CN102502941A - Method for treating organic wastewater through photocatalysis by inclined double-pole liquid film - Google Patents

Method for treating organic wastewater through photocatalysis by inclined double-pole liquid film Download PDF

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CN102502941A
CN102502941A CN201110343430XA CN201110343430A CN102502941A CN 102502941 A CN102502941 A CN 102502941A CN 201110343430X A CN201110343430X A CN 201110343430XA CN 201110343430 A CN201110343430 A CN 201110343430A CN 102502941 A CN102502941 A CN 102502941A
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light
waste water
liquid film
anode
tio
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徐云兰
钟登杰
全学军
李军
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Chongqing University of Technology
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
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    • Y02W10/30—Wastewater or sewage treatment systems using renewable energies
    • Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy

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Abstract

The invention relates to a method for treating organic wastewater through photocatalysis by an inclined double-pole liquid film in the technical field of environmental catalysis. The method comprises the following steps of: loading TiO2 on a substrate by a sol-gel method, wherein the substrate loaded with TiO2 is used as a photoanode, and Cu, Zn, Fe, or C is used as a cathode; placing the photoanode and the cathode in a reaction tank in an inclined way to ensure that the lower half parts of the photoanode and the cathode are immersed in the wastewater, and connecting the photoanode and the cathode by using a guide line; controlling the rotation speed of a peristaltic pump to ensure that the wastewater forms a liquid film on the surface of an electrode; irradiating the TiO2 photoanode by using an excitation light source; and sampling and analyzing after 0.5 to 3 hours, and determining organic matter removal rate to finish treating the organic wastewater. According to the method, metal and N-semiconductor TiO2 are contacted with an inherent Schottky barrier, photoinduced electrons on the surface of the photoanode are transferred to the surface of the cathode, the organic matter is directly reduced or the organic matter is reacted with saturated dissolved oxygen on the surface of the cathode so as to generate H2O2, so the organic matter is indirectly oxidized, and the organic matter is directly oxidized with the anode; and therefore, a double-pole double-effect treatment effect is achieved, the degradation efficiency is improved, and energy consumption is reduced simultaneously.

Description

The method of tilting bipolar liquid film photo catalytically treating waste water
Technical field
The present invention relates to a kind of environmental catalysis technical field and handle the method for organic waste water, relate in particular to the method that a kind of tilting bipolar flow hydrodynamic film photocatalytic is handled organic waste water.
Background technology
TiO 2Be a kind of efficient, stable, nontoxic, non-selectivity and the semiconductor light-catalyst that is easy to get.TiO 2Photocatalysis technology is gentle because of its reaction conditions, and does not produce secondary pollution, almost can make the pollutent permineralization in the sky G&W, has become a kind of Organic pollutants treatment process that receives much concern.
At present, TiO 2There is following problem in photocatalysis technology: 1. TiO 2Difficulty is separated with waste water; 2. the exciting light penetration depth is limited, and utilization ratio is low; 3. light induced electron and hole are prone to the compound problem.For addressing these problems TiO 2Be fixed on the various carriers, as anode, improve the separation efficiency in light induced electron and hole through adding anodic bias, this is a photoelectrocatalysis.But should technology use applying bias, and not only increase energy consumption, and increased the appliance arrangement expense.In addition; For solving the low problem of exciting light utilization ratio; Adopt the liquid film reaction to reduce the light loss that organism in the waste water causes the absorption of exciting light though have; But generally all adopt the form of light anode liquid film, think little of the application after light induced electron is transferred to negative electrode, bias toward the application of photohole direct oxidation effect.
Literature search through to prior art is found; Taicheng An etc. adopt three-diemsnional electrode-Ti load TiO in " Photoelectrocatalytic degradation of oxalic acid in aqueous phase with a novel three-dimensional electrode-hollow quartz tube photoelectrocatalytic reactor " " novel three-dimensional electrode-hollow quartz tube photo electrocatalysis reactor photoelectric catalysis degrading oxalic acid solution " literary composition that " Applied Catalysis A " (applied catalysis A) 2005 279 phase 247-256 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.Its weak point is: the one, and the part of exciting light entering silica tube is limited, causes irradiation Ti load TiO 2The excitating light strength of catalyzer is limited, and catalytic efficiency (is lower; The 2nd, utilize applying bias to shift light induced electron, increased energy consumption; The 3rd, there is not the equipment of reinforcing mass transfer, mass transfer effect is poor; The 4th, the power of excitation light source is bigger, and the reaction unit heating has obviously increased operation energy consumption.
In Chinese patent (method of two electrodes sensitive cell liquid film reactor photo catalytically treating waste water, application number 200810200039.2), with TiO 2Thin film positive pole and negative electrode all are made into rotating disc electrode, and the rotation that utilizes electrode 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.But electrode moves in this device, and inconvenience receives the occasion of sunshine easily and uses on landscape water body, roof etc.
 
