01-10% of total catalyst weight.Chinese patent CN103071489A discloses a kind of carried active carbon catalysis material of eliminating formaldehyde at room temperature, this catalysis material at room temperature clearance of PARA FORMALDEHYDE PRILLS(91,95) reaches more than 98.2%, but described catalysis material comprises 0.1~2% noble metal active component, noble metal is a kind of or its combination in gold, palladium, ruthenium, rhodium, platinum.Because Precious Metals Resources is rare, expensive, limited the promotion and application that room temperature catalytic oxidation method is removed formaldehyde.
The object of this invention is to provide and a kind ofly under room temperature and normal wet condition, airborne formaldehyde is completely oxidized to carbon dioxide (CO
2) and water (H
2o) carried copper manganese composite oxide catalysis material, is applicable to the removal of sealing, hemi-closure space formaldehyde pollutants.The advantage that this catalysis material is processed formaldehyde is: treatment effeciency is high, and cost is more cheap, there is no secondary pollution and does not adsorb the problems such as saturated.
Summary of the invention
The object of the present invention is to provide a kind of carried copper Mn complex oxide catalyst that airborne formaldehyde is completely oxidized to carbon dioxide and water under room temperature and normal wet condition.
The present invention also aims to provide the preparation technology of above-mentioned carried copper Mn complex oxide catalyst.
The object of the invention is to be achieved through the following technical solutions:
Remove a carried copper Mn complex oxide catalyst for formaldehyde, take Cu and Mn as active component, adopt TiO
2or activated alumina is carrier, Cu and Mn content account for 10%~30% of catalyst gross mass, and the molar ratio of Cu and Mn is 1:1~1:4.
Cu (the NO that the preparation method of the carried copper Mn complex oxide catalyst of removal formaldehyde of the present invention is 1:1~1:4 by molar ratio
3)
23H
2o and 50% manganese nitrate aqueous solution join and in distilled water, be made into mass fraction is 10%~20% mixed solution, and then dropping into quality is the Powdered TiO of 7~9 times of copper manganese gross masses
2carrier or graininess γ-Al
2o
3carrier, 30~50 ℃ of lower magnetic forces stir 2~6h, and dry 6~10h at 80~120 ℃ grinds screening after roasting 3~8h at 400~1000 ℃ of Muffle furnaces.
The purifying property evaluation of catalyst PARA FORMALDEHYDE PRILLS(91,95) of the present invention is carried out on homemade static catalyze oxidation of formaldehyde reaction experiment device.Catalyst and sample bottle are placed on to conical flask bottom, 37% formalin solution are added in sample bottle simultaneously, utilize the silica gel plug that balance bag is housed fast conical flask seal to also lucifuge and put in constant temperature water bath; After reaction a period of time, with methylene oxide detecting instrument, measure the now concentration of formaldehyde; Carrying out one group of blank assay (do not place catalyst in except conical flask, other all reaction conditions are consistent) in a set of identical experimental provision in addition, by two formaldehyde gas concentration differences, calculate formaldehyde clearance.
The purifying property evaluation of catalyst PARA FORMALDEHYDE PRILLS(91,95) of the present invention is carried out on miniature catalytic reaction experimental provision.After being diluted with quartz sand, catalyst is seated in stainless steel fixed bed, compressed air is controlled and is entered the conical flask that formalin is housed through pressure-reducing valve and flowmeter from air reservoir, carries formaldehyde gas and after surge flask, enters the fixed bed that is filled with catalyst and carry out catalytic oxidation.Fixed bed porch initial concentration of formaldehyde is 100~300ppm, and all the other are air.Reaction is carried out under 20~30 ℃ of normal temperature environments, and reaction gas flow is 300~500mLmin
-1, with methylene oxide detecting instrument, detect into, exit formaldehyde gas concentration, by front and back formaldehyde gas concentration difference, calculate formaldehyde clearance.
Compared with prior art, tool of the present invention has the following advantages: 1) treatment effeciency is high.Under room temperature and normal wet condition, formaldehyde clearance approaches 100%, and treatment effeciency is high, and treating capacity is large, processes completely, there is no secondary pollution, does not have the problems such as absorption is saturated.2) good economy and practicality.Catalyst does not contain noble metal composition, and preparation technology is simple, preparation condition is gentle, and production cost is low; Catalytic reaction is without any need for the external energy input of (as optical, electrical and hot), and energy consumption is low, and use cost is low, is more suitable for the removal of formaldehyde in indoor air.
