CN1331586C - Composite photocatalytic reaction system for eliminating environmental pollutants in air or water efficiently - Google Patents
Composite photocatalytic reaction system for eliminating environmental pollutants in air or water efficiently Download PDFInfo
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- CN1331586C CN1331586C CNB2005100185009A CN200510018500A CN1331586C CN 1331586 C CN1331586 C CN 1331586C CN B2005100185009 A CNB2005100185009 A CN B2005100185009A CN 200510018500 A CN200510018500 A CN 200510018500A CN 1331586 C CN1331586 C CN 1331586C
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Abstract
The present invention relates to a composite photocatalytic reaction system for efficiently eliminating environmental pollutants in air or water. The present invention can largely enhance the photocatalysis decomposition efficiency and activity stability of photocatalysts to environmental pollutants. The present invention comprises a water decomposing hydrogen making reactor and a pollutant photocatalysis decomposing reactor, and is formed by coupling a water decomposing hydrogen making reactor unit and a pollutant photocatalysis decomposing reactor unit, and an air or oxygen pipeline which is communicated with an air source containing pollutants is arranged at the front of the water decomposing hydrogen making reactor. The previous unit is a photocatalysis water decomposing hydrogen making system which provides needed hydrogen gas to the next photocatalysis reaction unit for decomposing pollutants; the two systems can be combined into a whole, and can be coupling in separated columns. The present invention can achieve high efficiency photocatalysis eliminating effects to pollutants. The present invention can not only used for eliminating pollutants in the air, but also be used for eliminating pollutants in water.
Description
Technical field:
The present invention relates to photocatalysis and environmental pollution treatment technology field thereof.Specifically, the present invention relates to the composite photocatalytic reaction system of environmental contaminants in a kind of efficient elimination air or the water.
Background technology:
Based on the photocatalysis technology of conductor oxidate be widely used at aspects such as clear energy sources, environmental protection and new materials background and important meaning.Yet, TiO
2The photochemical catalyst quantum efficiency is too low, and is not high to solar energy utilization rate, and other semiconductor is easy to photoetch thereby poor stability as CdS, ZnO etc., and these problems are seriously restricting the extensive extensive use of photocatalysis technology.For improving the efficient of photochemical catalyst and photocatalytic process, carried out a large amount of exploratory developments both at home and abroad.To semiconductor light-catalyst carried out comprising mix various metals and nonmetalloid, compound second kind of semiconductor even the third semiconductor, on carrier loadization, change acid, make lattice defect, make it particle nanometer or the like modification widely, modification and preparation research; Also photocatalytic process has been carried out additional various outfields, as electric field, microwave field, ultrasound field and plasma field etc. with fortifying catalytic agent absorptivity, photo-generated carrier separative efficiency with prolong the exploration that its life-span is a purpose.These methods all make the physical and chemical performance of photochemical catalyst and the efficient of photocatalytic process thereof make moderate progress to some extent, but effect is still unsatisfactory.From angle of practical application, with TiO
2Based photocatalyst is an example, and improving the photocatalytic conversion rate of pollutant and catalyst is the problem of the photocatalysis technology large-scale industrial application most critical that must solve at the activity stability of photocatalytic process.
Summary of the invention:
The objective of the invention is to overcome above-mentioned defective, provide a kind of can be enduringly, efficiently and be advantageously used in to various inorganic and organic composite photocatalytic reaction systems of environmental contaminants in the efficient elimination air eliminated of the photocatalysis of trace contaminant or the water in the empty G﹠W.
Technical scheme of the present invention is as follows, it is characterized in that: it comprises water decomposition hydrogen-manufacturing reactor and pollutant photocatalysis Decomposition reactor, be that water decomposition hydrogen-manufacturing reactor and pollutant photocatalysis Decomposition reactor are constituted by the pipeline coupling, before the water decomposition hydrogen-manufacturing reactor, also be provided with the air that contains pollutant or contain the pipeline that the oxygen source of pollutant communicates; Perhaps with water decomposition hydrogen-manufacturing reactor and the synthetic difunctional single-reactor that water decomposition hydrogen manufacturing and pollutant photocatalysis Decomposition function are arranged simultaneously of pollutant photocatalysis Decomposition reactor; Pollutant photocatalysis Decomposition reactor and difunctional single-reactor are shone by light source.
