CN103920442A - Photoelectric catalytic unit and photoelectric catalytic method - Google Patents
Photoelectric catalytic unit and photoelectric catalytic method Download PDFInfo
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- CN103920442A CN103920442A CN201410165635.7A CN201410165635A CN103920442A CN 103920442 A CN103920442 A CN 103920442A CN 201410165635 A CN201410165635 A CN 201410165635A CN 103920442 A CN103920442 A CN 103920442A
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Abstract
The invention relates to a photoelectric catalytic unit and a photoelectric catalytic method. The photoelectric catalytic unit comprises a photocatalytic film deposited on a conducting substrate, and a thermoelectric device electrically connected with the photocatalytic film, wherein the surface of the thermoelectric device is provided with a photothermal material. The photoelectric catalytic method comprises the following steps: photogenerated electrons and holes generated on the photocatalytic film deposited on the conducting substrate under the light excitation are utilized to degrade organic pollutants in contact with the photocatalytic film; and the thermoelectric device is utilized to convert heat energy, which is generated by the photothermal material on the surface under the irradiation of visible light or infrared light, into electric energy, and apply the electric energy onto the photocatalytic film electrically connected with the photocatalytic film to promote the separation of the photogenerated electrons and the holes.
Description
Technical field
The present invention relates to a kind of photoelectrocatalysidevice device and photoelectrocatalysis method, be specifically related to a kind of photocatalysis apparatus and the photoelectrocatalysis method of photocatalysis film and thermo-electric device coupling.
Background technology
Environmental pollution and energy crisis are the two large bottlenecks that restrict at present human social development, and Photocatalitic Technique of Semiconductor is expected to solve this two hang-up, and its research and application have caused people's extensive concern.Photocatalysis depollution of environment technology is to utilize the process of photo-excited semiconductor decomposing organic matter.Its mechanism is that semiconductor light-catalyst is subject to optical excitation to produce nonequilibrium carrier be light induced electron and hole, electronics and hole migration are after semiconductor surface, owing to thering is very strong oxidation and reducing power, can, with the organic pollution generation redox reaction contacting with it, by organic substance decomposing, be that little molecule is also finally decomposed into CO
2and water.Because photocatalysis can utilize the luminous energy long-term work of occurring in nature, Shi Qi environmental pollution improvement field has broad application prospects.The approach of Photocatalitic Technique of Semiconductor alleviating energy crisis is to realize by its photocatalytic hydrogen production by water decomposition.Its mechanism is that semiconductor light-catalyst is subject to after optical excitation, and the electron hole of generation moves to behind surface respectively and water generation redox reaction, generates hydrogen and oxygen.
The key problem one of restriction photocatalysis technology large-scale application is that photocatalysis efficiency is low at present, the 2nd, and solar energy utilization ratio is low.Photocatalysis performance depends on the separative efficiency that light induced electron-hole is right to a great extent.Separative efficiency is higher, and catalytic activity is general also better.Therefore suppressing being compounded with of electronics-hole is beneficial to raising catalytic performance.Because the conduction band of semiconductor light-catalyst is limited to the capture ability of high activity electronics, easily cause the compound again of high activity electronics and photohole.And photoelectrocatalysis can utilize the anode of extra electric field, catch high activity electronics, thereby avoided the compound again of photohole and high activity electronics, thereby improved light-catalyzed reaction efficiency.Because current photoelectrocatalysis needs additional power source, cost is higher, so photoelectrocatalysis technology does not obtain large-scale promotion in actual applications yet.How to realize that not need the photoelectrocatalysis of additional power source be current technical barrier.
Summary of the invention
The present invention is intended to overcome the defect of existing photocatalysis method, the invention provides a kind of photocatalysis apparatus and photocatalysis method.
First, the invention provides a kind of photocatalysis apparatus, described photoelectrocatalysidevice device comprises: be deposited on the photocatalysis film in conductive substrates, and the thermo-electric device being electrically connected to described photocatalysis film, wherein, the surface of described thermo-electric device has photic hot material.
In photocatalysis apparatus of the present invention, photocatalysis film and thermo-electric device coupling, the electromotive force producing because of thermo-electric device is on the one hand applied on photocatalysis film and has promoted photo-generated carrier separated, without additional power source, can greatly improve photocatalysis efficiency.And the electric energy that produces of thermo-electric device only need infrared light, visible ray according under can realize, so this device has also increased solar energy utilization ratio.Compare traditional photoelectrocatalysidevice device, this invention has not only improved catalytic efficiency but also improved light-use, has more application prospect.