Summary of the invention
The objective of the invention is to deficiency to prior art; A kind of method of tilting bipolar liquid film photo catalytically treating waste water of static electrode is proposed; Loss when reducing exciting light and in organic solution, transmit and utilize the circulating in the reinforcement mass transfer of waste water utilizes metal and N-semi-conductor TiO 2Schottky barrier rather than applying bias (having reduced energy consumption and cost of equipment) that contact forms are transferred to negative electrode with light induced electron, make light induced electron directly reduce organism at cathode surface, or embezzle with the negative electrode liquid film and the dissolved oxygen reaction generates H 2O 2, and then participate in organic pollutant oxidation and with light induced electron be used and the anodic direct oxidation together, realize the photocatalytic degradation treatment effect of bipolar economic benefits and social benefits.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 realizes through following technical scheme, the present invention with sol-gel method with TiO 2Photocatalyst loads in the substrate and is prepared into electrode as the light anode, makes negative electrode with materials such as Cu simultaneously, with TiO 2Membrane electrode is tilting at a certain angle together in reaction tank; Lower part of electrode is immersed in the waste water, two electrodes is connected into the loop, form tilting bipolar light catalyticreactor with lead; Through the rotating speed of peristaltic pump governor control peristaltic pump, make waste water form one deck liquid film at electrode surface.With uv lamp or sunshine is excitation light source, utilizes Schottky barrier with TiO 2The light induced electron on membrane electrode surface is transferred to cathode surface, directly reduces organism or generate H with saturated dissolved oxygen reaction in its surface solution at cathode surface 2O 2, H 2O 2Further participate in the oxidation of organic pollutant, realized that thus tilting bipolar bipolar economic benefits and social benefits treatment effect-negative electrode light induced electron directly reduces the H that organism or its surface generate 2O 2To organic indirect oxidation and TiO 2The photohole of film photoanode surface is to organic direct oxidation.Not only improve the separation efficiency and the degradation efficiency in utilization ratio, light induced electron and the hole of excitation light source, but also reduced operation energy consumption.
The method of a kind of tilting bipolar liquid film photo catalytically treating waste water of the present invention, concrete steps comprise:
The first step, with sol-gel method with TiO 2Photocatalyst loads on and makes the light anode in the substrate, makes negative electrode with Cu, Zn, Fe or C; Liquid storage tank is located at the top of reaction tank; By the pipeline that is provided with peristaltic pump liquid storage tank and reaction tank are communicated with; Said smooth anode and negative electrode is tilting in reaction tank, the last termination liquid storage tank of said smooth anode and negative electrode, lower part of electrode is immersed in the waste water of reaction tank; Said smooth anode is connected with lead with negative electrode;
Second step, start peristaltic pump, control peristaltic pump rotating speed makes waste water form one deck liquid film at said smooth anode and cathode surface;
In the 3rd step, adopt excitation light source irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface;
The 4th step, when adopting source of artificial light with aluminium foil reflection source TiO dorsad 2The exciting light of light anode one side, the utilization ratio of raising exciting light;
In the 5th step, sampling analysis after 0.5-3 hour is measured organic clearance in the waste water, accomplishes the processing of organic waste water.
Further, said smooth anode substrate material is stainless steel or titanium.
Said control peristaltic pump rotating speed is meant that the rotating speed that rotates through the governor control peristaltic pump is 40-90 r/min.
Said excitation light source is source of artificial light or sunshine, and the fluorescent tube back side of source of artificial light adopts aluminium foil to reflect to improve the light source utilization ratio.
Compare prior art, the present invention has following beneficial effect:
The present invention adopts unique tilting dipolar configuration and waste water to circulate form 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 anode surface is transferred to cathode surface, has reduced energy consumption; The 3rd, at cathode surface, light induced electron directly reduces organism or generate H with the reaction of the saturated dissolved oxygen of cathode surface 2O 2, and then participate in the oxidation of organic pollutant and light induced electron is used, realize tilting bipolar bipolar economic benefits and social benefits treatment effect thus, improved degradation efficiency; The 4th, the exchange of having accelerated electrode surface and main body solution material that circulates of waste water is upgraded, and has strengthened mass transfer, makes it more efficient.And do not need applying bias, reduce energy consumption and simplified device.
Tilting bipolar liquid film photocatalytic method is handled organic waste water, adopts static electrode, is convenient to suit measures to local conditions, and makes excitation light source at applications sunshines such as landscape water body, roofs, further cuts down the consumption of energy.Make photocatalysis technology really become efficient high-level oxidation technology, its application prospect aspect the actual waste water processing is with boundless.
 
