CN101353186B - Processing method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater - Google Patents
Processing method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater Download PDFInfo
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- CN101353186B CN101353186B CN2008102000392A CN200810200039A CN101353186B CN 101353186 B CN101353186 B CN 101353186B CN 2008102000392 A CN2008102000392 A CN 2008102000392A CN 200810200039 A CN200810200039 A CN 200810200039A CN 101353186 B CN101353186 B CN 101353186B
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Abstract
The invention relates to a method for disposing organic wastewater by photocatalysis of double rotating table photocell liquid film reactor in the technical field of environmental catalysis. TiO2 photocatalyst is loaded on the base and is used as photo anode, which is fixed together with the cathode on the rotating shaft for forming a double rotating table, the lower half of the double rotating table is immerged in wastewater, and the double rotating table is connected with the carbon brush connecting with the rotating shaft by leads. The motor is started, and the rotate speed of the double rotating table is controlled, thus a layer of liquid film is formed on the surface of the double rotating table. An uviol lamp is taken as the excitation light source, the photoinduced electrons on thesurface of the photo anode of the TiO2 film rotating table is transferred to the surface of the cathode of the rotating table, the photoinduced electrons react with the saturated dissolved oxygen on the surface of the cathode rotating table so as to generate H2O2, and the indirect oxidation to organic matter and the direct oxidation to organic matter by photo cavity on the surface of TiO2 film photo anode rotating table improve the degradation efficiency; and the rotation of the rotating table speeds up exchange and update of electrode surface and bulk solution substance, mass transfer is strengthened, and higher effect thereof can be realized.
Description
Technical field
What the present invention relates to is the method that a kind of chemical technology field is handled organic waste water, relates in particular to a kind of method of double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing.
Background technology
In recent years, TiO
2Be proved to be the semiconductor light-catalyst that a kind of efficient, stable, non-selectivity and material are easy to get.TiO
2Photocatalysis technology almost can make the pollutent permineralization in the sky G﹠W as a kind of high-level oxidation technology, does not produce secondary pollution, and the reaction conditions gentleness, has become a kind of extremely attractive Organic pollutants treatment process.Find TiO from Fujishima in 1972
2But since the photochemical catalysis splitting water, TiO
2The conductor photocatalysis technology has obtained extensive studies gradually aspect treatment of organic matters of organic.For solving TiO
2Difficulty and the isolating problem of waste water, TiO
2Be fixed on the various carriers, because TiO
2Thereby the immobilization meeting causes its surface-area decline its photocatalytic activity is descended, the investigator is TiO
2Mould material stops the simple composite in light induced electron and hole as anode by adding anodic bias, thereby improves photocatalysis efficiency, and this is a photoelectrocatalysis.TiO
2The semiconductor photoelectrocatalysielectrode technology is that a kind of UV-light of utilizing is made excitation light source, makes light induced electron and hole be able to effective the separation by applying bias, and respectively with H
2O or O
2Reaction generates a kind of oxidation technology that the living radical with strong oxidation capacity comes the oxidative degradation pollutent.
Find through literature search prior art, Wenbing Zhang etc. adopt three-diemsnional electrode-TiO in Photoelectrocatalyticdegradation of reactive brilliant orange K-R in a new continuouS flowphotoelectrocatalytic reactor (the new Continuous Flow photo electrocatalysis reactor photoelectric catalysis degrading reactive brilliant orange K-R) article that " Applied Catalysis A " (applied catalysis A) 2003 255 phase 221-229 pages or leaves are delivered
2Particle increases electrode area, enhancing degradation efficient; Adopt anodic bias to shift light induced electron, improve the separation efficiency in light induced electron and hole to negative electrode; Utilize the recirculated cooling water heat radiation; Strengthen mass transfer by air-blowing.Its weak point is: the one, and the solution that exciting light must see through thicker (several centimetres often) just can shine on the electrode, and the exciting light utilization ratio is very low; The 2nd, utilize bias voltage to shift light induced electron, increased energy consumption; The 3rd, strengthen mass transfer, poor effect by air-blowing; The 4th, the power of excitation light source is bigger, has increased recirculated cooling water device and has evacuated heat, has not only increased operation energy consumption, and reactor assembly is comparatively complicated.
