CN102306802A - Nanotube array fuel battery of visible light response - Google Patents
Nanotube array fuel battery of visible light response Download PDFInfo
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- CN102306802A CN102306802A CN201110203146A CN201110203146A CN102306802A CN 102306802 A CN102306802 A CN 102306802A CN 201110203146 A CN201110203146 A CN 201110203146A CN 201110203146 A CN201110203146 A CN 201110203146A CN 102306802 A CN102306802 A CN 102306802A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/30—Hydrogen technology
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Abstract
The invention discloses a nanotube array fuel battery of visible light response, which comprises a photoanode, a cathode, organic waste water, a light source, an electrolyte and a quartz reaction pool, wherein the cathode and the photoanode are respectively inserted into the organic waste water containing the electrolyte and is communicated through an external circuit; the photoanode is an electrode made from a TiO2 nanotube array film with visible light response; the light source is started for irradiating the photoanode; air is continuously introduced near the cathode; at this time, organic matter is oxidized near the photoanode; and generated electrons are transferred to the cathode through loads of the external circuit and are reduced by oxygen near the cathode. According to the invention, the purposes of treating the organic waste water and externally generating power are achieved; and the nanotube array fuel battery has higher battery performance and wider application prospect compared with the prior art.
Description
Technical field
The present invention relates to fuel cell, particularly a kind of visible light-responded nano-tube array fuel cell belongs to control and the utilization of new energy resources field of polluting.
Background technology
In recent years, along with the surge of population and the fast development of industry, a large amount of poisonous and hazardous industrial wastewaters and sanitary sewage drain into water body, have caused serious environmental to pollute and ecological disruption.Meanwhile, the organic substance in the waste water also is an important energy.Therefore, how can handle waste water apace, can reclaim the energy again efficiently simultaneously and then become a very significant research topic.
Based on the principle of primary cell, the organic substance in the waste water as substrate, is designed a kind of battery system and can will be converted into electric energy to organic chemical energy, then both can realize the recycling of the energy again to realizing treatment of organic matters of organic.1991, Habermann and Pommer at first attempted with the organic substance in the waste water as substrate, utilized microbiological fuel cell to handle organic substance and generating (W. Habermann; E. H. Pommer; Appl. Microbiol. Biotechnol. 1991,35, and 128).Microbiological fuel cell is under anoxia condition, utilize microbe with organic electron transport to anode, transfer to negative electrode and final then and realize generating (B. E. Logan, Nat. Rev. Microbiol. 2009,7,375).The key factor that influences the microbiological fuel cell performance is the electron transport efficient in the living things system.Yet the electron transfer process of microorganism system is very complicated, and electron transport speed is also slow relatively, and this has had a strong impact on the performance of battery.In addition, microbiological fuel cell also exists deficiencies such as the long and service conditions harshness of complicated operation, microbe culture, start-up time.
2006, Japanese scholar Kaneko etc. (M. Kaneko, J. Nemoto, H. Ueno, N. Gokan, K. Ohnuki, M. Horikawa, R. Saito, T. Shibata,
Electrochem. Commun.2006,8,336) proposed with TiO
2Photocatalysis technology is the fuel cell on basis, and it is with TiO
2Membrane electrode is the light anode, and oxidation of organic compounds is come in the hole that utilizes photocatalytic process to produce, and simultaneously light induced electron is passed to negative electrode, thereby realizes the dual purpose of fast processing organic substance and generating.This method is compared with traditional microbiological fuel cell, and the formation of electronics and transmission are more direct and quick, thereby show higher battery efficiency.But also there is obvious defects in existing photocatalysis fuel cell, and it adopts the powder nano-TiO
2Film is as the light anode, and this smooth anode material is to go up through the electro-conductive glass (FTO) that mixes at F to apply one deck powder nano-TiO
2Film and obtaining.But the photogenerated charge of this material is compound higher, TiO
2Nano particle very easily comes off from substrate, and electrode life is shorter, and can only response wave length short ultraviolet light and can not responding to visible light.