System of the present invention can make photochemical catalyst photocatalysis Decomposition efficient and activity stability to environmental pollutants be greatly improved.The inventor finds in the world first, gaseous mixture with the hydrogen-oxygen gas that contains small quantity of hydrogen in the gas-phase photocatalysis reaction replaces oxygen or air to change oxygen or air aeration as oxidant, in the suspension photocatalysis for hydrogen-oxygen mixture aeration provides photocatalytic process needed oxidant, can increase substantially the photocatalytic conversion rate and the stability of pollutant.
To gas pollutant with photocatalyst granular as fixed bed, the pollutant in the solution is suspended in photocatalyst granular in the solution.The photocatalysis Decomposition of gas pollutant is done carrier gas with the hydrogen-oxygen gaseous mixture or the hydrogen-air mixing that contain pollutant, and the photocatalysis Decomposition of the pollutant in the solution is with hydrogen-oxygen mix gas bell aeration.According to the photoresponse ability of photochemical catalyst, adopt ultraviolet light or adopt visible light to make light source irradiation catalyst bed or suspension, the pollutant in the gaseous mixture or the aqueous solution will be decomposed efficiently, and process will keep permanent high activity and stability.
Add small quantity of hydrogen in carrier gas and the aeration and cause photocatalytic process efficient and stability-enhanced mechanism not to be got clear fully as yet, think that according to Primary Study this is relevant in the absorption of dissociating of catalyst surface etc. with the structure of catalyst and composition, oxygen and hydrogen probably.In photocatalytic process; catalyst under operating temperature, dissociate effectively adsorption of oxygen and hydrogen molecule; the hydrogen atom and the oxygen atom that are attracted to catalyst surface shine light induced electron and the hole that the back produces owing to very vivaciously be easy to accept optical semiconductor; so that form hydroxyl radical free radical and superoxide radical; reduced the recombination rate in light induced electron and hole; quicken the decomposition of pollutant, and make catalyst in photocatalytic process, be difficult for gathering intermediate and have from power of regeneration.
Though in the non-photocatalysis of routine, give that to add hydrogen in the reaction mass very common and be easily, but for photocatalytic process, add cost and energy consumption that hydrogen can increase process greatly, the environmental protection low energy consumption theory that this and photocatalysis environmental pollution treatment technology are pursued runs in the opposite direction.The present invention is a coupling light catalytic reaction system of eliminating air and water pollutant according to a kind of high efficiency photocatalysis that this discovery is invented.This system need not to provide in addition hydrogen source gas, reacts required hydrogen and is produced by system self.
Description of drawings:
Fig. 1 is used for a kind of structural representation of the composite photocatalytic reaction system of air pollutant elimination for the present invention.
Fig. 2 is used for a kind of structural representation of the composite photocatalytic reaction system of solution pollutant elimination for the present invention.
Fig. 3 is used for a kind of structural representation of the composite photocatalytic reaction system of solution pollutant elimination for the present invention.
Fig. 4 is used for the another kind of structural representation of the composite photocatalytic reaction system of solution pollutant elimination for the present invention.
Fig. 5 is the structural representation of three kinds of photocatalysis hydrogen production unit in the used composite photocatalyst of the present invention system
Fig. 6 is the structural representation of the water electrolysis hydrogen production unit in the used composite photocatalyst of the present invention system
Label declaration:
1-contains the air of pollutant; The 2-cleaned air passes; The 3-light source; 4-hydrogen manufacturing unit; The 5-conduit; The 6-quartz glass tube; The 7-power supply; 8-oxygen or air aeration pipe; The 9-dc source; 10-connects the pollutant photocatalytic reaction unit; The 11-photochemical catalyst; 12-photochemical catalyst+the contain pollutant aqueous solution; 13-(photodissociation water catalyst+photocatalysis pollutant decomposition catalyst+pollutant aqueous solution) or (bifunctional catalyst+pollutant aqueous solution); 14-photodissociation water catalyst+aqueous solution; The 15-electrode; The 16-photocatalyst film; 17-contains the pollutant aqueous solution; The 18-aqueous solution; 19-coated electrode 1 and coated electrode 2; 20-metal electrode 1; 21-electrode 2; 22-electrolyte+aqueous solution.