Preferably, the material of described photocatalysis film is selected from ultraviolet, visible or infrared light catalytic material, comprises Bi
2wO
6, BiVO
4, TiO
2, SrTiO
3, WO
3, ZnO, MoS
2.
Preferably, described photic hot material is selected from carbon class, sulfide narrow gap semiconductor class or noble metal optothermal material, comprises graphene oxide, CuS, Au, Ag, CNT.
Preferably, described thermo-electric device is electrically connected to described photocatalysis film by conducting resinl.
On the other hand, the present invention also provides a kind of photoelectrocatalysis method, and described photoelectrocatalysis method comprises:
Utilization is deposited on the organic pollution that light induced electron that the photocatalysis film in conductive substrates produces under optical excitation contacts with it with hole degraded;
The heat energy that utilizes thermo-electric device that the photic hot material on its surface is produced under the irradiation of visible or infrared light, is converted into electric energy and is applied on the photocatalysis film with its electrical connection to promote described light induced electron separated with hole.
In method of the present invention, utilize photocatalysis film and thermo-electric device coupling, the electromotive force producing because of thermo-electric device is on the one hand applied on photocatalysis film and has promoted photo-generated carrier separated, without additional power source, can greatly improve photocatalysis efficiency.And method of the present invention can also improve solar energy utilization ratio.Compare traditional photoelectrocatalysis method, this invention has not only improved catalytic efficiency but also improved light-use, and the invention process is without special installation and harsh conditions, and technique is simple, and controllability is strong, easily accomplishes scale production, and has practicality.
Preferably, the material of described photocatalysis film is selected from ultraviolet, visible or infrared light catalytic material, comprises Bi
2wO
6, BiVO
4, TiO
2, SrTiO
3, WO
3, ZnO, MoS
2.
Preferably, described photic hot material is selected from carbon class, sulfide narrow gap semiconductor class or noble metal optothermal material, comprises graphene oxide, CuS, Au, Ag, CNT.
Preferably, described thermo-electric device is electrically connected to described photocatalysis film by conducting resinl.
Preferably, described organic pollution comprises alkane and arene organic pollution, organic dyestuff, inorganic ammonia nitrogen, specifically comprises phenol, formaldehyde.
Beneficial effect of the present invention:
1) device of the thermo-electric device being obtained by the present invention and catalysis material coupling, the electromotive force producing because of thermo-electric device is applied on photocatalysis film and has promoted photo-generated carrier separated, can greatly improve photocatalysis efficiency.And the electric energy that produces of thermo-electric device only need infrared light, visible ray according under can realize, so this device has also increased solar energy utilization ratio.Compare traditional photocatalysis method, this invention has not only improved catalytic efficiency but also improved light-use, has more application prospect;
2) the invention process is without special installation and harsh conditions, and technique is simple, and controllability is strong, easily accomplishes scale production, and has practicality;
3) this device and method can be used for without fields such as the photoelectric catalysis degrading pollutant of additional power source and photoelectrocatalysis hydrogen manufacturing.
Accompanying drawing explanation
Fig. 1 is the schematic diagram that photoelectrocatalysis is carried out in thermo-electric device and catalysis material coupling;
Fig. 2 is the thermograph of thermo-electric device under Infrared irradiation in an embodiment of the invention;
Fig. 3 is thermo-electric device and Bi in an embodiment of the invention
2wO
6after photocatalysis film coupling to the photoelectric catalysis degrading efficiency of phenol in water and the comparison diagram of common photocatalytic degradation efficiency.
The specific embodiment
By the following specific embodiment and with reference to accompanying drawing, the present invention is described in further detail; be interpreted as; following embodiment is only to explanation of the present invention; be not the restriction to content of the present invention, any technical scheme that content of the present invention is not done to material alteration still falls into protection scope of the present invention.
The invention discloses a kind of photoelectrocatalysis method without additional power source, described method adopts thermo-electric device and catalysis material coupling to realize, and comprising: the preparation of photocatalysis film material in conductive substrates; Thermo-electric device surface light hot material applies; Photocatalysis film is electrically connected to thermo-electric device; Under illumination condition, excite thermo-electric device and photocatalysis film etc. simultaneously.The photoelectrocatalysis method being provided by the inventive method, can more effectively utilize solar energy to realize the technology such as the photocatalysis depollution of environment and photocatalytic hydrogen production by water decomposition, and the bias voltage producing due to thermo-electric device is added in and on photocatalysis film, has realized photoelectrocatalysis, the method has higher photocatalytic activity than traditional photocatalysis, has broad application prospects; And the method for the invention is without special installation and harsh conditions, and technique is simple, and controllability is strong, easily realize scale volume production, there is high practicality.