Summary of the invention
The objective of the invention is to deficiency, a kind of visible light-responded nano-tube array fuel cell is provided, utilize visible light-responded nano-tube array fuel cell to prior art.The electrode performance of this fuel cell is more stable, and battery performance is better, and can responding to visible light.
The present invention realizes through following technical scheme:
A kind of visible light-responded nano-tube array fuel cell comprises light anode, negative electrode, organic wastewater, light source, electrolyte and quartz reaction pond, and described negative electrode, light anode insert respectively and contain in the electrolytical organic wastewater, and is communicated with through external circuit.Its characteristics are that described smooth anode is by having visible light-responded TiO
2Nano-pipe array thin film is processed.Open light source irradiation light anode; And near negative electrode, continue bubbling air; Organic substance will be oxidized near the light anode this moment; The electronics that produces will be through the external circuit load transfer to negative electrode; And by near the oxygen reduction the negative electrode; Thereby can realize both having handled organic wastewater, again the purpose of externally generating electricity.
Described have a visible light-responded TiO
2Nano-pipe array thin film is via CdS or Cu
2The TiO of O modified
2Nano-pipe array thin film.
Described light source is the simulated solar light source, or natural sunlight.
Described negative electrode is the platinized platinum electrode that plated platinum black.
Described electrolyte is the metabisulfite solution of concentration 0.1 ~ 0.5 M.
Described TiO
2The preparation method of nano-pipe array thin film is: at first with the metallic titanium plate cleaned as anode; Place the aqueous solution that contains 0.5% hydrofluoric acid; With platinum electrode for being 20V to electrode regulating voltage; Reaction system is being carried out under the lasting ultrasonic situation of ultrasonic wave; Metallic titanium plate was carried out anodic oxidation 30 minutes; Obtain the titanium based titanium oxide nano-tube array material that the titanium oxide by Titanium and titanium surface constitutes, described then titanium based titanium oxide nano-tube array material is through 450
°Behind the C high temperature sintering 3 hours, obtain having the TiO of anatase phase
2The nano-pipe array thin film material.
The described TiO that modifies through CdS
2The preparation method of nano-tube array film electrode adopts ultrasonic electro-deposition techniques to prepare, and its concrete preparation method is: with described TiO
2Nano-pipe array thin film is a negative electrode, and platinized platinum is an anode, is containing 0.05 M CdCl
2With apply bias voltage 0.44 V in the dimethyl sulfoxide solution of 0.1 M elemental sulfur, electro-deposition 10 minutes, it is ultrasonic that whole process adopts ultrasonic wave to continue.
Described through Cu
2The TiO that O modifies
2The preparation method of nano-tube array film electrode prepares for adopting ultrasonic electro-deposition techniques, and its concrete preparation method is: with described TiO
2Nano-tube array film electrode is an anode, and Pt is to electrode, and Ag/AgCl is a reference electrode, in the electrolyte solution that contains sodium acetate 0.1 M, Schweinfurt green 0.02 M, applies bias voltage-0.25 V, and deposition process continues 5 minutes, and it is ultrasonic that whole process adopts ultrasonic wave to continue.
Major advantage of the present invention is:
(1) TiO that adopts ultrasonic anodic oxidation to prepare
2Nano-pipe array thin film light anode, nanotube is short and solid, has good photocatalysis performance and mechanical stability; Adopt ultrasonic electrodeposition technology for preparing through CdS or Cu
2The TiO that O modifies
2Nano-tube array film electrode has good catalytic performance and mechanical stability.
(2) adopt through CdS or Cu
2The TiO of O modified
2Nano-tube array film electrode has the high visible light response performance, can utilize visible light.
(3) therefore, the visible light-responded nano-tube array fuel cell of the present invention can utilize visible light-responded processing and the generating of carrying out waste water, and electrode has good stable property and advantages of high catalytic activity.
Description of drawings
Fig. 1 is the structure and the fundamental diagram of the visible light-responded nano-tube array fuel cell of the present invention.
Three kinds of optoelectronic pole ultraviolet-visibles of Fig. 2 the present invention diffuse reflectance spectra spectrogram comparison diagram.