The specific embodiment:
Shown in Fig. 1,2 and 3, the present invention includes hydrogen-manufacturing reactor and pollutant photocatalysis Decomposition reactor, constitute composite photocatalytic reaction system by hydrogen-manufacturing reactor and pollutant photocatalysis Decomposition reactor, before the water decomposition hydrogen-manufacturing reactor, also be provided with air or oxygen or contain the pipeline that the source of the gas of pollutant communicates.
Hydrogen-manufacturing reactor is a water electrolysis hydrogen production system or photocatalysis water decomposition hydrogen generating system or two electrode system for producing hydrogen, and described two electrode system for producing hydrogen are that electrode surface is scribbled the water decomposition catalyst for preparing hydrogen, constitutes one two electrode photocatalysis system for producing hydrogen.Hydrogen-manufacturing reactor provides needed micro-hydrogen for pollutant photocatalysis Decomposition reactor, and two reactors connect by a preposition source of the gas, and this source of the gas can be air or oxygen or the air that contains pollutant.) photocatalysis water decomposition hydrogen generating system or two electrode system for producing hydrogen shine by light source.
Shown in Fig. 1,2 and 3, this composite photocatalytic reaction system can be a complete photocatalysis coupled reaction system, is made up of from hydrogen supply unit and photocatalysis pollutant resolving cell photocatalysis.Previous element is a photocatalysis water decomposition hydrogen generating system, and it provides needed hydrogen for the photocatalytic reaction unit of a back decomposing pollutant.Catalyst system therefor may be two kinds of compounds that The Nomenclature Composition and Structure of Complexes is different, a kind of photocatalytic hydrogen production by water decomposition that is used for, and another kind is used for the photocatalysis Decomposition pollutant; At this moment, two independently connect by pipeline between electrolysis aquatic products hydrogen unit and the photocatalysis Decomposition pollutant unit.Pollutant photocatalysis Decomposition reactor is shone by light source, is also shone by light source as the photocatalysis water decomposition hydrogen generating system or the two electrode system for producing hydrogen of water decomposition hydrogen-manufacturing reactor.
As shown in Figure 4, this composite photocatalytic reaction system also can be a single coupled system, have the difunctional single-reactor of water decomposition hydrogen production reaction and pollutant photocatalysis Decomposition dual-use function in a reactor simultaneously, difunctional single-reactor is shone by light source.Catalyst system therefor is difunctional photochemical catalyst or the two kinds of mixture of catalysts that have two kinds of performances concurrently, and they play photodissociation water and degradation of organic substances (Fig. 4 A) simultaneously in the aqueous solution; This system also can be made of the electrode that is attached with difunctional photochemical catalyst, and (Fig. 4 B) carried out in water decomposition and the coupling of organic matter photocatalysis Decomposition.
This composite photocatalytic reaction system also can be the coupled reaction system that an electrolysis aquatic products hydrogen unit and photocatalysis Decomposition pollutant unit constitute, and two unit also can integrate, but also apportion combination.To the system that integrates, produce hydrogen and pollutant photocatalysis Decomposition and occur in the same reactor; And to the apportion combined system, electrolysis system provides hydrogen for photocatalysis pollutant decomposing system independently, at this moment, connects by pipeline between separate electrolysis aquatic products hydrogen unit and the photocatalysis Decomposition pollutant unit.
No matter above-mentioned the sort of working method can both reach the effect that the high efficiency photocatalysis of pollutant is eliminated, and both can be used for the elimination of air pollutant, also can be used for the elimination of water pollutant.
