CN1377728A - Three phase three-diemsnional electrode photoelectric reactor - Google Patents
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- CN1377728A CN1377728A CN 02114739 CN02114739A CN1377728A CN 1377728 A CN1377728 A CN 1377728A CN 02114739 CN02114739 CN 02114739 CN 02114739 A CN02114739 A CN 02114739A CN 1377728 A CN1377728 A CN 1377728A
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Abstract
The photoelectric reactor used in treating organic waste water consists of casing, 3D particle electrode, porous cathode titanium plate, anode titanium net, light source UV lamp and photocatalyst. It is one combination of triphase 3D electrode and photocatalytic technology, and it can capture photoelectrons in anode with bias voltage to raise the photocatalytic oxidation efficiency of titania and utilize the indirect electrochemical oxidatino and photocatalytic oxidation of H2O2 as strong oxidant produced in the 3D cathode. In addition, the porous titanium plate as both electrical feeder and aeration unit results in compact and reasonable structure, increased dissolution speed of oxygen of air in water and thus organic pollutant eliminating efficiency.
Description
Technical Field
The invention relates to a three-phase three-dimensional electrode photoelectric reactor and application thereof in treating organic wastewater.
Technical Field
The application of Advanced Oxidation Process (Advanced Oxidation Process) to environmental pollution control has attracted widespread attention in the eighties. Wherein the TiO is2Semiconductor heterogeneous photocatalytic processes are receiving much attention due to their unique advantages of room temperature and deep reaction. It has the functions of oxidizing and mineralizing organic pollutant, reducing heavy metal ion, deodorizing, antisepticizing and sterilizing. Has great application potential in the aspects of air and water purification and the like (M.Hoffman, S Martin, W.Choi and D.Bahnemann, chem.Rev., 1995, 95: 69).
However, the electron-hole pairs generated by light excitation are easy to recombine, so that the quantum efficiency of photocatalysis is very low (generally less than 0.1%), and therefore, the rapid capture of light-excited electrons and the inhibition of the recombination of the light-excited electrons and high-energy holes are crucial to the improvement of the efficiency of semiconductor photocatalytic degradation of organic pollutants. To achieve this, many improvements have been proposed from different perspectives. Such as noble metal deposition on semiconductor surfaces, semiconductor recombination or metal ion doping, etc. (K.T. Ranjit and B.Viswanathan, J.Photochem.and Photobiol., A: chem., 1997, 107: 215; J.C.Yu, J Lin and R.W.M.Kwok, J.Photochem.and Photobiol., A: chem., 1997, 111: 199). Recently, Vinodgopal et al found that TiO can be effectively removed by an applied electric field2Photoexcited electrons on the fixed membrane electrode inhibit the recombination of the excited electrons with high-energy holes, and accelerate the photodegradation speed of 4-chlorophenol and the like (K. Vinodgopal, S. Hotchanddani and P. V. Kamat, J. Phys chem.1993, 97: 9040). This study stimulated interest in controlling photocatalytic reactions electrochemically (j.m. kesselman, n.s. Lewis, and m.r.hoffman, environ.sci.technol., 1997, 31: 2298; k.vinodgopal, u.stafford, k.gray and p.kamat, j.phys.chem., 1994, 98: 6797). However, the current research is only limited to the proof of the concept that the anode bias can capture photo-generated electrons. In order to make the heterogeneous photoelectrocatalysis process practical, the technology in this aspect is urgently needed.
Among the numerous wastewater treatment methods, the electrochemical method has the advantages of compact equipment, small occupied area, no need of a large amount of chemical agents, small sludge amount and the like, and is known as a clean wastewater treatment method. This method has been actively studied in wastewater treatment in recent years, and has been reported a lot (k.rajeshwar, j.ibanez and g.swain, j.appl.electrochem., 1994, 24: 1077). Especially, the three-dimensional electrode has large volume-to-surface ratio and small distance between particles, greatly improves the mass transfer effect, and is an electrochemical reactor with higher practical and theoretical values. It has also found many applications in wastewater treatment, but most of them have been focused on the treatment of metal ion wastewater and studies in the field of organic wastewater have not been common.