The invention provides a kind of photoelectrocatalysis method without additional power source, comprise following concrete steps:
A) catalysis material is deposited on and in conductive substrates, prepares photocatalysis film;
B) thermo-electric device surface is applied to the photic hot material of one deck;
C) by thermo-electric device or step b) thermo-electric device of the band coating that obtains is connected on step photocatalysis film a);
D) thermo-electric device combining and photocatalysis film are placed under light source and irradiate and carry out photoelectrocatalysis.
The catalysis material of step described in a) comprises all UV, visible lights and infrared ray excited catalysis material, for example Bi
2wO
6, TiO
2, BiVO
4, TiO
2, SrTiO
3, WO
3, ZnO, MoS
2deng semiconductor ultraviolet, visible and infrared light catalytic material.Conductive substrates comprises and is not limited to FTO, ito glass etc.
Step b) photic hot material described in comprises all materials that can be heat energy by transform light energy, such as graphene oxide, CuS, Au, Ag, CNT etc.
Step c), in, one end of thermo-electric device can be electrically connected to photocatalysis film by conductors such as conducting resinls.But should understand the conductor that can be used for being electrically connected to, be not limited to conducting resinl, such as adopting conductive paper, conductive clip, conductor wire etc.
Steps d) light source described in comprises sunshine, the light source of some forms such as artificial light.
As a kind of preferred version, step a) described in catalysis material adopt and to be deposited on FTO Bi on glass
2wO
6nano thin-film.
As a kind of preferred version, step b) described in the photic hot material on thermo-electric device surface adopt graphene oxide.
As a kind of preferred version, steps d) described in light source adopt the visible and infrared light part in xenon lamp and infrared lamp simulated solar irradiation.
The method can be used for without fields such as the photoelectric catalysis degrading pollutant of additional power source and photoelectrocatalysis hydrogen manufacturing.Catalysis material and thermo-electric device coupling, to improve the method for photocatalysis efficiency, belong to photocatalysis technology field.
For the low problem of the low catalytic efficiency causing of solar energy utilization ratio in current photocatalysis technology.Current research is mainly to prepare visible light catalytic material to substitute traditional TiO2 ultraviolet light catalyst.But visible ray also only accounts in solar spectral 43% energy.In solar energy, accounting for most infrared lights can not be utilized by catalysis material at present.In view of current existing photochemical catalyst is in the defect aspect light-use, research and develop new and effective infrared optical response photocatalysis technology, being to utilize solar energy to realize the key of optical catalytic environment purification and photolysis water hydrogen, is also that practical inexorable trend and developing direction further moved towards in photocatalysis.Although infrared light can not directly excite most photochemical catalysts, it has good pyrogenicity effect, so we consider that utilizing thermo-electric device to be converted to electric energy this part energy is used.Because thermo-electric device surfacing can not fully absorb solar energy mid-infrared light, need to apply on thermo-electric device surface one deck infrared light pyrogenicity material, graphene oxide as more in current research.Graphene oxide has good dispersiveness in water, and rich surface is containing oxy radical, and surface can be larger.These features make it easily on thermo-electric device surface, form evenly firmly coating, and the solar heat that increases thermo-electric device is sent a telegraph responding ability.
Based on above technical need, we develop a kind of method of thermo-electric device and catalysis material coupling raising photocatalysis efficiency, improve photocatalysis efficiency when increasing solar energy utilization ratio.The method utilizes the thermic electrical effect of thermo-electric device that infrared part in solar energy is converted to electric energy, although this part electric energy producing is less, can not brine electrolysis or pollutant, but it can fill-in light catalysis material, thereby utilize photoelectrocatalysis to improve the efficiency of electron hole separative efficiency raising catalysis material in catalysis material, realize the full spectrum utilization of solar energy in photocatalysis technology simultaneously.This technology has important scientific value and has again and curb environmental pollution and the practical significance of alleviating energy crisis, for the practical application of solar energy photocatalytic technology provides a feasible technology path.