Though at Chinese patent (TiO
2Film electrode photoelectric turnplate is handled the method for organic wastewater with difficult degradation thereby, application number 200810035837.4) in, with TiO
2Membrane electrode is made into rotating disk, and the rotation that utilizes rotating disk is at TiO
2The membrane electrode surface has formed tens microns liquid film, has strengthened the utilization ratio and the mass-transfer efficiency of exciting light simultaneously; And utilize the small power low pressure mercury lamp to make excitation light source, having reduced energy consumption does not need the recirculated cooling water device heat radiation, has simplified device.But negative electrode leaves standstill in this device, remain with anodic bias and shift light induced electron, and transfer transport does not effectively utilize behind negative electrode, to the not contribution of processing of waste water.So its energy consumption is expected to further reduction, processing efficiency remains further to be improved.
Summary of the invention
The objective of the invention is at the deficiencies in the prior art, a kind of method of double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing is proposed, loss when reducing exciting light and in organic solution, transmit and utilize the rotation reinforcement mass transfer of rotating disk in, utilize metal and N-semi-conductor TiO
2Schottky barrier rather than applying bias that contact forms are transferred to cathode surface with light induced electron, generate H at cathode surface and saturated dissolved oxygen reaction
2O
2, and then participate in the oxidation of organic pollutant and with light induced electron indirect application in addition, realize the bipolar oxidizing in two rotating plate photoelectricity ponds thus.Improved utilization ratio, mass-transfer efficiency and the photocatalysis efficiency of exciting light simultaneously, and do not needed applying bias, reduced energy consumption and simplified device.
The present invention is achieved by the following technical solutions, the present invention with sol-gel method with TiO
2Photocatalyst loads in the substrate and is prepared into rotating disc electrode as the light anode, becomes rotating disk to make negative electrode material preparations such as Cu simultaneously, with TiO
2The film rotating disc electrode is fixed in the same rotating shaft together, be placed in the semi arch reaction tank, lower part of rotating disk is immersed in the waste water, with lead two rotating disks are connected into the loop by carbon brush, form two rotating plate photoelectricity ponds, hotwire makes disc surfaces form one deck liquid film by the rotating speed of governor control rotating disk.With the ultraviolet lamp is excitation light source, utilizes Schottky barrier with TiO
2The light induced electron on film rotating disc electrode surface is transferred to the negative electrode disc surfaces, with the saturated dissolved oxygen reaction generation H in its surface solution
2O
2, H
2O
2Can further participate in the oxidation of organic pollutant, realize the H of bipolar oxidizing-negative electrode disc surfaces generation in two rotating plate photoelectricity pond thus
2O
2To organic indirect oxidation and TiO
2The photohole of film light anode disc surfaces is to organic direct oxidation.Not only improve the separation efficiency and the degradation efficiency in utilization ratio, light dirt electronics and the hole of excitation light source, but also reduced operation energy consumption.
The present invention includes following steps:
The first step, with sol-gel method with TiO
2Photocatalyst loads on and makes the light anode in the substrate, and light anode and cathode disk are fixed on together forms two rotating disks in the rotating shaft, and the rotating shaft of rotating disk is connected with motor.
Second step was placed on rotating disk in the semi arch reaction tank, and the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by carbon brush with the negative electrode rotating disk.
The 3rd step, hotwire, the control rotary speed makes disc surfaces form one deck liquid film.
In the 4th step, adopt excitation light source irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface.
In the 5th step, use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio.
In the 6th step, sampling analysis after for some time is measured organic clearance in the waste water, finishes the processing of organic waste water.
Described smooth anode substrate material is stainless steel or titanium.
Described cathode material is a kind of among Cu, Zn, Fe and the C.
Described control rotary speed is meant that the rotating speed by the governor control dial rotation is 30-90rpm.
Described excitation light source is a ultraviolet lamp, and the fluorescent tube back side of ultraviolet lamp adopts aluminium foil to reflect to improve the light source utilization ratio.
Sampling analysis after described for some time, be meant 0.5-2 hour after sampling analysis.