Particularly, a photoelectric reactor is formed by combining a three-dimensional electrode reactor and a photocatalytic reactor, and the photoelectric reactor is used for efficiently treating organic wastewater, which has not been reported yet.
Disclosure of Invention
The invention aims to provide a photoelectric reactor based on a three-phase three-dimensional electrode, which not only has the function of efficiently electrooxidating organic pollutants, but also can capture photoproduction electrons, inhibit the recombination of the photoproduction electrons and high-energy holes, improve the efficiency of photocatalytic oxidation, and can be used as an efficient and clean organic wastewater deep oxidation treatment device.
The three-phase three-dimensional electrode photoelectric reactor consists of a shell, a three-dimensional particle electrode (three-dimensional electrode), a cathode electrode microporous titanium plate, an anode electrode metallic titanium mesh, a light source UV lamp and a photocatalyst; the micropore titanium plate is positioned at the lower part of the shell, an air chamber is formed between the micropore titanium plate and the bottom of the shell, and the air chamber is provided with an air inlet communicated with the outside; the three-dimensional particle electrode is a packed bed consisting of activated carbon or graphite and is arranged on the microporous titanium plate; the metal titanium mesh is positioned on the upper part of the shell, a light reaction chamber is arranged between the metal titanium mesh and the three-dimensional particle electrode, and the photocatalyst and the UV lamp are arranged in the light reaction chamber; the microporous titanium plate and the metal titanium net are respectively provided with an electric connector which can be connected with a direct current power supply.
The three-phase three-dimensional electrode photoelectric reactor can be used for keeping the reactor at a constant temperature, wherein a quartz cold well can be sleeved outside a UV lamp used as a light source.
The pore diameter of the microporous titanium plate used is generally 15 to 25 μm. The photocatalyst is nano-grade TiO2A photocatalyst. The photocatalyst is usually added to the reactor together with the waste water to be treated, and may be in the form of a fluidized bed or a fixed bed. The amount of photocatalyst used is generally: calculated according to the volume of the waste water or the volume of the light reaction chamber, 0.05-0.5 mg/L.
The three-phase three-dimensional electrode photoelectric reactor can also be provided with a water inlet at the upper part of the shell and a water outlet at the lower part of the shell so as to be convenient for continuously treating wastewater.
The process of treating organic wastewater by the three-phase three-dimensional electrode photoelectric reactor comprises the following steps:
(1) uniformly mixing a photocatalyst and organic wastewater to be treated, and then adding the mixture into the photoelectric reactor; (2) turning on the ultraviolet lamp; (3) starting an air compressor to introduce compressed air from an air inlet and adjusting the air flow; (4) and (4) switching on a direct current power supply, namely starting the photoelectric oxidation reaction of the organic pollutants.
The three-phase three-dimensional electrode photoelectric reactor has the following outstanding characteristics and beneficial effects:
(1) the cathode and the aeration plate of the reactor are integrated by the microporous titanium plate, so that the structure of the reactor is compact and reasonable, the pore diameter of the titanium plate is small (the SEM spectrum of the surface of the titanium plate is shown in figure 3), and extremely uniform tiny bubbles (shown in figure 4) can be generated, thereby increasing the dissolving speed of oxygen in air in water. Due to oxygen in TiO2The photocatalyst plays an important role in photocatalytic reaction, and can capture photoproduction electrons, inhibit the recombination of the photoproduction electrons and holes and increase the efficiency of the photocatalytic reaction.
(2) Is capable of electrically generating H2O2The three-phase three-dimensional electrode reactor and the immersed photocatalytic reactor. It can not only utilize anode to capture photoproduction electron, inhibit its recombination with high-energy cavity and raise photocatalytic oxidation efficiency, but also can effectively and directly electrochemically oxidize organic pollutant, and can utilize cathode to make electric H production2O2And the indirect electrochemical oxidation of H2O2So that the reactor can be used as an organic waste waterHigh-efficient advanced treatment unit.
The main chemical reactions of the three-phase three-dimensional electrode photoelectric reactor for treating organic wastewater are as follows:
anode + R → product
Wherein R is an organic compound
Drawings
Fig. 1 is a schematic structural diagram of an embodiment of the three-phase three-dimensional electrode photoelectric reactor of the present invention.