Accompanying drawing explanation
Fig. 1 is the Experimental equipment of the static catalyze oxidation of formaldehyde reaction of the present invention.
Wherein: 1-catalyst; 2-sample bottle; 3-balance bag; 4-valve; 5-conical flask; 6-methylene oxide detecting instrument.Balance bag is the key of this device, and its effect is the pressure of balance conical flask inside, extracting gases from conical flask smoothly while guaranteeing that methylene oxide detecting instrument detects concentration of formaldehyde.In device, catalyst and sample bottle are placed on conical flask bottom, and balance bag is connected to conical flask by valvular glass tube and silica gel plug, and methylene oxide detecting instrument is connected with conical flask by silicone tube, valve.
Fig. 2 is the miniature catalytic reaction experimental provision of the present invention schematic flow sheet.
Wherein: 7-air reservoir; 8-pressure-reducing valve; 9-flowmeter; 10-constant temperature water bath; 5-conical flask; 11-surge flask; 12-fixed bed; 13-thermocouple.Compressed air is controlled and is entered the conical flask that formalin is housed through pressure-reducing valve and flowmeter from air reservoir, carries formaldehyde gas and after surge flask, enters the fixed bed that is filled with catalyst and carry out catalytic oxidation.The conical flask that formalin is housed is placed in constant temperature water bath, by controlling the temperature of water bath with thermostatic control, controls airborne concentration of formaldehyde.Thermocouple inserts in beds to measure bed temperature.
The specific embodiment
Embodiment 1
Take 1.72gCu (NO
3)
23H
2o and 10.32g50% manganese nitrate aqueous solution join the mixed solution that is made into 10% in distilled water, then drop into the pulverous TiO of 18g
2, 50 ℃ of lower magnetic forces stir 2h, dry 6h at 120 ℃, and roasting 3h at 1000 ℃ of Muffle furnaces, obtains catalyst.In the catalyst of making, the molar ratio that copper manganese component is 10%, Cu and Mn by metal element wt conversion load capacity is 1:4.
The performance test of catalyst is carried out on the static catalyze oxidation of formaldehyde reaction experiment device shown in accompanying drawing 1.The sample bottle 2 that is 1mL by 0.5g catalyst 1 and volume is placed on conical flask 5 bottoms that volume is 1L, 37% formalin solution of 5 μ L is added in sample bottle 2 simultaneously, utilize the silica gel plug that balance bag 3 is housed fast conical flask 5 seal to lucifuge also and put in the constant temperature water bath 10 of 25 ℃; Reaction 24h, opens valve 4, with methylene oxide detecting instrument 6, measures the now concentration of formaldehyde; In a set of identical experimental provision, carrying out one group of blank assay (do not place catalyst 1 in except conical flask 5, other all reaction conditions are consistent) in addition.By two formaldehyde gas concentration differences, calculating formaldehyde clearance is 88.7%.
Embodiment 2
Take 5.62gCu (NO
3)
23H
2o and 16.86g50% manganese nitrate aqueous solution join the mixed solution that is made into 15% in distilled water, then drop into the pulverous TiO of 16g
2, 40 ℃ of lower magnetic forces stir 4h, dry 8h at 100 ℃, and roasting 5h at 700 ℃ of Muffle furnaces, obtains catalyst.In the catalyst of making, the molar ratio that copper manganese component is 20%, Cu and Mn by metal element wt conversion load capacity is 1:2.
The performance test of catalyst is carried out on the miniature catalytic reaction experimental provision of fixed bed of the continuous-flow shown in accompanying drawing 2.After being diluted with quartz sand, 5g catalyst is seated in (caliber 20mm in stainless steel fixed bed 12, long 550mm), compressed air enters through pressure-reducing valve 8 and flowmeter 9 controls the conical flask 5 that formalin is housed from air reservoir 7, carry formaldehyde gas and after surge flask 11, enter the fixed bed 12 that is filled with catalyst and carry out catalytic oxidation, the temperature of beds is measured by thermocouple 13.The conical flask 5 that formalin is housed is placed in constant temperature water bath 10, by controlling the temperature of water bath with thermostatic control, controls airborne concentration of formaldehyde.Fixed bed 12 porch concentration of formaldehyde are 200ppm, and reaction is carried out under 25 ℃ of normal temperature environments, and reaction gas flow is 300mLmin
-1, with methylene oxide detecting instrument, detect into, exit formaldehyde gas concentration, by front and back formaldehyde gas concentration difference, calculating formaldehyde clearance is 92.5%.
