CN1562795A - Photoelectrocatalysis and oxidation device for treating organic substance in water - Google Patents
Photoelectrocatalysis and oxidation device for treating organic substance in water Download PDFInfo
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- CN1562795A CN1562795A CN 200410012222 CN200410012222A CN1562795A CN 1562795 A CN1562795 A CN 1562795A CN 200410012222 CN200410012222 CN 200410012222 CN 200410012222 A CN200410012222 A CN 200410012222A CN 1562795 A CN1562795 A CN 1562795A
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- 150000004706 metal oxides Chemical class 0.000 claims description 6
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Abstract
一种光电催化氧化处理水中有机物的装置，属于环境化工光催化氧化水处理技术领域。具体来说是一种流化床光电催化有机水处理装置。该反应装置主要由钛基氧化物阳极6、空气氧电极阴极7、TiO2/C流化颗粒8、紫外灯光源9、恒电位仪直流电源10、空气分布板3、壳体11等构成。此反应器不仅利用阳极的氧化作用、空气氧电极阴极的还原作用，而且利用电场所产生的·OH、H2O2、OH－等活性基团与光、光催化发生协同作用，在TiO2流化颗粒的剧烈扰动下深入床层内部，使体系的·OH浓度提高并趋于均匀，同时流化床颗粒表面的TiO2在光照下也在源源不断产生·OH，且TiO2颗粒表面不断更新，反应体系有机协调，降解反应全面展开。这一新颖反应装置高效、快速适合含较高浓度、难降解有机污染物的处理，不产生二次污染，也可将多个反应器串联使用，机动灵活。
The invention discloses a device for photocatalytic oxidation treatment of organic matter in water, which belongs to the technical field of environmental chemical photocatalytic oxidation water treatment. Specifically, it is a fluidized bed photocatalytic organic water treatment device. The reaction device is mainly composed of titanium-based oxide anode 6, air oxygen electrode cathode 7, TiO 2 /C fluidized particles 8, ultraviolet light source 9, potentiostat DC power supply 10, air distribution plate 3, housing 11 and so on. This reactor not only utilizes the oxidation of the anode and the reduction of the cathode of the air oxygen electrode, but also uses the active groups such as OH, H 2 O 2 , OH - generated by the electric field to cooperate with light and photocatalysis. Under the violent disturbance of the fluidized particles, it goes deep into the bed , so that the concentration of OH in the system increases and tends to be uniform. Renewal, the reaction system is organically coordinated, and the degradation reaction is in full swing. This novel reaction device is efficient and fast and is suitable for the treatment of high-concentration and refractory organic pollutants without secondary pollution. Multiple reactors can also be used in series, which is flexible.
Description
Technical Field
The invention discloses a device for treating organic matters in water through photoelectrocatalysis oxidation, and belongs to the technical field of environmental chemical industry photocatalysis oxidation water treatment. In particular to a fluidized bed photoelectrocatalysis organic water treatment device.
Technical Field
Since the middle of the 20 th century, with the rapid development of industry, a large number of non-living organic matters which do not exist in the nature are generated, and most of the non-living organic matters are organic matters which are difficult to degrade and pose great threat to the ecological environment and human survival.
Photo-active semiconductors (typically TiO is used)2) Photogenerated holes in the valence band (Fujishima a, Honda K, Nature, 1972, 238: 37 to 38; matthews r.w.j.catal.1988, 111: 264-272; ollis D F, Al-Ekabi H.Amsterdam: elsevier, 1993) generates OH free radicals with strong oxidizing ability (standard electrode potential of 2.80eV) in water, can completely mineralize organic pollutants which are difficult to degrade in water, has almost no selectivity to substrates, can carry out the degradation process at normal temperature and normal pressure, does not need to add chemical reagents, has no secondary pollution, and becomes the leading edge of research and development of the current domestic and foreign water purification technology.
To date, numerous studies have revealed that one of the major problems with this process is that the quantum efficiency is too low and the reaction rate is not high. In recent years, researchers have utilized light sources reasonably and nano TiO2Preparation and doping of (2), TiO2A great deal of research has been carried out on immobilization and other aspects, as well as the use of electrochemically assisted photocatalytic methods, or photoelectrocatalytic methods, to prevent simple recombination of photogenerated electrons and holes to improve quantum efficiency (Vinodgopal K, Hotchandani S and Kamat P V.J.Phys.chem., 1993, 97 (26): 9040-. Generally, photocatalytic technologies based on titanium dioxide are suitable for purifying low and/or slightly contaminated media (zhanpengzhe, yungjiang environmental science progress 1998, 6 (5): 50-56).
