CN106823789A - 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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CN106823789A
CN106823789A CN201710143909.6A CN201710143909A CN106823789A CN 106823789 A CN106823789 A CN 106823789A CN 201710143909 A CN201710143909 A CN 201710143909A CN 106823789 A CN106823789 A CN 106823789A
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vapor phase
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phase contaminants
catalysis
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CN106823789B (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
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/06—Polluted air

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  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Materials Engineering (AREA)
  • Biomedical Technology (AREA)
  • Organic Chemistry (AREA)
  • Toxicology (AREA)
  • Electrochemistry (AREA)
  • Catalysts (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)
  • Disinfection, Sterilisation Or Deodorisation Of Air (AREA)

Abstract

The invention provides a kind of method that photoelectric coupling promotes vapor phase contaminants decomposing, purifying, belong to vapor phase contaminants purified treatment and energy saving resources technical field.Use Pt/TiO2The method that ZnO and Ludox fix coating forms conductive catalytic compound film electrode on stainless (steel) wire, itself and anode are connected, circuit loop is constituted through with electrolyte solution and external resistance, therefore applies photoelectric action on catalysis electrode, constitute the efficient energy-saving catalytic purification system of vapor phase contaminants.The degraded purification of the vapor phase contaminants under photocatalysis electro-catalysis and photoelectrocatalysis effect is realized respectively.Under catalysis membrane electrode and component booster action, the formaldehyde in system purification removal air.The change 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 treatment and energy saving resources technical field, it is related to Pt/TiO2- ZnO nano The preparation of composite catalyst and photoelectrocatalysis function membrane module, and its photoelectrocatalysis synergy, decomposing, purifying pollutant and product Raw electric energy, while facilitation is played in the degraded to VOCs in air, is favorably improved air quality, dirty to administer room air Dye plays facilitation.
Background technology
The operation temperature of catalysis oxidation formaldehyde is typically much higher than room temperature, it is difficult to which the normal temperature needed for meeting indoor air purification is normal Pressure, the low requirement of energy consumption, thus only develop under room temperature, normal pressure can complete oxidation of formaldehyde be H2O and CO2Material, just have uncommon Prestige realize the concentration of practical application indoor pollutant formaldehyde in terms of catalytic oxidation technologies air formaldehyde purification indoors it is general compared with It is low, the removal effect of pollutant under low concentration how is improved, become the research focus of researcher.Different purification methods (are planted Thing ecological method, physisorphtion, Ozonation, photocatalysis technology, heat catalytic oxidation technology), catharsis can played While all there is respective limitation.At present, by Pt/TiO2- ZnO photoelectrocatalysis removes room in being introduced into electric light concerted reaction The report of interior formaldehyde does not occur also.
In order to improve the removal effect of pollutant under indoor low consistency conditions, experiment early stage is by photocatalysis technology and electro-catalysis Technology is combined, by Pt/TiO2- ZnO catalyst is introduced into photoelectric-synergetic reactor, to reach the purpose of 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.At present, with Pt/TiO2- ZnO makees catalyst, and technology both this is mutually tied Close, the content of formaldehyde in indoor air greatly reduces, it is significant in air purifying process indoors.
TiO2Taken in terms of the photocatalysis removal of the organic and inorganic pollutant of water and gas phase of the multiphase photocatalysis in field of Environment Protection Obtained greater advance, it is considered to be a kind of environmental pollution advanced purification technology of great future；TiO2With its chemical stability it is good, Nontoxic, cheap and easy to get the features such as, it is described as ideal environmental improvement photochemical catalyst；Nano-TiO2Particle has specific surface area The characteristic such as greatly, diffusivity is good, uses TiO2Active high, good, the anti-Poisoning of selectivity of catalyst of making carrier is strong, low temperature active Well, the advantages of surface acidity is adjustable, high temperature is reducible；But, single TiO2Some defects are there is also in photocatalytic process, For example, greater band gap, ultraviolet light and the more low of photocatalysis efficiency can only be absorbed therefore, by TiO2It is multiple with other semi-conducting materials The research of conjunction gradually increases；Correlative study shows, TiO2After compound with other semi-conducting materials, synthesized composite is often There is physically better chemical property and photocatalytic activity than monomer
In addition, ZnO belongs to broad stopband (3.37eV) semi-conducting material, the optically and electrically performance of its uniqueness not only make its It is widely used in nano laser, solar cell etc., and in the application of photoelectric catalysis degrading organic pollution Also there is significant performance simultaneously, ZnO stable chemical performances, abundant raw material the advantages of cheap, also becomes one kind There is the catalysis material of extensive prospect.Should say, from the point of view of the level of energy of semiconductor energy gap and conduction band and valence band, TiO2 It is photochemical catalyst more satisfactory at present with ZnO, by TiO2It is compound with ZnO to effectively improve its photoelectrocatalysis to a certain extent Performance.
Most results of study show that the noble metal such as supporting Pt can improve the photocatalytic activity of titanium dioxide, and carrying platinum can also prolong The deactivation time of photochemical catalyst long, and with good conductive capability, have in the size optoelectronic coupling system of its 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 Degrade significantly vapor phase contaminants, to reach the effect of purification of air.
The content of the invention