Fig. 2 is an X-ray electron energy spectrum of an activated carbon particle electrode.
FIG. 3 is a Scanning Electron Microscope (SEM) image of the surface of a microporous titanium electrode. From this figure, it can be seen that the pore size of the microporous titanium electrode is about 20 microns.
FIG. 4 is a photograph of bubbles generated by the photoelectric reactor through the microporous titanium electrode. These bubbles are small in diameter (about 1-2mm) and are uniformly distributed.
Detailed Description
Referring to fig. 1, the three-phase three-dimensional electrode photoelectric reactor of the present invention is mainly formed by combining a three-phase three-dimensional electrode reactor and an immersed photocatalytic reactor. The three-phase three-dimensional electrode reactor takes compressed air as an air source; with commercial activated carbon orThe graphite packed bed is a three-dimensional particle electrode 10; corrosion-resistant metal titanium is used as a material of the feed electrode, the anode is a metal titanium mesh 7, and the cathode is a commercial microporous titanium plate 5 with the aperture of 15-25 mu m; the metal titanium mesh and the microporous titanium plate are respectively provided with electric connectors 71 and 51 which can be connected with a direct current power supply 8. The microporous titanium plate 5 can play two roles, namely serving as a cathode of the reactor and serving as an aeration plate of the reactor; compressed air enters an air chamber 12 at the bottom of the reactor from an air inlet 11 and is aerated into the reactor through the microporous titanium plate 5. A three-dimensional particle electrode 10 consisting of an activated carbon or graphite packed bed is arranged on the microporous titanium plate 5, and a photoreaction chamber 13 is formed between the three-dimensional particle electrode and a metallic titanium mesh 7 at the upper part of the reactor. The immersed photocatalytic reactor mainly comprises a light source UV lamp 2 and a concentration (concentration of photocatalyst in the treated wastewater) of 0.05-0.5mg.l-1Of TiO with a nano particle diameter2A photocatalyst 4; wherein the UV lamp tube is positioned in the middle of the cylindrical reactor and between the cathode electrode microporous titanium plate 5 and the anode electrode metallic titanium mesh 7; the UV lamp 2 is externally sleeved with a quartz cold well 3 to keep the reactor at a constant temperature. The upper part of the quartz cold well 3 is provided with a cooling water inlet 1 and a cooling water outlet 6. The photocatalyst is usually added to the reactor together with the waste water to be treated. The shell 9 of the whole cylindrical reactor can be welded by PVC.
The following is a test example of the three-phase three-dimensional electrode photoelectric reactor of the present invention for treating organic wastewater. The diameter of the shell of the three-phase three-dimensional electrode photoelectric reactor is 6-12cm, the height is 40-60cm, and the height of the particle electrode packed bed is 3-7 cm.
Example 1:
formic acid wastewater is treated by a photoelectric reactor which takes an activated carbon packed bed with the bed height of 4cm as a three-dimensional electrode. We found that its COD removal efficiency is related to the applied voltage, which increases with increasing applied voltage. At 10.0 volts, 0.1m3h-1Air flow of (2), 500W high pressure mercury lamp illumination and 0.08mgl-1Degussa P25 TiO2Reacting for 1 hour in the presence of a photocatalyst to obtain 20.0mmol-1The COD concentration of the formic acid solution of (2) is from 320.5mgl-1Reduced to 118.4mgl-1The removal rate was 62.9%. The removal rate is higher than that of pure lightThe COD removal efficiency of the catalyst (except no voltage) is 35.5 percent higher.
Example 2:
printing and dyeing wastewater is one of the organic wastewater which is known to be difficult to treat. It has color contamination in addition to COD contamination. The photoelectric reactor taking the graphite packed bed with the bed height of 3cm as a three-dimensional electrode can effectively remove COD and color of the dye wastewater. At 30.0 volts, 0.6m3h-1Air flow of (2), 500W high pressure mercury exposure and 0.1mgl-11.0 mmolel in the presence of Degussa P25 photocatalyst-1The photoelectric degradation of methylene blue accords with the quasi-first-order reaction kinetics as the photocatalytic degradation of the methylene blue, but the speed constant of the methylene blue is 0.088min-11.6 times as much as the latter. After 0.5 hour of reaction, the solution was completely decolorized, the removal efficiency of COD was 87.2%, and the removal efficiency of TOC wasThe removal efficiency was 81.1%. COD and TOC removal efficiencies were so similar, indicating that methylene blue was almost mineralized.