Place the aqueous solution on the electrode material with loading on as film in a kind of photochemical catalyst adding aqueous solution or with it, light source is placed light source on solution or the container peripheral equipment, constitute a photocatalysis water decomposition system.Its feature functionality is: the catalyst in the water photocatalysis light decomposing system is applied the artificial light source of sunshine or wavelength 200～800nm, water is decomposed on the surface of catalyst produce hydrogen and oxygen.Can there be multiple structure this photocatalysis hydrogen production unit.Photocatalysis hydrogen production unit as shown in Figure 5 is the suspension system, be about to photochemical catalyst and add in the entry, with ultraviolet light or visible light from managing outside or manage internal radiation and make water resolve into hydrogen and oxygen.Can also adopt the electrode system that scribbles photochemical catalyst, as the photocatalysis hydrogen production unit.
With pack into quartz glass reactor or load on other carrier and install light source (artificial light source comprises various forms of mercury lamps, fluorescent lamp, or visible light source, sunshine) additional and constitute gas-phase photocatalysis reaction member (see figure 1) of another kind of photochemical catalyst; Or catalyst granules (loadization or unsupportedization) adding is contained in the solution of pollutant and add that light source constitutes the liquid phase photocatalytic reaction unit, sees Fig. 2 and Fig. 3.The feature and the function of this unit are: catalyst is applied the artificial light source of sunshine or wavelength 200～800nm, make the pollutant photocatalysis Decomposition in gas phase or the water; The titanium dioxide that photochemical catalyst in the described photo catalysis reactor can mix be modified for titanium dioxide, through transition metal (as Fe, Co, Ni, Pt, Pd, Ru, Rh etc.), with the compound solid of other oxide, by the titanium dioxide of loadization and film; Also can be other photochemical catalyst, as CdS, ZnO, Fe
2O
3, SnO
2, ZrO
2And the compound of modification; Also can be InVO
3, the SnCdS solid, or the electrode material that comprises metallic substrates that behind these catalyst of load on the metallic substrates, forms.Also can there be multiple structure in this pollutant photocatalysis Decomposition system.To the pollutant in the gas, catalyst can adopt fills the fixed-bed type filling, also can adopt filming to load on catalyst on the materials such as porous ceramics, activated carbon, activated carbon fiber, glass fibre, metallic substrates, and arrange with flat, multiple field.Light source can be installed in the outside also can be installed in the internal irradiation catalyst.
To gas pollutant, needed carrier gas is supplied with by an air pressure pump, air steel cylinder, oxygen bottle and previous element, promptly allow the air or oxygen stream that contains pollutant take the hydrogen and the oxygen that generate by this unit out of and obtain a hydrogen-oxygen-pollutant gaseous mixture that contains small quantity of hydrogen by first unit, it will be as the carrier gas of Unit second by second unit, makes wherein pollutant and hydrogen generation light-catalyzed reaction and eliminating.To the pollutant in the solution, as the pollutant in the water, second unit is the liquid phase photocatalytic reaction unit, carrier gas is also supplied with by an air pressure pump, air steel cylinder, oxygen bottle and previous element, it forms oxygen or the air that contains small quantity of hydrogen during by first unit, and this carrier gas is as the aeration gas of the second unit solution.
By source of the gas and said two units the composite photocatalyst system that constitutes be can be used for the high efficiency photocatalysis of gas phase and the contained pollutant of solution is handled.Pollutant comprises: contain aerial and be contained in various organic and inorganic pollutant in the water, as aldehyde, phenol, alcohol, ether, alkane, aromatic hydrocarbons, heterocyclic compound, dyestuff, agricultural chemicals, warfare agent, nitrogen oxide, sulfur oxide or the like.
At one common electrolytic water device of two platinum electrodes compositions of insertion in the aqueous solution that contains small amount of electrolyte is housed, applies certain voltage and make water electrolysis produce hydrogen and oxygen, constitute a hydrogen manufacturing unit that meets the second unit needs as required.The feature and the function of this device are: can control the burst size of hydrogen and oxygen easily, and the gas that produces can be brought into photocatalysis pollutant resolving cell by preposition gas easily.