Embodiment 3
Take 24.6gCu (NO
3)
23H
2o and 37.02g50% manganese nitrate aqueous solution join the mixed solution that is made into 20% in distilled water, then drop into the pulverous TiO of 28g
2, 30 ℃ of lower magnetic forces stir 6h, dry 10h at 80 ℃, and roasting 8h at 400 ℃ of Muffle furnaces, obtains catalyst.In the catalyst of making, the molar ratio that copper manganese component is 30%, Cu and Mn by metal element wt conversion load capacity is 1:1.
The performance test of catalyst is with embodiment 2, but porch concentration of formaldehyde is 100ppm, and reaction gas flow is 400mLmin
-1, reaction temperature is 20 ℃, by front and back formaldehyde gas concentration difference, calculating formaldehyde clearance is 90.3%.
Take 4.10gCu (NO
3)
23H
2o and 6.17g50% manganese nitrate aqueous solution join the mixed solution that is made into 10% in distilled water, then drop into the granular γ-Al of 18g
2o
3, 40 ℃ of lower magnetic forces stir 5h, dry 8h at 100 ℃, and roasting 5h at 800 ℃ of Muffle furnaces, obtains catalyst.In the catalyst of making, the molar ratio that copper manganese component is 10%, Cu and Mn by metal element wt conversion load capacity is 1:1.
The performance test of catalyst is with embodiment 1, and by two formaldehyde gas concentration differences, calculating formaldehyde clearance is 93.1%.
Take 5.16gCu (NO
3)
23H
2o and 30.96g50% manganese nitrate aqueous solution join the mixed solution that is made into 20% in distilled water, then drop into the granular γ-Al of 14g
2o
3, 30 ℃ of lower magnetic forces stir 6h, dry 6h at 120 ℃, and roasting 8h at 400 ℃ of Muffle furnaces, obtains catalyst.In the catalyst of making, the molar ratio that copper manganese component is 30%, Cu and Mn by metal element wt conversion load capacity is 1:4.
The performance test of catalyst is with embodiment 2, but porch concentration of formaldehyde is 300ppm, and reaction gas flow is 400mLmin
-1, reaction temperature is 30 ℃, by front and back formaldehyde gas concentration difference, calculating formaldehyde clearance is 96.9%.
Embodiment 6
Take 10.32gCu (NO
3)
23H
2o and 61.92g50% manganese nitrate aqueous solution join the mixed solution that is made into 20% in distilled water, then drop into the granular γ-Al of 28g
2o
3, 50 ℃ of lower magnetic forces stir 4h, dry 6h at 120 ℃, and roasting 6h at 500 ℃ of Muffle furnaces, obtains catalyst.In the catalyst of making, the molar ratio that copper manganese component is 30%, Cu and Mn by metal element wt conversion load capacity is 1:4.
The performance test of catalyst is with embodiment 2, but porch concentration of formaldehyde is 300ppm, and reaction gas flow is 500mLmin
-1, reaction temperature is 25 ℃, by front and back formaldehyde gas concentration difference, calculating formaldehyde clearance is 98.6%.
Claims (2)
1. remove a carried copper Mn complex oxide catalyst for formaldehyde, it is characterized in that take that Cu and Mn are as active component, adopt TiO
2or activated alumina is carrier, Cu and Mn content account for 10%~30% of catalyst gross mass, and the molar ratio of Cu and Mn is 1:1~1:4.
2. the preparation method of the carried copper Mn complex oxide catalyst of the removal formaldehyde of claim 1, the Cu (NO that to it is characterized in that molar ratio be 1:1~1:4
3)
23H
2o and 50% manganese nitrate aqueous solution join and in distilled water, be made into mass fraction is 10%~20% mixed solution, and then dropping into quality is the Powdered TiO of 7~9 times of copper manganese gross masses
2carrier or graininess γ-Al
2o
3carrier, 30~50 ℃ of lower magnetic forces stir 2~6h, and dry 6~10h at 80~120 ℃ grinds screening after roasting 3~8h at 400~1000 ℃ of Muffle furnaces.