Compared with prior art, the present invention has following beneficial effect:
1) device of the thermo-electric device being obtained by the inventive method and catalysis material coupling, the electromotive force producing because of thermo-electric device is applied on photocatalysis film and has promoted photo-generated carrier separated, can greatly improve photocatalysis efficiency.And the electric energy that produces of thermo-electric device only need infrared light according under can realize, so this device has also increased solar energy utilization ratio.Compare traditional photocatalysis method, this invention has not only improved catalytic efficiency but also improved light-use, has more application prospect;
2) the invention process is without special installation and harsh conditions, and technique is simple, and controllability is strong, easily accomplishes scale production, and has practicality.
Fig. 1 is the schematic diagram that photoelectrocatalysis is carried out in thermo-electric device and catalysis material coupling;
Fig. 2 is the thermograph of thermo-electric device under Infrared irradiation in an embodiment of the invention;
Fig. 3 is thermo-electric device and Bi in an embodiment of the invention
2wO
6after photocatalysis film coupling to the photoelectric catalysis degrading efficiency of phenol in water and the comparison diagram of common photocatalytic degradation efficiency.
Below further list some exemplary embodiments so that the present invention to be described better.Should understand; the above-mentioned embodiment that the present invention describes in detail; and following examples are only not used in and limit the scope of the invention for the present invention is described, some nonessential improvement that those skilled in the art's foregoing according to the present invention is made and adjust and all belong to protection scope of the present invention.In addition, the concrete proportioning in following technological parameter, time, temperature etc. are only also exemplary, and those skilled in the art can select suitable value in the scope of above-mentioned restriction.
Described in embodiment " graphene oxide ", be reference literature (Phys.Chem.Chem.Phys.2011,13,2887-2893.) preparation and obtain; Thermo-electric device adopts commercial p-n junction type thermo-electric device (p:Bi
2te
3– Sb
2te
3, n:Bi
2te
3– Bi
2se3).
Embodiment 1
The graphene oxide of the 0.5g/L that 1mL is dispersed in water is coated in thermo-electric device surface and dries in 60 ℃ of thermostatic drying chambers; Reference literature (J.Phys.Chem.C2012,116,19413 – 19418.) is prepared FTO/Bi
2wO
6nano thin-film;
Thermo-electric device one end is connected to FTO/Bi by conducting resinl
2wO
6on nano thin-film, prepare photoelectrocatalysidevice device.
Fig. 1 is the device schematic diagram that in the present embodiment, photoelectrocatalysis is carried out in thermo-electric device and catalysis material coupling.
Fig. 2 is the thermal imaging picture of thermo-electric device under Infrared irradiation in the present embodiment, and in Fig. 2, a is the thermo-electric device that is coated with one deck graphene oxide, and in Fig. 2, b represents uncoated thermo-electric device.Be coated with as seen from Figure 2 after one deck graphene oxide, thermo-electric device two ends Temperature Difference Ratio does not have cated device to have obvious increase, shows to have the thermo-electric device of pyrogenicity coating to have stronger thermic power.
Photocatalysis performance for institute system thermo-electric device and catalysis material combined apparatus, designs the experiment of degradation of phenol under infrared and visible ray.Phenol is hard degradation under field conditions (factors), and toxicity is larger, there is no photoactivate phenomenon, so degradation of phenol can be weighed photocatalysis performance well.In experiment, pass through UV absorption spectrometry phenol solution in the absorbance of 269nm, characterize the variation of Phenol in Aqueous Solution concentration, and then draw degradation rate.
Simple light catalysis experiment is by FTO/Bi
2wO
6it is in the phenol solution of 8mg/L that nano thin-film adds 10mL concentration, is then placed under 300W xenon lamp and irradiates, and detects phenol absorbance and records result.The auxiliary photoelectrocatalysis experiment of thermo-electric device is under the same conditions by FTO/Bi
2wO
6nano thin-film one end is connected on thermo-electric device, thermo-electric device is placed under infrared light simultaneously.
Fig. 3 is thermo-electric device in this enforcement and Bi
2wO
6after photocatalysis film coupling to the photoelectric catalysis degrading efficiency of phenol in water and the comparison diagram of common photocatalytic degradation efficiency, as seen from Figure 3, thermo-electric device and Bi
2wO
6after photocatalysis film coupling, the photoelectric catalysis degrading rate of phenol in water has been improved to nearly 2 times than normal optical catalysis degradation modulus.
Embodiment 2
The difference of the present embodiment and embodiment 1 is only: the photocatalysis film of employing is by commercial TiO
2(P25) be deposited on FTO film;
All the other contents are all with identical described in embodiment 1.
Analyze and learn after testing: thermo-electric device and TiO in the present embodiment
2after photocatalysis film coupling to the photoelectric catalysis degrading efficiency of phenol in water than simple TiO
2photocatalytic degradation efficiency is significantly improved.