Photocatalysis pollutant resolving cell is identical with embodiment 1.
The water electrolysis hydrogen production unit that is used for this composite photocatalytic reaction system adopts conventional electrolysis water device shown in Figure 6.
As shown in Figure 4, photocatalysis Decomposition to pollutant in the solution, can adopt a single reactor, simultaneously a kind of photochemical catalyst of photodissociation water, the photochemical catalyst that pollutant decomposes are suspended in the aqueous solution that contains pollutant, with ultraviolet light or radiation of visible light suspension, the hydrogen and the contaminated thing photocatalytic process of oxygen that are produced by photodissociation water catalyst are utilized from outside or inner; Also can adopt difunctional photochemical catalyst, pollutant is decomposed fast; Can also adopt electrode system, photocatalyst coating at electrode surface, is applied certain bias voltage and illumination, system photocatalysis product hydrogen process and pollutant photocatalysis Decomposition process are coupled, reach the purpose of efficient decomposing pollutant.
Claims (7)
1, the composite photocatalytic reaction system of environmental contaminants in a kind of efficient elimination air or the water, it is characterized in that: it comprises water decomposition hydrogen-manufacturing reactor and pollutant photocatalysis Decomposition reactor, be that water decomposition hydrogen-manufacturing reactor and pollutant photocatalysis Decomposition reactor are constituted by the pipeline coupling, before the water decomposition hydrogen-manufacturing reactor, also be provided with the air that contains pollutant or contain the pipeline that the oxygen source of pollutant communicates; Perhaps with water decomposition hydrogen-manufacturing reactor and the synthetic difunctional single-reactor that water decomposition hydrogen manufacturing and pollutant photocatalysis Decomposition function are arranged simultaneously of pollutant photocatalysis Decomposition reactor; Pollutant photocatalysis Decomposition reactor and difunctional single-reactor are shone by light source.
2, the composite photocatalytic reaction system of environmental contaminants in efficient elimination air according to claim 1 or the water, it is characterized in that: to the photocatalysis Decomposition of water pollutant, adopt difunctional single-reactor, be simultaneously a kind of photochemical catalyst of photodissociation water and the photochemical catalyst of pollutant decomposition to be suspended in the reactor that contains the pollutant aqueous solution jointly, in the aqueous solution that contains pollutant or the reactor outside with ultraviolet light or visible light source irradiation suspension, the hydrogen and the contaminated thing photocatalytic process of oxygen that are produced by photodissociation water catalyst are utilized; Perhaps adopt difunctional single-reactor and adopt the difunctional photochemical catalyst in the aqueous solution, play photodissociation water and degradation of organic substances simultaneously, from the aqueous solution that contains pollutant inner or from the reactor outside with ultraviolet light or radiation of visible light suspension; Perhaps adopt electrode system, bifunctional catalyst is coated in electrode surface, electrode inserts and to contain in the reactor of pollutant, applies bias voltage and illumination, makes photocatalysis produce hydrogen process and pollutant photocatalysis Decomposition process and carries out simultaneously and coupled reaction takes place.
3, the composite photocatalytic reaction system of environmental contaminants in efficient elimination air according to claim 1 or the water, it is characterized in that: the water decomposition hydrogen-manufacturing reactor is a water electrolysis hydrogen production system or photocatalysis water decomposition hydrogen generating system or two electrode system for producing hydrogen, described two electrode system for producing hydrogen are that electrode surface is coated with the water decomposition catalyst for preparing hydrogen, constitute one two electrode photocatalysis system for producing hydrogen; Described photocatalysis water decomposition hydrogen generating system or two electrode system for producing hydrogen are shone by light source.
