CN106823789B - Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method - Google Patents

Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method Download PDF

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CN106823789B
CN106823789B CN201710143909.6A CN201710143909A CN106823789B CN 106823789 B CN106823789 B CN 106823789B CN 201710143909 A CN201710143909 A CN 201710143909A CN 106823789 B CN106823789 B CN 106823789B
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vapor phase
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phase contaminants
catalysis
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CN106823789A (en
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柳丽芬
聂成
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Dalian University of Technology
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/8678—Removing components of undefined structure
    • B01D53/8687—Organic components
    • 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
    • B01D53/007—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by irradiation
    • 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
    • B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
    • B01D53/326—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 in electrochemical cells
    • 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
    • B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/56—Platinum group metals
    • B01J23/60—Platinum group metals with zinc, cadmium or mercury
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/80—Type of catalytic reaction
    • B01D2255/802—Photocatalytic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/80—Type of catalytic reaction
    • B01D2255/806—Electrocatalytic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
    • B01D2257/708—Volatile organic compounds V.O.C.'s
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01D2258/00—Sources of waste gases
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  • Oil, Petroleum & Natural Gas (AREA)
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Abstract

The present invention provides a kind of methods that photoelectric coupling promotes vapor phase contaminants decomposing, purifying, belong to vapor phase contaminants purified treatment and energy saving resources technical field.Use Pt/TiO2- ZnO and the method for the fixed coating of silica solution form conductive catalytic compound film electrode on stainless (steel) wire, it is connected with anode, through constituting circuit loop with electrolyte solution and external resistance, therefore apply photoelectric action in the energy-efficient catalytic purification system on catalysis electrode, constituting vapor phase contaminants.The degradation purification of the vapor phase contaminants under photocatalysis electro-catalysis and photoelectrocatalysis effect is realized respectively.It is catalyzed under membrane electrode and component booster action, system purification removes the formaldehyde in air.The variation of external resistance directly affects the clean-up effect of photocatalysis and electro-catalysis.Under the conditions of photocatalysis or electro-catalysis, system still can purify degradation of formaldehyde gas and produce electricity.