Description of drawings
The tilting bipolar liquid film photocatalytic method of Fig. 1 is handled the experimental installation synoptic diagram of organic waste water;
Among the figure: 1 is TiO 2The film anode, 2 is negative electrode, and 3 is reaction tank, and 4 is the liquid storage tank support, and 5 is peristaltic pump, and 6 is lead, and 7 is light source, and 8 for pump line waste water flows to, and 9 is liquid storage tank, and 10 is reflective aluminium foil.
 
Embodiment
Below in conjunction with accompanying drawing embodiments of the invention are elaborated.Present embodiment provided detailed embodiment and concrete operating process, but protection scope of the present invention is not limited to following embodiment being to implement under the prerequisite with technical scheme of the present invention.
Experimental equipment as shown in Figure 1, that the embodiment of the invention adopts, the embodiment treating processes is:
1) with sol-gel method with TiO 2Photocatalyst loads on and makes the light anode in the substrate, makes negative electrode with Cu, Zn, Fe or C; Liquid storage tank is located at the top of reaction tank; By the pipeline that is provided with peristaltic pump liquid storage tank and reaction tank are communicated with; Said smooth anode and negative electrode is tilting in reaction tank, the last termination liquid storage tank of said smooth anode and negative electrode, lower part of electrode is immersed in the waste water of reaction tank; Said smooth anode is connected with lead with negative electrode; Liquid storage tank 9 adopts support to be fixed in the top of reaction tank, makes treatment solution from liquid storage tank reinjects reaction tank through light anode 1 and negative electrode 2; Said smooth anode 1 is connected with negative electrode 2 usefulness leads 6;
1) start peristaltic pump 5, and the rotating speed that rotates through governor control peristaltic pump 5 is 40-90r/min, waste water pumped in the liquid storage tank 9 that waste water overflows the said smooth anode 1 of flowing through behind the liquid storage tank 9 and forms one deck liquid film with negative electrode 2 and on its surface;
2) adopt excitation light source 7 irradiates light anodes 1, make exciting light see through liquid film and shine light anode 1 surface;
3) excitation light source 7 is source of artificial light or sunshine, and source of artificial light is with aluminium foil 10 reflection sources TiO dorsad 2The exciting light of light anode one side strengthens the light source utilization ratio;
4) sampling analysis after 0.5-3 hour, organic clearance in the assaying reaction pond 3 is accomplished the processing of organic waste water.
Said sol-gel method is present mature technology, this no longer tired stating.
Embodiment 1: the tilting bipolar light catalytic treatment of different cathode materials waste water from dyestuff (referring to Fig. 1);
Process object is 20 mg L -1Famille rose (pH2.5,4.0 g/L Na 2SO 4) dye wastewater.Wastewater volume is 250ml.
1) adopt titanium as substrate, with sol-gel method with TiO 2Photocatalyst loads on and makes the light anode in the substrate; Form tilting bipolar liquid film reactor with Cu, Zn, Fe or C negative electrode respectively; Electrode is tilting in reaction tank, and its lower part is immersed in the waste water, makes treatment solution from liquid storage tank reinjects reaction tank through light anode and negative electrode; Anode is connected with lead with negative electrode.
2) start peristaltic pump, and be 40r/min, make waste water form one deck liquid film at electrode surface through the rotating speed that the governor control peristaltic pump rotates.
3) adopt 11W254nm low pressure mercury lamp irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface.
4) with aluminium foil reflection source TiO dorsad 2The exciting light of light anode one side strengthens the light source utilization ratio.
5) sampling analysis after 60 minutes is measured carmine absorbancy at the 508nm place, asks chroma removal rate (%).The result is following:
Figure 662930DEST_PATH_IMAGE001
Embodiment 2:TiO 2The tilting bipolar liquid film of/Ti and Cu is handled the different concns waste water from dyestuff;
Process object is famille rose (pH2.5, the 4.0 g/L Na of different concns 2SO 4) dye wastewater.Wastewater volume is 250ml.
1) adopt titanium as substrate, with sol-gel method with TiO 2Photocatalyst loads on makes light anode 1 and the Cu negative electrode is formed tilting bipolar liquid film reactor in the substrate, electrode is tilting in reaction tank, and lower part of electrode is immersed in the waste water, makes treatment solution from liquid storage tank reinjects reaction tank through light anode and negative electrode; Said smooth anode is connected with lead with negative electrode.
2) start peristaltic pump, the rotating speed that rotates through the governor control peristaltic pump is 40r/min, makes waste water form one deck liquid film at electrode surface.
3) adopt 11W254nm low pressure mercury lamp irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface.
4) with aluminium foil reflection source TiO dorsad 2The exciting light of light anode one side strengthens the light source utilization ratio.
5) sampling analysis after 60 minutes is measured carmine absorbancy at the 508nm place, asks percent of decolourization (%), and calculates carmine removal amount (mg), and the result is following:
It is thus clear that along with the increase of dye strength, dyestuff removal amount increases gradually, show that tilting bipolar liquid film photocatalytic method especially is fit to the treatment of high concentration waste water from dyestuff.