4, the composite photocatalytic reaction system of environmental contaminants in efficient elimination air according to claim 3 or the water is characterized in that: described pollutant photocatalysis Decomposition reactor comprises quartz glass tube or container, light source, solid photochemical catalyst and contains the aqueous solution of pollutant; The solid photochemical catalyst is suspended in the aqueous solution that contains pollutant, and places quartz glass tube or container, light source to be placed in the center or the top of the aqueous solution that contains pollutant, from top or internal irradiation contain the aqueous solution of pollutant; Quartz glass tube or container have a gas vent and inlet.
5, the composite photocatalytic reaction system of environmental contaminants in efficient elimination air according to claim 3 or the water, it is characterized in that: described pollutant photocatalysis Decomposition reactor comprises outer tube, quartz glass tube, light source, pollutant photocatalysis Decomposition catalyst, gas pollutant; Photochemical catalyst is loaded in the described quartz glass tube, or photochemical catalyst loaded on places on the carrier in the described quartz glass tube; Quartz glass tube places in the outer tube, and light source places the gap that quartz glass tube is outer and outer tube is interior, and light shines gas pollutant by quartz glass tube, and quartz glass tube has gas pollutant outlet and inlet.
6, according to the composite photocatalytic reaction system of environmental contaminants in claim 2 or 3 or 4 or 5 described efficient elimination air or the water, it is characterized in that: described catalyst comprises photodissociation water catalyst, pollutant decomposition catalyst or bifunctional catalyst, they are titanium dioxide or by one or more the titanium dioxide solid of transient metal doped modification among Fe or Co or Ni or Pt or Pd or Ru or the Rh, perhaps InVO
3, the SnCdS solid, or on metallic substrates the film of these catalyst of institute's load, or the electrode material that comprises metallic substrates that behind these catalyst of load on the metallic substrates, forms.
7, the composite photocatalytic reaction system of environmental contaminants in efficient elimination air according to claim 6 or the water, it is characterized in that: described light source is that sunshine or wavelength are the artificial light source of 200～800nm, and artificial light source comprises mercury lamp, the fluorescent lamp of different shape.
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| CN101940875B (en) * | 2010-10-25 | 2012-10-17 | 上海电力学院 | Method for decomposing high-concentration methane mixed gas by fast photocatalysis by using low pressure mercury lamp |
| WO2013035291A1 (en) * | 2011-09-06 | 2013-03-14 | パナソニック株式会社 | Semiconductor material, optical hydrogen generating device using same, and method of producing hydrogen |
| CN105905988B (en) * | 2016-05-25 | 2018-11-30 | 安徽普氏生态环境工程有限公司 | A method of based on visible light catalytic-electro-catalysis air oxidation degradation COD of sewage |
| CN105967409A (en) * | 2016-05-25 | 2016-09-28 | 安徽普氏生态环境工程有限公司 | Method for degrading COD (chemical oxygen demand) in sewage on the basis of visible-light-catalyzed air oxidation |
| CN114749169B (en) * | 2022-04-22 | 2023-12-22 | 陕西科技大学 | Thermoelectric base photocatalyst and preparation method and application thereof |
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| CN1460542A (en) * | 2003-05-31 | 2003-12-10 | 福州大学 | Photo-magnetic synergistic catalytic technique and its application for degrading organic pollutant |
| US20040022700A1 (en) * | 2000-06-10 | 2004-02-05 | Kim Hak Soo | Method and apparatus for removing pollutants using photoelectrocatalytic system |
| JP2004325177A (en) * | 2003-04-23 | 2004-11-18 | Toshiba Plant Systems & Services Corp | Treatment device for water solution containing organic acid |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| US20040022700A1 (en) * | 2000-06-10 | 2004-02-05 | Kim Hak Soo | Method and apparatus for removing pollutants using photoelectrocatalytic system |
| JP2004325177A (en) * | 2003-04-23 | 2004-11-18 | Toshiba Plant Systems & Services Corp | Treatment device for water solution containing organic acid |
| CN1460542A (en) * | 2003-05-31 | 2003-12-10 | 福州大学 | Photo-magnetic synergistic catalytic technique and its application for degrading organic pollutant |
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