The present invention devises Pt/TiO2- ZnO photoelectrocatalysis multifunctional membrane components, successfully construct photoelectric coupling catalysis net Change system.The film serves not only as electrode, also has photocatalysis and conduction concurrently, and disposed of in its entirety purification efficiency is carried significantly Height, energy consumption is relatively low, and the concentration of its dusty gas is substantially reduced.Degradable vapor phase contaminants in the Systems Theory, extend load The application of type photochemical catalyst, and some thinkings are provided when other meteorological pollutants are processed.
Technical scheme：
Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method, and step is as follows：
(1) nanometer xPt/TiO is prepared2- ZnO series compounds：To ZnSO4Solution adds methyl alcohol, adjusts pH=9, then add Positive four butyl ester of metatitanic acid, stirring obtains leucosol；Then, under 70 DEG C of temperature conditionss, stirring forms white powder, dries and grinds Mill, calcines 2h under 500 DEG C of temperature conditionss, cools down, and is milled into powder, as TiO2-ZnO；Wherein, ZnSO4Water in solution with plus The volume ratio of the methyl alcohol for entering is 1:4, the TiO for obtaining2The mass ratio of Zn/Ti is 1/10 in-ZnO；By TiO2- ZnO is soluble in water, Add H2PtCl6, stirring, and pH=8 is adjusted, under 70 DEG C of temperature conditionss, HCHO is added, continue to stir 2h, obtain mixture Through centrifugation, drying, grinding obtains nanometer xPt/TiO2-ZnO；Wherein, H2PtCl6It is 1 with the volume ratio of HCHO：3, x be Pt with The mass ratio of Ti, 0.2~1.0；
(2) prepared by photoelectrocatalysis membrane module：To the nanometer xPt/TiO that step (1) is prepared2In-ZnO series compounds Addition 0.2g Ludox, ultrasound is uniform, is applied in stainless steel mesh sheet, nanometer xPt/TiO on area every square centimeter2- The load capacity of ZnO series compounds is 3.7mg, is put into oven drying, and film is fixed on the membrane module of assembling；
(3) photoelectric coupling catalytic purification system builds：Optoelectronic coupling system is divided into two Room by PEM, in a Room It is placed with 0.5mol/L K2SO4Solution is inserted in electrolyte as electrolyte, copper wire；Vapor phase contaminants are contacted in another room and is placed Photoelectrocatalysis membrane module and natural light lamp, the two poles of the earth connect through copper conductor and 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 degraded removal air, especially VOCs；Volatile organic compounds in indoor air is realized effectively net Change, photochemical catalyst can well ensure that it does not lose activity in the system, and can produce electricity.
Brief description of the drawings
Fig. 1 is the Contrast on effect topic of purifying formaldehyde gas of degrading, figure under electro-catalysis (EC) effect under different resistance values In, abscissa is the time (min), and ordinate is content of formaldehyde (ppm).
Fig. 2 is photocatalysis (PC), and electro-catalysis (EC), photoelectrocatalysis (PEC) couples three kinds of different modes in confined space The middle lower treatment and purification of external resistance effect determines formaldehyde gas removal effect comparison diagram.In figure, abscissa is the time (min), indulges and sits It is designated as content of formaldehyde (ppm).
Specific embodiment
Specific embodiment of the invention is described in detail below in conjunction with technical scheme and accompanying drawing.
Embodiment one：Electric catalyticing system processes indoor formaldehyde gas
Membrane module, the inside injection 0.16ppm formaldehyde gases are put into cylindrical systems, and membrane module is put into formaldehyde gas atmosphere In enclosing, and it is 0.5mol/L K to insert a copper wire connection electrolyte2SO4The anode of solution, will be coated with stainless (steel) wire and urge The photocathode of agent crocodile clip junctional membrane top, connects different external resistances and forms circuit between the two poles of the earth.Will be small before reaction Fan is opened uniformly to be mixed, and during reaction, connects circuit, dense with formaldehyde in methylene oxide detecting instrument detecting system every 15 minutes Degree, reacts duration 2h, and calculate the removal efficiency of formaldehyde.
In Fig. 2, electro-catalysis removal effect is optimal, is 53%.And removal efficiency is far superior to 13.4%, 39%, 29% Removal efficiency.
Embodiment two：Optoelectronic coupling system processes indoor formaldehyde gas
In cylindrical systems, membrane module and natural light are put into system, with copper wire be put into PEM 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 lines are opened during reaction, before reaction Power supply is closed, is mixed by small fan in reactor, realize that the formaldehyde gas mixing in reactor is equal, after reaction starts, It is sampled with methylene oxide detecting instrument every 15min, reaction carries out 2h altogether, and calculates the clearance of formaldehyde.
In Fig. 2, there is photocatalysis, electro-catalysis, photoelectric coupling is contrasted, it is found that 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, it is characterised in that step is as follows：
(1) nanometer xPt/TiO is prepared2- ZnO series compounds：To ZnSO4Solution adds methyl alcohol, adjusts pH=9, then add metatitanic acid Positive four butyl ester, stirring obtains leucosol；Then, under 70 DEG C of temperature conditionss, stirring forms white powder, and drying is milled, temperature 2h is calcined under 500 DEG C of temperature conditionss of degree, is cooled down, be milled into powder, as TiO2-ZnO；Wherein, ZnSO4Water and addition in solution Methyl alcohol volume ratio be 1:4, the TiO for obtaining2The mass ratio of Zn/Ti is 1/10 in-ZnO；By TiO2- ZnO is soluble in water, then Add H2PtCl6, stirring, and pH=8 is adjusted, under 70 DEG C of temperature conditionss, HCHO is added, continue to stir 2h, obtain mixture warp Centrifugation, drying, grinding obtains nanometer xPt/TiO2-ZnO；Wherein, H2PtCl6It is 1 with the volume ratio of HCHO：3, x is Pt and Ti Mass ratio, 0.2~1.0；
(2) prepared by photoelectrocatalysis membrane module：To the nanometer xPt/TiO that step (1) is prepared2Added in-ZnO series compounds 0.2g Ludox, ultrasound is uniform, is applied in stainless steel mesh sheet, nanometer xPt/TiO on area every square centimeter2- ZnO systems The load capacity of row compound is 3.7mg, is put into oven drying, and film is fixed on the membrane module of assembling；
(3) photoelectric coupling catalytic purification system builds：Optoelectronic coupling system is divided into two Room by PEM, is placed with a Room 0.5mol/L K2SO4Solution is inserted in electrolyte as electrolyte, copper wire；Vapor phase contaminants are contacted in another room and photoelectricity is placed Catalysis membrane module and natural light lamp, the two poles of the earth connect through copper conductor and 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, it is characterised in that described Vapor phase contaminants are the formaldehyde gas in room air.
CN201710143909.6A 2017-03-14 2017-03-14 Photoelectric coupling promotes vapor phase contaminants decomposing, purifying method Active CN106823789B (en)