Much attention has been paid to TiO in the past2The promotion effect of the photoanode on the quantum efficiency improvement of the process is not paid enough attention to the contribution of the photoelectrochemical process cathode, so that the total reaction speed of the process is increasedThe rate cannot be improved. In recent years, air-oxygen electrode cathodes have been introduced into the electro-optic chemistry system (Chuanen, Wangpin, Wang Eifeng, et al. applied chemistry, 1999, 16 (2): 87-89; Tomas Harrington, Derek pletcher.Jthe electrochem. society, 1999, 146 (8): 2983-.
Fluidized bed photoelectrocatalysis reaction device utilizing TiO2the/C is taken as fluidized particles, so that the problem that the photocatalyst is difficult to separate from water can be solved, the solution concentration tends to be uniform by utilizing the severe disturbance of the fluidized particles, and the thickness of a mass transfer membrane on the surface of the particles is effectively reduced, thereby providing a huge electrode activation area and mass transfer rate to improve the photocatalytic quantum efficiency. H produced by the cathodic reduction reaction of the air oxygen electrode2O2OH generated by the anodic oxidation reaction of active groups such as OH, OH-and the like and titanium-based oxide on TiO2The fluidized particles can enter into the bed layer under the severe disturbance, the OH concentration of the system tends to be uniform, and meanwhile, TiO on the surfaces of the fluidized bed particles2OH and TiO are continuously generated under illumination2The particle surface is continuously updated, the reaction system is organically coordinated, and the degradation reaction is comprehensively developed, so that the novel reactor is high-efficient and quick and is suitable for treating wastewater (hospital sewage) containing organic pollutants with higher concentration, particularly refractory organics and toxic inhibitors.
Disclosure of Invention
The invention aims to provide a device for treating organic matters in water through photoelectrocatalysis oxidation, which realizes high-efficiency degradation of organic pollutants in water through the combined action of photocatalysis and electrocatalysis. The combined action can improve the concentration of OH free radicals required by the degradation process, thereby improving the degradation efficiency of process organic matters. In addition, the ultraviolet light can also directly oxidize organic matters with absorption wavelength more than 254nm in the water. The photoelectrochemical reactor can effectively degrade organic matters in water into CO2、H2Small molecular substances such as O, inorganic ions and the like, high treatment efficiency and no secondary pollution problem.
The invention relates to a device for treating organic matters in water by photoelectrocatalysis oxidation, which is a reaction device mainly used for a fluidized bed photoelectrocatalysis organic water treatment system and is prepared from titanium-based oxide TiO2/SnO2a/Ti anode (6), an air oxygen electrode cathode (7), TiO2The device comprises/C fluidized particles (8), an ultraviolet lamp light source (9), a potentiostat direct-current power supply (10), an air distribution plate (3), a shell (11), a wastewater inlet (4), a wastewater outlet (5), an air inlet (1), particle fillers (2) and a wire mesh plate (12); the integral porous air distribution plate (3) is positioned at the lower part of the device and forms an air distribution chamber with the shell, the air distribution chamber is filled with particle fillers (2), and the air distribution chamber is provided with an air inlet (1) communicated with the outside; the air oxygen electrode cathode (7) and the titanium-based oxide anode (6) are opposite and respectively close to the wall of the device; the ultraviolet lamp light source (9) is arranged between the cathode and the anode, namely the middle of the device; the air oxygen electrode and the titanium-based oxide electrode are respectively provided with an electric connector connected with a constant potential rectifier direct current power supply (10), and the upper part of the electrode chamber is provided with a TiO-preventing electrode2the/C photocatalytic particles are carried out of the wire mesh plate (12) outside the device.
The cathode electrode is an air oxygen electrode cathode (7) which is composed of a catalytic layer and a conductive framework, wherein the catalytic layer is composed of activated carbon, metal oxide, graphite powder and polytetrafluoroethylene, and the metal oxide is TiO2ZnO or MnO2The catalyst layer contains 70-85% of active carbon, 2-10% of metal oxide, 5-15% of graphite powder and 5-10% of polytetrafluoroethylene; the conductive framework is a nickel net or a silver-plated copper net.
The distance between the cathode and the anode is 4-15 cm.
The wavelength of the uv light source described above is 254 nm.
TiO as described above2The particle size of the/C fluidized particles (8) is 1-2 mm; the air distribution plate (3) is made of ceramic material, and the inner aperture of the air distribution plate is 15-50 mu m; the mesh of the wire mesh plate (12) arranged at the upper part of the electrode chamber is smaller than the TiO2Particle size of the/C fluidized particles.