Embodiment 3: TiO 2The tilting bipolar liquid film photocatalysis treatment different concns waste water from dyestuff of/stainless steel and Cu;
Process object is famille rose (pH2.5, the 4.0 g/L Na of different concns 2SO 4) dye wastewater.Wastewater volume is 250ml.
1) adopt stainless steel as substrate, with sol-gel method with TiO 2Photocatalyst loads on and makes light anode 1 in the substrate; Form tilting bipolar liquid film reactor with Cu negative electrode 2; Electrode is tilting in reaction tank, lower part of electrode is immersed in the waste water, make treatment solution from liquid storage tank reinjects reaction tank through light anode and negative electrode; Said smooth anode is connected with lead with negative electrode.
2) start peristaltic pump, the rotating speed that rotates through the governor control peristaltic pump is 40r/min, makes waste water form one deck liquid film at electrode surface.
3) adopt 11W254nm low pressure mercury lamp irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface.
4) with aluminium foil reflection source TiO dorsad 2The exciting light of light anode one side strengthens the light source utilization ratio.
5) sampling analysis after 60 minutes is measured carmine absorbancy at the 508nm place, asks chroma removal rate (%), and the result is following:
Figure 733709DEST_PATH_IMAGE003
It is thus clear that when adopting stainless steel as the light anode substrate, its treatment effect is good as the treatment effect of base material not as adopting titanium among the embodiment 2, the base material titanium is superior to stainless steel.
Embodiment 4:TiO 2Tilting bipolar other dye wastewater of liquid film photocatalysis treatment of/Ti and Cu;
Process object is 20mg L -1Reactive brilliant red x-3b, red, the amaranth of temptation and erie black ATT dye wastewater.Wastewater volume is 250ml respectively, is pH2.5 and 4.0 g/L Na 2SO 4
1) adopt titanium as substrate, with sol-gel method with TiO 2Photocatalyst loads on makes the light anode and the Cu negative electrode is formed tilting bipolar liquid film reactor in the substrate, electrode is tilting in reaction tank, and lower part of electrode is immersed in the waste water, makes treatment solution from liquid storage tank reinjects reaction tank through light anode and negative electrode; Said smooth anode is connected with lead with negative electrode.
2) start peristaltic pump, the rotating speed that rotates through the governor control peristaltic pump is 40r/min, makes waste water form one deck liquid film at electrode surface.
3) adopt 11W254nm low pressure mercury lamp irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface.
4) with aluminium foil reflection source TiO dorsad 2The exciting light of light anode one side strengthens the light source utilization ratio.
5) sampling analysis after 60 minutes is measured the absorbancy of each dyestuff maximum absorption wave strong point, asks chroma removal rate (%).The result is following:
Figure 128918DEST_PATH_IMAGE004
Embodiment 5: TiO 2Dye wastewater treatment using under the tilting bipolar liquid film photochemical catalysis sunshine of/Ti and Cu;
Process object is 30mg L -1Carmine (pH2.5,4.0 g/L Na 2SO 4) dye wastewater.Wastewater volume is 250ml.
1) adopt titanium as substrate, with sol-gel method with TiO 2Photocatalyst loads on makes the light anode and the Cu negative electrode is formed tilting bipolar liquid film reactor in the substrate, electrode is tilting in reaction tank, and lower part of electrode is immersed in the waste water, makes treatment solution from liquid storage tank reinjects reaction tank through light anode and negative electrode; Said smooth anode is connected with lead with negative electrode.
2) start peristaltic pump, the rotating speed that rotates through the governor control peristaltic pump is 90r/min, makes waste water form one deck liquid film at electrode surface.
3) adopt solar light irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface.
4) 30 minutes sampling analysis in every interval in 3 hours, the absorbancy at mensuration waste water from dyestuff 508nm place is calculated percent of decolourization (%), and the result is following:
Figure 880973DEST_PATH_IMAGE005
The explanation of above-mentioned experimental result, the method for the tilting bipolar liquid film photo catalytically treating waste water of the present invention (is example with the waste water from dyestuff) is utilized source of artificial light or sunshine, and all effective degradation of dye waste water has very big application prospect in industry.
The liquid film that the present invention utilizes electrode surface to form reduces organism in the solution to the light loss that the absorption of exciting light causes, and improves the utilization ratio of exciting light; Utilize metal and N-semi-conductor TiO 2Contact inherent Schottky barrier (rather than applying bias) is transferred to cathode surface with the light induced electron of photoanode surface, directly reduces organism or generate H with the reaction of the saturated dissolved oxygen of cathode surface 2O 2, further participate in organic indirect oxidation, and TiO 2The photoanode surface photohole reaches the treatment effect of bipolar economic benefits and social benefits to organic direct oxidation together, has improved degradation efficiency; The exchange that utilizes circulating of waste water to accelerate electrode surface and main body solution material is upgraded, and reinforcing mass transfer makes it more efficient.