Embodiment 3
The difference of the present embodiment and embodiment 1 is only: thermo-electric device face coat adopts CuS to replace graphene oxide;
All the other contents are all with identical described in embodiment 1.
Analyze and learn after testing: the thermo-electric device ratio that applies CuS in the present embodiment does not have the two ends temperature difference under cated the same terms to be significantly increased, and thermo-electric device and Bi yet
2wO
6after photocatalysis film coupling to the photoelectric catalysis degrading efficiency of phenol in water than simple Bi
2wO
6photocatalytic degradation efficiency is also significantly improved.
The invention process is without special installation and harsh conditions, and technique is simple, and controllability is strong, easily accomplishes scale production, and has practicality; This device and method can be used for without fields such as the photoelectric catalysis degrading pollutant of additional power source and photoelectrocatalysis hydrogen manufacturing.
Claims (9)
1. a photoelectrocatalysidevice device, is characterized in that, described photoelectrocatalysidevice device comprises:
Be deposited on the photocatalysis film in conductive substrates, and the thermo-electric device being electrically connected to described photocatalysis film, wherein, the surface of described thermo-electric device has photic hot material.
2. photoelectrocatalysidevice device according to claim 1, is characterized in that, the material of described photocatalysis film is selected from ultraviolet, visible or infrared light catalytic material, comprises Bi
2wO
6, BiVO
4, TiO
2, SrTiO
3, WO
3, ZnO, MoS
2.
3. photoelectrocatalysidevice device according to claim 1 and 2, is characterized in that, described photic hot material is selected from carbon class, sulfide narrow gap semiconductor class or noble metal optothermal material, comprises graphene oxide, CuS, Au, Ag, CNT.
4. according to the photoelectrocatalysidevice device described in any one in claim 1-3, it is characterized in that, described thermo-electric device is electrically connected to described photocatalysis film by conducting resinl.
5. a photoelectrocatalysis method, is characterized in that, described photoelectrocatalysis method comprises:
Utilization is deposited on the organic pollution that light induced electron that the photocatalysis film in conductive substrates produces under optical excitation contacts with it with hole degraded;
The heat energy that utilizes thermo-electric device that the photic hot material on its surface is produced under the irradiation of visible or infrared light, is converted into electric energy and is applied on the photocatalysis film with its electrical connection to promote described light induced electron separated with hole.
6. photoelectrocatalysis method according to claim 5, is characterized in that, the material of described photocatalysis film is selected from ultraviolet, visible or infrared light catalytic material, comprises Bi
2wO
6, BiVO
4, TiO
2, SrTiO
3, WO
3, ZnO, MoS
2.
7. according to the photoelectrocatalysis method described in claim 5 or 6, it is characterized in that, described photic hot material is selected from carbon class, sulfide narrow gap semiconductor class or noble metal optothermal material, comprises graphene oxide, CuS, Au, Ag, CNT.
8. according to the photoelectrocatalysis method described in any one in claim 5-7, it is characterized in that, described thermo-electric device, by conducting resinl, conductive paper, conductive clip or conductor wire, is electrically connected to described photocatalysis film.
9. according to the photoelectrocatalysis method described in any one in claim 5-8, it is characterized in that, described organic pollution comprises alkane and arene organic pollution, organic dyestuff, inorganic ammonia nitrogen, specifically comprises phenol, formaldehyde.
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| US11833490B1 (en) | 2019-06-11 | 2023-12-05 | Imam Abdulrahman Bin Faisal University | Green synthesis method for making a photocatalyst nanocomposite |
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| CN112138537B (en) * | 2019-06-27 | 2022-04-19 | 奇鼎科技股份有限公司 | Filter screen structure of photocatalytic decomposition material |
| CN111957297A (en) * | 2020-08-20 | 2020-11-20 | 常州良福朗清生物科技有限公司 | Preparation method and application of nano CuS-loaded sulfur and nitrogen co-doped graphene aerogel |
| CN113818030A (en) * | 2021-09-30 | 2021-12-21 | 北华航天工业学院 | Electro-catalysis hydrogen production integrated system based on Au @ rGO-PEI/PVB photo-thermal-thermoelectric driving, preparation and application |
| CN113818030B (en) * | 2021-09-30 | 2022-09-02 | 北华航天工业学院 | Electro-catalytic hydrogen production integrated system based on Au @ rGO-PEI/PVB photo-thermal-thermoelectric driving, preparation and application |
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