Two turntable structures of uniqueness of the present invention and rotation formula and traditional photoelectrocatalysis method (TiO
2The light anode all is immersed in the solution, exciting light need could arrive light anode catalyst surface with one deck reactor wall through several centimetres waste water) compare, the one, greatly reduce the light loss that is caused by solution absorption when exciting light transmits in organic waste water, improved the utilization ratio of exciting light; The 2nd, utilize metal and N-N-type semiconductorN TiO
2Schottky barrier that contact forms rather than applying bias are with TiO
2The light induced electron of film rotating disk photoanode surface is transferred to the rotating disk cathode surface, has reduced energy consumption; The 3rd, in the negative electrode disc surfaces, the reaction of the saturated dissolved oxygen of light induced electron and negative electrode disc surfaces generates H
2O
2, and then participate in the oxidation of organic pollutant and light induced electron is applied, realize thus having improved degradation efficiency by the bipolar oxidizing of two rotating disks; The 4th, the exchange renewal of electrode surface and main body solution material has been accelerated in the rotation of rotating disk, has strengthened mass transfer, makes it more efficient.
Description of drawings
The two rotating plate photoelectricity ponds of Fig. 1 liquid film reactor is handled the experimental installation synoptic diagram of organic waste water;
Among the figure: 1 is speed regulator, and 2 is motor, and 3 is the Cu rotating shaft, and 4 is the rotating disk negative electrode, and 5 is TiO
2Film rotating disk light anode, 6 is carbon brush, and 7 is reaction tank, and 8 is waste water, and 9 is excitation light source, 10 is aluminium foil.
Embodiment
Below in conjunction with accompanying drawing embodiments of the invention are elaborated: present embodiment is being to implement under the prerequisite with the technical solution of the present invention, provided detailed embodiment and concrete operating process, but protection scope of the present invention is not limited to following embodiment.
As shown in Figure 1, the testing apparatus figure that the embodiment of the invention adopts, the embodiment treating processes is:
1) adopt stainless steel disk or titanium disk as substrate, with sol-gel method with TiO
2Photocatalyst loads in the substrate, as light anode 5, is fixed on the two rotating plate photoelectricity ponds of composition liquid film reactor in the rotating shaft 3 with Cu, Zn, Fe or C negative electrode 4, and rotating shaft 3 is connected with motor 2;
2) light anode 5 and negative electrode 4 are placed in the semi arch reaction tank 7, the rotating shaft 3 of two rotating disks is in the water surface site of waste water 8, and lower part of two rotating disks is immersed in the waste water, and light anode 5 is connected by the carbon brush 6 usefulness leads that link to each other with rotating shaft respectively with negative electrode 4;
3) hotwire 2, and are 30-90rpm by the rotating speed of speed regulator 1 control dial rotation, make light anode 5 and negative electrode 4 surfaces form one deck liquid films;
4) adopt excitation light source 9 irradiates light anodes 5, make exciting light see through liquid film and shine light anode 5 surfaces;
5) use aluminium foil 10 reflection sources TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio;
6) sampling analysis after 0.5-2 hour is measured organic clearance in the waste water 8, finishes the processing of organic waste water.
The two rotating plate photoelectricity ponds of embodiment 1 different cathode materials liquid film reactor dye wastewater treatment using
Process object is 20mg L
-1Rhodamine B (pH2.5,1.0g/L Na
2SO
4) dye wastewater.Wastewater volume is 55ml.
1) adopt the titanium disk as substrate, with sol-gel method with TiO
2Photocatalyst loads on and makes the light anode in the substrate, is fixed on Cu, Zn, Fe or C disk negative electrode respectively and forms two rotating disks in the rotating shaft, and the rotating shaft of rotating disk is connected with motor.
2) rotating disk is placed in the semi arch reactive tank, the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by the carbon brush that links to each other with rotating shaft with the negative electrode rotating disk.
3) hotwire, and be 90rpm by the rotating speed of governor control dial rotation, make disc surfaces form one deck liquid film.
4) adopt 11W254nm low pressure mercury lamp irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface.
5) use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio.
6) sampling analysis after 30 minutes is measured the absorbancy of rhodamine B at the 563nm place, asks chroma removal rate (%).The result is as follows:
| Cathode material | Cu | Zn | Fe | C |
| Rhodamine B percent of decolourization (%) | 99.9 | 72.9 | 18.8 | 64.2 |
Process object is rhodamine B (pH2.5, the 1.0g/L Na of different concns
2SO
4) dye wastewater.Wastewater volume is 55ml.
1) adopt the titanium disk as substrate, with sol-gel method with TiO
2Photocatalyst loads on to be made light anode and Cu disk negative electrode and is fixed on together and forms two rotating disks in the rotating shaft in the substrate, the rotating shaft of rotating disk is connected with motor.