Description

Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method
Technical field
The invention belongs to vapor phase contaminants purified treatments and energy saving resources technical field, are related to Pt/TiO2ZnO nano The preparation of composite catalyst and photoelectrocatalysis function membrane module and its photoelectrocatalysis synergistic effect, decomposing, purifying pollutant and production Raw electric energy, while facilitation is played to the degradation of VOCs in air, air quality is helped to improve, it is dirty to administer room air Dye plays facilitation.
Background technique
The operation temperature of catalysis oxidation formaldehyde is typically much higher than room temperature, it is difficult to which room temperature needed for meeting indoor air purification is normal Pressure, the requirement that low energy consumption, therefore only developing energy complete oxidation of formaldehyde under room temperature, normal pressure is H2O and CO2Material, It is hopeful to realize the concentration one of the practical application indoor pollutant formaldehyde of the catalytic oxidation technologies aspect of air formaldehyde purification indoors As it is lower, how to improve the removal effect of pollutant under low concentration, become the research focus of researcher.Different purification methods (plant ecological method, physisorphtion, Ozonation, photocatalysis technology, heat catalytic oxidation technology) is made that can play purification With while all there is respective limitations.Currently, by Pt/TiO2- ZnO photoelectrocatalysis is introduced into electric light concerted reaction and removes The report of indoor formaldehyde does not occur also.
In order to improve the removal effect of pollutant under indoor low consistency conditions, early period is tested by photocatalysis technology and electro-catalysis Technology combines, by Pt/TiO2ZnO catalyst is introduced into photoelectric-synergetic reactor, to achieve the purpose that depollution, He Hong Group research loaded noble metal catalyst is used in room temperature catalytic oxidation formaldehyde and indoor air purification, by Pt/TiO2Catalyst Formaldehyde is removed at room temperature, there is preferable removal effect.Currently, with Pt/TiO2- ZnO makees catalyst, and both this technology is mutually tied It closes, the content of formaldehyde in indoor air greatly reduces, it is significant in air purifying process indoors.
TiO2It is taken in terms of the photocatalysis removal of the organic and inorganic pollutant of water and gas phase of the multiphase photocatalysis in environment protection field Obtained greater advance, it is considered to be a kind of environmental pollution advanced purification technology of great future；TiO2Good with its chemical stability, The features such as nontoxic, cheap and easy to get, is known as ideal environmental improvement photochemical catalyst；Nano-TiO2Particle has specific surface area Greatly, the characteristics such as diffusivity is good, use TiO2Make carrier catalyst it is active it is high, the good, anti-toxicity of selectivity is strong, low temperature active Well, the advantages that surface acidity is adjustable, high temperature can restore；But, single TiO2It has some defects in the photocatalytic process, For example, greater band gap, can only absorb ultraviolet light and the more low of photocatalysis efficiency for this purpose, by TiO2It is multiple with other semiconductor materials The research of conjunction gradually increases；Correlative study shows, TiO2With other semiconductor materials it is compound after, synthesized composite material is often There is physically better chemical property and photocatalytic activity than monomer
In addition, ZnO belongs to broad stopband (3. 37 eV) semiconductor material, unique optically and electrically performance is not only It is set to be widely used in nano laser, solar battery etc., and in photoelectric catalysis degrading organic pollutant Also have significant performance in simultaneously, ZnO stable chemical performance, abundant raw material, it is cheap the advantages that, also make it As a kind of catalysis material for having extensive prospect.It should say, from the level of energy of semiconductor forbidden bandwidth and conduction band and valence band From the point of view of, TiO2It is photochemical catalyst more satisfactory at present with ZnO, by TiO2With ZnO is compound can effectively improve to a certain extent The performance of its photoelectrocatalysis.
Most results of study show that the noble metals such as supporting Pt can improve the photocatalytic activity of titanium dioxide, and carrying platinum can also prolong The deactivation time of long photochemical catalyst, and there is good conductive capability, have in the size optoelectronic coupling system of nano particle Help promote the purification of vapor phase contaminants.The application is with Pt/TiO2- ZnO is used as experiment catalyst, it is desirable to can with this catalyst Degradation vapor phase contaminants significantly, to achieve the effect that air cleaning.
Summary of the invention