Claims (4)

1. the method for tilting bipolar liquid film photo catalytically treating waste water is characterized in that, comprises the steps:
The first step, with sol-gel method with TiO 2Photocatalyst loads on and makes the light anode in the substrate, makes negative electrode with Cu, Zn, Fe or C; Liquid storage tank is located at the top of reaction tank; By the pipeline that is provided with peristaltic pump liquid storage tank and reaction tank are communicated with; Said smooth anode and negative electrode is tilting in reaction tank, the last termination liquid storage tank of said smooth anode and negative electrode, lower part of electrode is immersed in the waste water of reaction tank; Said smooth anode is connected with lead with negative electrode;
Second step, start peristaltic pump, control peristaltic pump rotating speed makes waste water form one deck liquid film at said smooth anode and cathode surface;
In the 3rd step, adopt excitation light source irradiation TiO 2The light anode makes exciting light see through liquid film and shines TiO 2Catalyst surface;
The 4th step, when adopting source of artificial light with aluminium foil reflection source TiO dorsad 2The exciting light of light anode one side, the utilization ratio of raising exciting light;
In the 5th step, sampling analysis after 0.5-3 hour is measured organic clearance in the waste water, accomplishes the processing of organic waste water.
2. the method for tilting bipolar liquid film photo catalytically treating waste water according to claim 1 is characterized in that, said smooth anode substrate material is stainless steel or titanium.
3. the method for tilting bipolar liquid film photo catalytically treating waste water according to claim 1 is characterized in that, said control peristaltic pump rotating speed is meant that the rotating speed through the governor control peristaltic pump is 40-90r/min.
4. the method for tilting bipolar liquid film photo catalytically treating waste water according to claim 1 is characterized in that, said excitation light source is source of artificial light or sunshine, and the fluorescent tube back side of source of artificial light adopts aluminium foil to reflect.
CN201110343430XA 2011-11-03 2011-11-03 Method for treating organic wastewater through photocatalysis by inclined double-pole liquid film Pending CN102502941A (en)

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5308458A (en) * 1991-02-09 1994-05-03 Tioxide Group Services Limited Destruction process
JP2004249284A (en) * 2003-01-31 2004-09-09 Kansai Paint Co Ltd Waste water treatment apparatus and waste water treatment method by photocatalyst
CN101254962A (en) * 2008-04-10 2008-09-03 上海交通大学 Method for photoelectrocatalytic treatment of refractory organic wastewater by inclined plate-type liquid membrane
CN101254961A (en) * 2008-04-10 2008-09-03 上海交通大学 Method for treating refractory organic wastewater by TiO2 film electrode photoelectric turnplate
CN101353186A (en) * 2008-09-18 2009-01-28 上海交通大学 Double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing method

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5308458A (en) * 1991-02-09 1994-05-03 Tioxide Group Services Limited Destruction process
JP2004249284A (en) * 2003-01-31 2004-09-09 Kansai Paint Co Ltd Waste water treatment apparatus and waste water treatment method by photocatalyst
CN101254962A (en) * 2008-04-10 2008-09-03 上海交通大学 Method for photoelectrocatalytic treatment of refractory organic wastewater by inclined plate-type liquid membrane
CN101254961A (en) * 2008-04-10 2008-09-03 上海交通大学 Method for treating refractory organic wastewater by TiO2 film electrode photoelectric turnplate
CN101353186A (en) * 2008-09-18 2009-01-28 上海交通大学 Double turntable light-sensitive cell liquid membrane reactor photocatalysis organic wastewater processing method

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