2) rotating disk is placed in the semi arch reactive tank, the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by the carbon brush that links to each other with rotating shaft with the negative electrode rotating disk.
3) hotwire, the rotating speed by the governor control dial rotation is 90rpm, makes disc surfaces form one deck liquid film.
4) adopt 11W254nm low pressure mercury lamp irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface.
5) use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio.
6) sampling analysis after 60 minutes is measured the absorbancy of rhodamine B at the 563nm place, asks chroma removal rate (%), and calculates rhodamine B removal amount (mg), and the result is as follows:
| Rhodamine B concentration (mg L -1) | 20 | 30 | 50 | 80 | 100 | 150 |
| Chroma removal rate (%) | 100 | 89.8 | 87.9 | 87.7 | 78.6 | 74.7 |
| Rhodamine B removal amount (mg) | 1.10 | 1.48 | 2.42 | 3.86 | 4.32 | 6.16 |
As seen along with the increase of dye strength, the dyestuff removal amount increases gradually, shows that two rotating plate photoelectricity ponds liquid-film method especially is fit to handle dye wastewater with high concentration.
Process object is rhodamine B (pH2.5, the 1.0g/L Na of different concns
2SO
4) dye wastewater.Wastewater volume is 55ml.
1) adopt the stainless steel disk as substrate, with sol-gel method with TiO
2Photocatalyst loads on to be made light anode and Cu disk and is fixed on together and forms two rotating disks in the rotating shaft in the substrate, the rotating shaft of rotating disk is connected with motor.
2) rotating disk is placed in the semi arch reactive tank, the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by the carbon brush that links to each other with rotating shaft with the negative electrode rotating disk.
3) hotwire, the rotating speed by the governor control dial rotation is 30rpm, makes disc surfaces form one deck liquid film.
4) adopt 11W254nm low pressure mercury lamp irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface.
5) use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio.
6) sampling analysis after 60 minutes is measured the absorbancy of rhodamine B at the 563nm place, asks chroma removal rate (%), and the result is as follows:
| Rhodamine B concentration (mg L -1) | 20 | 30 | 50 | 80 | 100 | 150 |
| Chroma removal rate (%) | 96.8 | 85.4 | 83.5 | 83.6 | 74.9 | 71.2 |
Process object is 20mgL
-1Reactive brilliant red x-3b, red, the direct copper blue 2r of temptation, direct fast blue FRL, direct dark green B, dark blue 5R, erie black ATT and weak acid brilliant green GS dye wastewater.Wastewater volume is 55ml respectively, is pH2.5 and 1.0g/L Na
2SO
4
1) adopt the titanium disk as substrate, with sol-gel method with TiO
2Photocatalyst loads on to be made light anode and Cu disk negative electrode and is fixed on together and forms two rotating disks in the rotating shaft in the substrate, the rotating shaft of rotating disk is connected with motor.
2) rotating disk is placed in the semi arch reactive tank, the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by the carbon brush that links to each other with rotating shaft with the negative electrode rotating disk.
3) hotwire, the rotating speed by the governor control dial rotation is 90rpm, makes disc surfaces form one deck liquid film.
4) adopt 11W254nm low pressure mercury lamp irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface.
5) use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio.
6) sampling analysis after 30 minutes is measured the absorbancy of each dyestuff maximum absorption wave strong point, asks chroma removal rate (%).The result is as follows:
| Dyestuff | λmax(nm) | Percent of decolourization (%) | Dyestuff | λmax(nm) | Percent of decolourization (%) |
| Reactive brilliant red x-3b | 538 | 88.4 | Dark blue 5R | 568 | 31.5 |
| Lure red | 501 | 59.6 | Erie black ATT | 562 | 81.6 |
| Direct copper blue 2r | 562 | 52.5 | Weak acid brilliant green GS | 606 | 28.4 |
| Direct fast blue FRL | 584 | 25.8 | Direct dark green B | 624 | 26.6 |
Process object is actual dying (pH11.3).This waste water is taken from Changzhou printing and dyeing mill.Wastewater volume is 55ml.
1) adopt the titanium disk as substrate, with sol-gel method with TiO
2Photocatalyst loads on to be made light anode and Cu disk and is fixed on together and forms two rotating disks in the rotating shaft in the substrate, the rotating shaft of rotating disk is connected with motor.