The present invention devises Pt/TiO2It is net successfully to construct photoelectric coupling catalysis for-ZnO photoelectrocatalysis multifunctional membrane component Change system.The film serves not only as electrode, also has both photocatalysis and conduction, and disposed of in its entirety purification efficiency mentions significantly Height, energy consumption is lower, and the concentration of polluted gas substantially reduces.Degradable vapor phase contaminants in the Systems Theory, extend load The application of type photochemical catalyst, and some thinkings are provided when handling other meteorological pollutants.
Technical solution of the present invention:
Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method, and steps are as follows:
(1) nanometer xPt/TiO is prepared2- ZnO series compound: to ZnSO4Solution adds methanol, adjusts pH=9, then add Positive four butyl ester of metatitanic acid, stirs to get leucosol；Then, under the conditions of 70 DEG C of temperature, stirring forms white powder, dry to grind Mill, calcines 2h under the conditions of 500 DEG C of temperature, cooling, is milled into powder, as TiO2-ZnO；Wherein, ZnSO4Water in solution with plus The volume ratio of the methanol entered is 1:4, obtained TiO2The mass ratio of Zn/Ti is 1/10 in-ZnO；By TiO2- ZnO is dissolved in water In, add H2PtCl6, stirring, and pH=8 are adjusted, under the conditions of 70 DEG C of temperature, HCHO is added, continues to stir 2h, be mixed Object is centrifuged, and is dried, and grinding obtains nanometer xPt/TiO2-ZnO；Wherein, H2PtCl6Volume ratio with HCHO is 1:3, x Pt With the mass ratio of Ti, 0.2 ~ 1.0；
(2) prepared by photoelectrocatalysis membrane module: the nanometer xPt/TiO being prepared to step (1)2In-ZnO series compound 0.2g silica solution is added, ultrasound uniformly, is applied to stainless (steel) wire on piece, nanometer xPt/TiO on area every square centimeter2- The load capacity of ZnO series compound is 3.7mg, is put into oven drying, film is fixed on the membrane module of assembling；
(3) photoelectric coupling catalytic purification system constructs: optoelectronic coupling system is divided into two Room by proton exchange membrane, in a Room It is placed with 0.5mol/L K2SO4Solution is inserted into electrolyte as electrolyte, copper wire；Vapor phase contaminants are contacted in another room and are placed Photoelectrocatalysis membrane module and natural light lamp, the two poles of the earth are connected through copper conductor with external resistance, form circuit, natural light lamp vertical irradiation film Electrode, simulated solar irradiation.
Beneficial effects of the present invention: the system integration light catalytic purifying and electro-catalysis purification and photoelectric-synergetic operation, Indoor gas phase organic matter in degradation removal air, especially VOCs；Volatile organic compounds in indoor air is realized effectively net Change, photochemical catalyst can guarantee that well it does not lose activity in the system, and can produce electricity.
Detailed description of the invention
Fig. 1 is the effect contrast figure for purifying formaldehyde gas of degrading under resistance value different under electro-catalysis (EC) effect, figure In, abscissa is time (min), and ordinate is content of formaldehyde (ppm).
Fig. 2 is photocatalysis (PC), and electro-catalysis (EC), photoelectrocatalysis (PEC) three kinds of different modes of coupling are in confined space Middle external resistance acts on lower treatment and purification and measures formaldehyde gas removal effect comparison diagram.In figure, abscissa is time (min), indulges and sits It is designated as content of formaldehyde (ppm).
Specific embodiment
A specific embodiment of the invention is described in detail below in conjunction with technical solution and attached drawing.
Embodiment one: electric catalyticing system handles indoor formaldehyde gas
Membrane module is put into cylindrical systems, 0.16ppm formaldehyde gas is injected in the inside, and membrane module is put into formaldehyde gas In atmosphere, and being inserted into a copper wire connection electrolyte is 0.5mol/L K2SO4The anode of solution will be coated on stainless (steel) wire Above the photocathode of catalyst crocodile clip junctional membrane, different external resistances is connected between the two poles of the earth and forms circuit.It will before reaction Small fan is opened uniformly to be mixed, and when reaction, connects circuit, every 15 minutes with formaldehyde in methylene oxide detecting instrument detection system Concentration reacts duration 2h, and calculates the removal efficiency of formaldehyde.
Embodiment two: optoelectronic coupling system handles indoor formaldehyde gas
In cylindrical systems, membrane module and natural light are put into system, with copper wire be put into proton exchange membrane every In the electrolyte anode opened, the formaldehyde gas in photochemical catalyst contact system is photocathode, above crocodile clip junctional membrane, and There is external resistance to be attached, natural light lamp is put into reaction unit, 7.5W220V LED line is opened when reaction, before reaction Power supply is closed, is mixed by small fan in reactor, realizes that the formaldehyde gas mixing in reactor is equal, after reaction starts, It is sampled every 15min with methylene oxide detecting instrument, reaction carries out 2h altogether, and calculates the removal rate of formaldehyde.
In Fig. 2, there are photocatalysis, electro-catalysis, photoelectric coupling compares, and discovery optoelectronic coupling system is removed in confined space The efficiency (74%) of formaldehyde is far superior to photocatalysis (42%) and electro-catalysis (13%).