The device for treating organic matters in water through photoelectrocatalysis oxidation can be provided with a water inlet at the lower part of the shell and a water outlet at the upper part of the shell, so that organic wastewater can be continuously treated.
The process for realizing the treatment of the organic matters in the water comprises the following steps: the wastewater containing organic matters is fed into the photoelectrochemical reactor from a water inlet and added with TiO2the/C fluidizes the particles, at the same time, the air compressor is started to blow compressed air from the air inlet, and the air flow is adjusted. Secondly, turning on an ultraviolet lamp, switching on a direct current power supply, and under the combined action of the ultraviolet light and an electric field, oxidizing and degrading organic pollutants into nontoxic and harmless CO2、H2O, inorganic ions, and the like.
The invention has the advantages that: the fluidized bed photocatalytic reactor and the electrochemical reactor are combined into a whole, so that the structure of a reaction device is compact and reasonable, more importantly, the electrochemical reaction and the photocatalytic reaction can be organically combined to continuously generate required strong oxidizing property OH free radicals, and the reaction and mass transfer of the reaction device are coordinated, so that the organic matters in water can be efficiently degraded. The concrete advantages are that:
1) the anode has two main functions: firstly, photo-generated electrons are captured to produce OH; secondly, organic pollutants in water are directly oxidized electrochemically.
2) The air oxygen electrode has two main functions: first, production of H2O2、OH-And nascent oxygen.
3) Air oxygen electrode and light combined action production
4)TiO2The fluidized particles have the functions of ① multipole, each particle is a microbattery to perform oxidation-reduction reaction, ② organic matter and O are enriched2③ production of OH and its combination with an air oxygen electrode, ④ eliminates the effect of mass transfer.
Therefore, the invention can rapidly and thoroughly remove the organic matters in the water, does not need to add chemical reagents, has no secondary pollution, no solid-liquid separation problem and high treatment efficiency, and is a comprehensive, harmonious and sustainable device for organic water treatment.
Drawings
FIG. 1 is a schematic structural diagram of a reactor for treating organic matters in water by photoelectrocatalysis oxidation according to an embodiment of the present invention.
FIG. 2 is a schematic cross-sectional view of a longitudinal structure of the photoelectrocatalysis reactor of the present invention.
The reference numbers in the figures are: 1 air inlet, 2 particle fillers, 3 air distribution plates, 4 wastewater inlets, 5 wastewater outlets, 6 titanium-based oxide anode, 7 air oxygen electrode cathode, 8 TiO2The reactor comprises/C fluidized particles, 9 ultraviolet lamp light sources, 10 constant potential rectifier direct current power supplies, 11 reactor shells and 12 wire mesh plates.
Detailed Description
Referring to fig. 1, the reaction device for treating organic matters in water by fluidized bed photoelectrocatalysis oxidation has the following structure: with titanium-based oxides TiO2/SnO2the/Ti anode 6 is an anode, the air oxygen electrode cathode 7 is a cathode, and the cathode and the anode are respectively provided with an electric connector which can be connected with a direct current power supply 10; compressed air is used as an air source; exterior coating of TiO particles made from commercial activated carbon and graphite powder2Formed TiO2the/C fluidized particles 8 are photocatalyst particles. Compressed air enters the bottom air chamber of the reactor from the air inlet 1 and blows air into the reactor through the micropore air distribution plate 3. The two electrodes are opposed and each is close to one wall of the device. TiO 22TiO fluidized particles are arranged on an air distribution plate and are in a fluidized state under the action of air flow2The concentration of (A) is 0.5-1.5 g/L. The uv lamp source 9 is placed vertically between the two electrodes, i.e. in the middle of the rectangular arrangement. A wire mesh plate 12 is placed on top of the electrode chamber. The whole rectangular reactor shell 11 is formed by welding organic glass. The organic wastewater to be treated enters from a wastewater inlet 4 and exits from a wastewater outlet 5 of the reaction device.
The phenol aqueous solution is treated. The setting conditions are as follows: 15W ultraviolet light source, TiO2Particle size of 1mm, P25 TiO, photocatalytic fluidized particles2Concentration of (2) is 1.0g/L and air flow is 0.3m3/h，TiO2/SnO2The anode is Ti, the cathode is air oxygen electrode, the distance between the anode and the cathode is 5cm, and the electrode area is 20cm2Current density 15mA/cm2. After 1 hour of photoelectrocatalysis reaction, the removal rate of 50mg/L and 120mL of phenol water solution COD is 95.6%.