2) rotating disk is placed in the semi arch reactive tank, the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by the carbon brush that links to each other with rotating shaft with the negative electrode rotating disk.
3) hotwire, the rotating speed by the governor control dial rotation is 90rpm, makes disc surfaces form one deck liquid film.
4) adopt 11W254nm low pressure mercury lamp irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface.
5) use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side strengthens the light source utilization ratio.
6) 30 minutes sampling analysis in every interval in 2 hours, the absorbancy and total organic carbon (TOC) concentration at mensuration dyeing waste water 514nm place are asked clearance (%), and the result is as follows:
| Time (min) | 30 | 60 | 90 | 120 |
| Percent of decolourization (%) | 25.9 | 59.8 | 80.0 | 88.0 |
| TOC clearance (%) | 13.1 | 25.1 | 35.7 | 44.4 |
The explanation of above-mentioned experimental result, the two rotating plate photoelectricity ponds of the present invention liquid film reactor is handled the method for organic waste waters (is example with the waste water from dyestuff), and can effectively degrade dye wastewater and actual dying have a very big application prospect industrial.
Claims (6)
1. the method for a double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing is characterized in that comprising the steps:
The first step, with sol-gel method with TiO
2Photocatalyst loads on and makes the light anode in the substrate, and light anode and cathode disk are fixed on together forms two rotating disks in the rotating shaft, and the rotating shaft of rotating disk is connected with motor;
Second step was placed on rotating disk in the semi arch reaction tank, and the rotating shaft of rotating disk is in the water surface site of waste water, and lower part of rotating disk is immersed in the waste water, and the light anode is connected with lead by carbon brush with the negative electrode rotating disk;
The 3rd step, hotwire, the control rotary speed makes disc surfaces form one deck liquid film;
In the 4th step, adopt excitation light source irradiation TiO
2The light anode makes exciting light see through liquid film and shines TiO
2Catalyst surface;
In the 5th step, use aluminium foil reflection source TiO dorsad
2The exciting light of light anode one side;
In the 6th step, sampling analysis after for some time is measured organic clearance in the waste water, finishes the processing of organic waste water.
2. the method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing according to claim 1 is characterized in that, light anode substrate material is stainless steel or titanium.
3. the method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing according to claim 1 is characterized in that, cathode material is a kind of among Cu, Zn, Fe or the C.
4. the method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing according to claim 1 is characterized in that, described control rotary speed is meant that the rotating speed by the governor control dial rotation is 30-90rpm.
5. the method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing according to claim 1 is characterized in that, described excitation light source is a ultraviolet lamp, and the fluorescent tube back side of ultraviolet lamp adopts aluminium foil to reflect.
6. the method for double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing according to claim 1 is characterized in that, sampling analysis after described for some time, be meant 0.5-2 hour after sampling analysis.
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| CN101774661B (en) * | 2010-01-28 | 2012-12-26 | 上海交通大学 | Composite rotating disk liquid film reactor and method for processing organic wastewater |
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| CN102398955A (en) * | 2011-09-15 | 2012-04-04 | 上海交通大学 | Device and method for treating organic wastewater with TiO2 photocatalysis rotary disc fuel cell |
| CN102403523B (en) * | 2011-09-15 | 2014-12-10 | 上海交通大学 | Apparatus and method for processing organic wastewater by using TiO2-based photocatalytic composite-electrode fuel cell |
| CN102502941A (en) * | 2011-11-03 | 2012-06-20 | 重庆理工大学 | Method for treating organic wastewater through photocatalysis by inclined double-pole liquid film |
| CN102826631B (en) * | 2012-09-11 | 2014-11-19 | 北京师范大学 | Hydrodynamic impeller disk reactor for efficiently evaluating efficiency of photoelectric catalytic reaction |
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| CN107651733A (en) * | 2016-07-26 | 2018-02-02 | 中国科学院生态环境研究中心 | A kind of method that rotating cathode strengthens photoelectrocatalysioxidization oxidization processing complex state heavy metal wastewater thereby and negative electrode recovery heavy metal |
| CN106673114B (en) * | 2016-11-14 | 2021-04-06 | 苏州大学 | Photodegradation purification device and manufacturing method and purification method thereof |
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