Claims (2)

1. a kind of photoelectric coupling promotes vapor phase contaminants decomposing, purifying method, which is characterized in that steps are as follows:
(1) nanometer xPt/TiO is prepared2- ZnO series compound: to ZnSO4Solution adds methanol, adjusts pH=9, then add metatitanic acid Positive four butyl ester, stirs to get leucosol；Then, under the conditions of 70 DEG C of temperature, stirring forms white powder, and drying is milled, temperature It spends under the conditions of 500 DEG C of temperature and calcines 2h, it is cooling, it is milled into powder, as TiO2-ZnO；Wherein, ZnSO4Water and addition in solution Methanol volume ratio be 1:4, obtained TiO2The mass ratio of Zn/Ti is 1/10 in-ZnO；By TiO2- ZnO is soluble in water, Add H2PtCl6, stirring, and pH=8 are adjusted, under the conditions of 70 DEG C of temperature, HCHO is added, continues to stir 2h, obtains mixture It is centrifuged, is dried, grinding obtains nanometer xPt/TiO2-ZnO；Wherein, H2PtCl6Volume ratio with HCHO is 1:3, Pt and Ti Mass ratio x be 0.2 ~ 1.0；
(2) prepared by photoelectrocatalysis membrane module: the nanometer xPt/TiO being prepared to step (1)2It is added in-ZnO series compound 0.2g silica solution, ultrasound uniformly, are applied to stainless (steel) wire on piece, nanometer xPt/TiO on area every square centimeter2- ZnO system The load capacity of column compound is 3.7mg, is put into oven drying, film is fixed on the membrane module of assembling；
(3) photoelectric coupling catalytic purification system constructs: optoelectronic coupling system is divided into two Room by proton exchange membrane, is placed in a Room 0.5mol/L K2SO4Solution is inserted into electrolyte as electrolyte, copper wire；Vapor phase contaminants are contacted in another room and place photoelectricity Catalysis membrane module and natural light lamp, the two poles of the earth are connected through copper conductor with external resistance, form circuit, natural light lamp vertical irradiation film electricity Pole, simulated solar irradiation.
2. photoelectric coupling according to claim 1 promotes vapor phase contaminants decomposing, purifying method, which is characterized in that described Vapor phase contaminants are the formaldehyde gas in room air.
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Publication number Priority date Publication date Assignee Title
CN107930381B (en) * 2017-11-08 2020-06-16 大连理工大学 Method for accelerating VOC (volatile organic compounds) degradation and generating electricity by coupling photoelectrocatalysis membrane with microbial fuel cell system
CN109847735B (en) * 2019-01-18 2021-05-18 大连理工大学 Nano-catalyst for efficiently degrading ammonia pollutants and application thereof
CN110201688B (en) * 2019-05-31 2022-02-15 大连理工大学 Preparation and control method of catalytic electrode for bioelectrochemistry and photoelectrocatalysis degradation of ethyl acetate and toluene gas

Citations (4)

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Publication number Priority date Publication date Assignee Title
CN102188902A (en) * 2011-05-06 2011-09-21 中国科学院广州能源研究所 Method for treating organic gas by combining photocatalytic fuel cell photoelectrocatalysis and phase transfer
CN102658112A (en) * 2012-04-14 2012-09-12 黑龙江省金昇新能源与环境材料研究院 Preparation method of ZnO-TiO2 composite photocatalyst
CN104617323A (en) * 2015-01-28 2015-05-13 大连理工大学 Non-photocatalytic and photocatalytic fuel cell system capable of generating power and degrading pollutants
CN105498525A (en) * 2015-11-27 2016-04-20 大连理工大学 Catalysis system capable of removing harmful component formaldehyde in air

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102188902A (en) * 2011-05-06 2011-09-21 中国科学院广州能源研究所 Method for treating organic gas by combining photocatalytic fuel cell photoelectrocatalysis and phase transfer
CN102658112A (en) * 2012-04-14 2012-09-12 黑龙江省金昇新能源与环境材料研究院 Preparation method of ZnO-TiO2 composite photocatalyst
CN104617323A (en) * 2015-01-28 2015-05-13 大连理工大学 Non-photocatalytic and photocatalytic fuel cell system capable of generating power and degrading pollutants
CN105498525A (en) * 2015-11-27 2016-04-20 大连理工大学 Catalysis system capable of removing harmful component formaldehyde in air

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