Example 3:
the photoelectric reactor has obvious photoelectric synergistic effect in the process of oxidizing and decomposing organic matters. For 20.0mmol-10.1mgl of formic acid solution of-1Degussa P25 photocatalyst, 0.2m3·h-1The air flow and bed height of the photoelectrochemical reactor(s) of which the activated carbon packed bed is a three-dimensional electrode, the photoproduction current at 10 seconds of light irradiation is 12.3 muA at no voltage, the current at 0.5 volts and no light irradiation is 127.6 muA at 0.5 volts and the photoelectricity current at 10 seconds of light irradiation is 188.5 muA at 0.5 volts, which exceeds the sum of the currents of the individual electrochemical and individual photochemical processes by 48.6 muA. For 20.0mmol-1The formic acid solution and graphite packed bed with bed height of 4cm are three-dimensional electrodes, the photoproduction current is 15.6 muA when the reactor is irradiated by light for 10 seconds under no voltage, the current is 133.2 muA when the reactor is irradiated by 0.5 volt and no light, the photoelectricity current is 200.5 muA when the reactor is irradiated by light for 10 seconds under 0.5 volt, and the sum of the currents of single electrochemical process and single photochemical process is more than 51.7 muA. This enhancement of current can be attributed to a synergy between photochemical and electrochemical processes. This synergy is also manifested in the removal of COD.
Example 4:
one of the key problems in the industrialization of photocatalytic treatment of organic wastewater is how to solve the poisoning effect of inorganic ions existing in actual industrial wastewater on a photocatalyst. The photoelectric reactor is used for treating common toxic inorganic ions Cl-Has strong antitoxic effect. The activated carbon packed bed with bed height of 5.0cm is a three-dimensional electrode, 0.3mgl-1Degussa P25 photocatalyst and 0.15m3h-1At 1.0mmol of the gas flow rate of-1In the presence of NaCl, the COD photocatalytic removal efficiency of the formic acid solution is reduced from 28.9% to 16.5%, and the relative deactivation rate is 42.9%, while the COD photoelectric removal efficiency at a voltage of 10.0V is reduced from 62.9% to 46.3%, and the relative deactivation rate is only 26.4%.
Claims (4)
1. A three-phase three-dimensional electrode photoelectric reactor is characterized in that the reactor consists of a shell (9), a three-dimensional particle electrode (10), a cathode electrode microporous titanium plate (5), an anode electrode metallic titanium mesh (7), a light source UV lamp (2) and a photocatalyst (4); the microporous titanium plate (5) is positioned at the lower part of the shell (9), and an air chamber (12) is formed between the microporous titanium plate and the bottom of the shell and is provided with an air inlet (11) communicated with the outside; the three-dimensional particle electrode (10) is a packed bed composed of activated carbon or graphite and is arranged on the microporous titanium plate; the titanium mesh (7) is positioned at the upper part of the shell, a light reaction chamber (13) is arranged between the titanium mesh and the three-dimensional particle electrode, and the photocatalyst and the UV lamp (2) are arranged in the light reaction chamber; the microporous titanium plate and the titanium mesh are respectively provided with electric connectors (51) and (71) which can be connected with a direct current power supply.
2. The three-phase three-dimensional electrode photoelectric reactor as claimed in claim 1, wherein the light source UV lamp (2) is sheathed with a quartz cold well (3).
3. A three-phase three-dimensional electrode photoelectric reactor according to claim 1 or 2, wherein the pore size of the microporous titanium plate (5) is 15 to 25 μm.
4. Three-phase three-dimensional electrode according to claim 1 or 2The photoelectric reactor is characterized in that the photocatalyst is nano-TiO2A photocatalyst.