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2019091119A1 (en) * 2017-11-08 2019-05-16 大连理工大学 Method for accelerating voc degradation and generating electricity via microbial fuel cell-photoelectrocatalytic membrane combined system
CN109847735A (en) * 2019-01-18 2019-06-07 大连理工大学 A kind of novel nano catalyst of efficient degradation ammonia pollutant and application
CN110201688A (en) * 2019-05-31 2019-09-06 大连理工大学 A kind of preparation and control method of bioelectrochemistry and photoelectric catalysis degrading ethyl acetate and the catalysis electrode of toluene gas

Citations (4)

* Cited by examiner, † Cited by third party
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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

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2019091119A1 (en) * 2017-11-08 2019-05-16 大连理工大学 Method for accelerating voc degradation and generating electricity via microbial fuel cell-photoelectrocatalytic membrane combined system
CN109847735A (en) * 2019-01-18 2019-06-07 大连理工大学 A kind of novel nano catalyst of efficient degradation ammonia pollutant and application
CN109847735B (en) * 2019-01-18 2021-05-18 大连理工大学 Nano-catalyst for efficiently degrading ammonia pollutants and application thereof
CN110201688A (en) * 2019-05-31 2019-09-06 大连理工大学 A kind of preparation and control method of bioelectrochemistry and photoelectric catalysis degrading ethyl acetate and the catalysis electrode of toluene gas
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

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