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Cited By (10)
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CN105478134A (en) * | 2014-09-19 | 2016-04-13 | 合众(佛山)化工有限公司 | Applicable load-type catalyst for purifying air at room temperature |
CN106975493A (en) * | 2017-04-20 | 2017-07-25 | 宁波钛安新材料科技有限公司 | A kind of honeycomb catalyst materials and its forming method |
US20170333885A1 (en) * | 2014-11-12 | 2017-11-23 | Hitachi Zosen Corporation | Aldehyde decomposition catalyst, exhaust gas treatment apparatus, and exhaust gas treatment method |
CN108144628A (en) * | 2017-12-25 | 2018-06-12 | 湖北工业大学 | A kind of preparation method and application for the carbon monoxide-olefin polymeric for handling formaldehyde in waste water |
CN108295863A (en) * | 2017-12-25 | 2018-07-20 | 湖北工业大学 | A kind of preparation method and application of the carbon monoxide-olefin polymeric of processing formaldehyde |
CN108295839A (en) * | 2017-12-25 | 2018-07-20 | 湖北工业大学 | The preparation method and application of the carbon monoxide-olefin polymeric of low concentration formaldehyde in degrading waste water |
CN109939692A (en) * | 2019-02-14 | 2019-06-28 | 北京氦舶科技有限责任公司 | A kind of manganese oxide catalyst and its preparation method and application |
CN111748228A (en) * | 2020-06-29 | 2020-10-09 | 焦作市流金伟业科技有限公司 | Shell powder interior wall paint and preparation method and device thereof |
CN114054020A (en) * | 2021-11-19 | 2022-02-18 | 中国科学院生态环境研究中心 | Perovskite structure material and application thereof in removing formaldehyde at room temperature |
CN115445634A (en) * | 2022-09-27 | 2022-12-09 | 西安向阳航天材料股份有限公司 | Modified hopcalite catalyst and preparation method and application thereof |
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CN105478134A (en) * | 2014-09-19 | 2016-04-13 | 合众(佛山)化工有限公司 | Applicable load-type catalyst for purifying air at room temperature |
US20170333885A1 (en) * | 2014-11-12 | 2017-11-23 | Hitachi Zosen Corporation | Aldehyde decomposition catalyst, exhaust gas treatment apparatus, and exhaust gas treatment method |
CN106975493A (en) * | 2017-04-20 | 2017-07-25 | 宁波钛安新材料科技有限公司 | A kind of honeycomb catalyst materials and its forming method |
CN108144628A (en) * | 2017-12-25 | 2018-06-12 | 湖北工业大学 | A kind of preparation method and application for the carbon monoxide-olefin polymeric for handling formaldehyde in waste water |
CN108295863A (en) * | 2017-12-25 | 2018-07-20 | 湖北工业大学 | A kind of preparation method and application of the carbon monoxide-olefin polymeric of processing formaldehyde |
CN108295839A (en) * | 2017-12-25 | 2018-07-20 | 湖北工业大学 | The preparation method and application of the carbon monoxide-olefin polymeric of low concentration formaldehyde in degrading waste water |
CN108295839B (en) * | 2017-12-25 | 2020-09-11 | 湖北工业大学 | Preparation method and application of catalyst composition for degrading low-concentration formaldehyde in wastewater |
CN109939692A (en) * | 2019-02-14 | 2019-06-28 | 北京氦舶科技有限责任公司 | A kind of manganese oxide catalyst and its preparation method and application |
CN111748228A (en) * | 2020-06-29 | 2020-10-09 | 焦作市流金伟业科技有限公司 | Shell powder interior wall paint and preparation method and device thereof |
CN111748228B (en) * | 2020-06-29 | 2021-08-24 | 焦作市流金伟业科技有限公司 | Shell powder interior wall paint and preparation method and device thereof |
CN114054020A (en) * | 2021-11-19 | 2022-02-18 | 中国科学院生态环境研究中心 | Perovskite structure material and application thereof in removing formaldehyde at room temperature |
CN115445634A (en) * | 2022-09-27 | 2022-12-09 | 西安向阳航天材料股份有限公司 | Modified hopcalite catalyst and preparation method and application thereof |
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Application publication date: 20140226 |