The water-soluble humic acid solution was treated in accordance with the apparatus configuration and treatment process of embodiment 1. Is provided withThe conditions are as follows: 15W ultraviolet light source, TiO2Particle size of 1.5mm, P25 TiO, photocatalytic fluidized particles2Concentration of (2) is 1.5g/L and air flow is 0.5m3/h，TiO2/SnO2The anode is Ti, the cathode is air oxygen electrode, the distance between the anode and the cathode is 8cm, and the area of the electrode is 20cm2Current density 15mA/cm2. After 1 hour of photoelectrocatalysis reaction, the removal rate of 20mg/L and 120mL of water-soluble humic acid solution COD is 86.2%, and the decolorization rate is 100%.
The formic acid aqueous solution was treated in accordance with the apparatus structure and treatment process of embodiment 1. The setting conditions are as follows: 15W ultraviolet light source, TiO2Particle size of 2mm, P25 TiO, photocatalytic fluidized particles2Concentration of (2) is 0.8g/L and air flow is 0.6m3/h，TiO2/SnO2The anode is Ti, the cathode is air oxygen electrode, the distance between the anode and the cathode is 15cm, and the electrode area is 20cm2Current density 15mA/cm2. After 1 hour of photoelectrocatalysis reaction, the removal rate of 460mg/L and 120mL of formic acid water solution COD is 96.8%, and the decolorization rate is 100%.
The same two apparatuses were connected in series to treat the aqueous phenol solution in accordance with the apparatus configuration, treatment process and installation conditions in embodiment 1.
Claims (7)
1 device for treating organic matters in water by photoelectrocatalysis oxidation, which is a reaction device mainly used for a fluidized bed photoelectrocatalysis organic water treatment system and is characterized in that the device is prepared by titanium-based oxide TiO2/SnO2a/Ti anode (6), an air oxygen electrode cathode (7), TiO2The device comprises/C fluidized particles (8), an ultraviolet lamp light source (9), a potentiostat direct-current power supply (10), an air distribution plate (3), a shell (11), a wastewater inlet (4), a wastewater outlet (5), an air inlet (1), particle fillers (2) and a wire mesh plate (12); the integral porous air distribution plate (3) is positioned at the lower part of the device and forms an air distribution chamber with the shell, the air distribution chamber is filled with particle fillers (2), and the air distribution chamber is provided with an air inlet (1) communicated with the outside; the air oxygen electrode cathode (7) and the titanium-based oxide anode (6) are opposite and respectively close to the wall of the device; the ultraviolet lamp light source (9) is arranged between the cathode and the anode, namely the middle of the device; the air oxygen electrode and the titanium-based oxide electrode are respectively provided with an electric connector connected with a constant potential rectifier direct current power supply (10), and the upper part of the electrode chamber is provided with a TiO-preventing electrode2the/C photocatalytic particles are carried out of the wire mesh plate (12) outside the device.
The apparatus for treating organic matters in water by photoelectrocatalytic oxidation as set forth in claim 1, wherein said cathode electrode is an air oxygen electrode cathode (7) comprising a catalyst layer and a conductive skeleton, the catalyst layer is composed of activated carbon, metal oxide, graphite powder and polytetrafluoroethylene, wherein the metal oxide is TiO2、ZnO、MnO2The catalyst layer contains 70-85% of active carbon, 2-10% of metal oxide, 5-15% of graphite powder and 5-10% of polytetrafluoroethylene; the conductive framework is a nickel net or a silver-plated copper net.
The apparatus for treating organic matters in water by photoelectrocatalytic oxidation as set forth in claim 1, wherein the distance between the cathode and the anode is 4-15 cm.
The apparatus for treating organic substances in water by photoelectrocatalytic oxidation as set forth in claim 1, wherein the wavelength of the ultraviolet light source is 254 nm.
The reactor for photoelectrocatalytic oxidation treatment of organic matters in water as set forth in claim 1, wherein TiO is used2The particle diameter of the/C fluidized particles (8) is 1-2 mm.
The apparatus for treating organic matters in water by photoelectrocatalytic oxidation as set forth in claim 1, wherein the air distribution plate (3) is made of a ceramic material and has an inner pore diameter of 15 to 50 μm.
The apparatus for treating organic matters in water by photoelectrocatalytic oxidation as set forth in claim 1, wherein a wire mesh plate (12) placed on the upper portion of the electrode chamber has a mesh size smaller than that of TiO2Particle size of the/C fluidized particles.
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