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN1300012C (en) * | 2004-02-26 | 2007-02-14 | 江苏省环境科学研究院 | Process for treating waste water of nitrobenzene, 2,4-dinitrophenol, p-nitro-chlorebenzene |
| CN101111458B (en) * | 2005-01-28 | 2010-05-26 | 皇家飞利浦电子股份有限公司 | Treatment system comprising a dielectric barrier discharge lamp |
| CN101224401B (en) * | 2007-10-19 | 2010-07-07 | 东华大学 | Fixed bed inhomogeneous three dimensional electrode photo electrocatalysis reactor |
| CN101857309A (en) * | 2010-06-12 | 2010-10-13 | 浙江工商大学 | Electrochemical biological combined denitrification reactor |
| CN102020342A (en) * | 2011-01-14 | 2011-04-20 | 南京大学 | Compound three-dimensional electrode reactor and application thereof in treatment of nitrogenous organic wastewater |
| CN101700485B (en) * | 2009-11-04 | 2011-12-28 | 北京大学 | Photoelectric catalytic device |
| CN102358635A (en) * | 2011-09-21 | 2012-02-22 | 河海大学 | Photoelectrocatalysis device used for treating refractory organics |
| CN103420452A (en) * | 2013-07-08 | 2013-12-04 | 南通大学 | Bipolar packed bed type three-dimensional electrode photo-electricity catalytic reactor |
| CN104803444A (en) * | 2015-04-03 | 2015-07-29 | 江苏润聚新材料科技有限公司 | Advanced oxidation pollution control technology and device |
| CN105293644A (en) * | 2015-10-10 | 2016-02-03 | 泉州师范学院 | Photoelectrochemical electrolytic equipment and electrode plates for photoelectrochemical electrolytic equipment |
| CN106745542A (en) * | 2017-03-13 | 2017-05-31 | 盐城工学院 | The photoelectrocatalysis processing system and method for high-salt wastewater |
| CN113562816A (en) * | 2021-08-27 | 2021-10-29 | 中国石油化工股份有限公司 | Three-dimensional electrode reaction device and method for removing COD (chemical oxygen demand) in wastewater |
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2002
- 2002-01-16 CN CNB021147396A patent/CN1162215C/en not_active Expired - Fee Related
Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1300012C (en) * | 2004-02-26 | 2007-02-14 | 江苏省环境科学研究院 | Process for treating waste water of nitrobenzene, 2,4-dinitrophenol, p-nitro-chlorebenzene |
| CN101111458B (en) * | 2005-01-28 | 2010-05-26 | 皇家飞利浦电子股份有限公司 | Treatment system comprising a dielectric barrier discharge lamp |
| CN101224401B (en) * | 2007-10-19 | 2010-07-07 | 东华大学 | Fixed bed inhomogeneous three dimensional electrode photo electrocatalysis reactor |
| CN101700485B (en) * | 2009-11-04 | 2011-12-28 | 北京大学 | Photoelectric catalytic device |
| CN101857309A (en) * | 2010-06-12 | 2010-10-13 | 浙江工商大学 | Electrochemical biological combined denitrification reactor |
| CN102020342A (en) * | 2011-01-14 | 2011-04-20 | 南京大学 | Compound three-dimensional electrode reactor and application thereof in treatment of nitrogenous organic wastewater |
| CN102358635A (en) * | 2011-09-21 | 2012-02-22 | 河海大学 | Photoelectrocatalysis device used for treating refractory organics |
| CN103420452A (en) * | 2013-07-08 | 2013-12-04 | 南通大学 | Bipolar packed bed type three-dimensional electrode photo-electricity catalytic reactor |
| CN104803444A (en) * | 2015-04-03 | 2015-07-29 | 江苏润聚新材料科技有限公司 | Advanced oxidation pollution control technology and device |
| CN105293644A (en) * | 2015-10-10 | 2016-02-03 | 泉州师范学院 | Photoelectrochemical electrolytic equipment and electrode plates for photoelectrochemical electrolytic equipment |
| CN106745542A (en) * | 2017-03-13 | 2017-05-31 | 盐城工学院 | The photoelectrocatalysis processing system and method for high-salt wastewater |
| CN113562816A (en) * | 2021-08-27 | 2021-10-29 | 中国石油化工股份有限公司 | Three-dimensional electrode reaction device and method for removing COD (chemical oxygen demand) in wastewater |
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