Embodiment
Below in conjunction with embodiment and accompanying drawing the present invention is elaborated, but should not limit protection scope of the present invention with this.
See also Fig. 1 earlier, Fig. 1 is the structure and the fundamental diagram of the visible light-responded nano-tube array fuel cell of the present invention.Visible by figure; The nano-tube array fuel cell that the present invention is visible light-responded; Comprise light anode 1, negative electrode 2, organic wastewater, light source, electrolyte and quartz reaction pond; Described negative electrode, light anode insert respectively and contain in the electrolytical organic wastewater; And through external circuit 3 connections, its characteristics are that described smooth anode 1 is by having visible light-responded TiO
2Nano-pipe array thin film is processed, or by CdS or Cu
2The TiO of O modified
2Nano-tube array film electrode.Open light source irradiation light anode 1; And near negative electrode 2, continue bubbling air; Organic substance will be oxidized near light anode 1 this moment; The electronics that produces will be through external circuit 3 load transfer to negative electrode 2; And by near the oxygen reduction the negative electrode 2; Thereby can realize both having handled organic wastewater, again the purpose of externally generating electricity.
Described light source is the simulated solar light source, or natural sunlight.
Described negative electrode is the platinized platinum electrode that plated platinum black.
Described electrolyte is the metabisulfite solution of concentration 0.1-0.5 M.
The preparation method of light anode of the present invention is described with embodiment below.
With the Titanium cleaned as anode; Place the aqueous solution that contains 0.5% hydrofluoric acid; With platinum electrode for being 20 V to electrode and regulation voltage; Reaction system is being carried out under the lasting ultrasonic situation of ultrasonic wave; Titanium is carried out anodic oxidation 30 min, obtain the titanium based titanium oxide nano-tube array material that constitutes by Titanium and the surperficial titanium oxide of titanium.Then with described titanium based titanium oxide nano-tube array material warp 450
°Behind the C high temperature sintering 3 hours, can obtain having the TiO of anatase phase
2The nano-pipe array thin film material.
With the TiO that makes
2Nano-tube array film electrode is a negative electrode, and platinized platinum is an anode, is containing 0.05 M CdCl
2With apply bias voltage 0.44 V in the dimethyl sulfoxide solution of 0.1 M elemental sulfur, electro-deposition 10 min, it is ultrasonic that whole process adopts ultrasonic wave to continue, and can obtain through CdS/TiO
2The nano-tube array combination electrode.
Through three kinds of optoelectronic pole ultraviolet-visibles of test the present invention diffuse reflectance spectra spectrogram comparison diagram as shown in Figure 2, among the figure, (1) expression TiO
2The diffuse reflectance spectra of nano-tube array film electrode, (2) CdS/TiO
2The diffuse reflectance spectra of nano-pipe array thin film combination electrode and (3) Cu
2O/TiO
2The diffuse reflectance spectra spectrum of nano-pipe array thin film combination electrode.Visible by Fig. 2, without the TiO that modifies
2Nano-tube array film electrode only has absorption at the ultraviolet region that is lower than 370nm, and for through CdS or Cu
2The combination electrode that O modifies, its absorption region then obviously expands to the visible region, and CdS or Cu are described
2The combination electrode that O modifies has visible light-responded performance.
With CdS/TiO
2The nano-tube array combination electrode is a light anode 1, and the platinized platinum that plated platinum black is a negative electrode 2.Cathode and anode is inserted respectively in the simulative organic wastewater that contains 0.1 M sodium sulphate, and be communicated with through external circuit 3.(light intensity is 100 mW cm to open the simulated solar light source
-2) irradiates light anode 1; And near negative electrode 2, continue bubbling air, and the organic substance in the waste water is oxidized near light anode 1 at this moment, and the electronics of generation passes through external circuit 3 load transfer to negative electrode; Near the negative electrode oxygen is reduced, and can realize the purpose of organic degraded and generating simultaneously.If simulated wastewater is respectively 0.05 M phenol, 0.22 mM tetracycline, when 0.27 mM is Congo red, measures through electrochemical workstation, open circuit voltage, short circuit current and maximum power density that the visible light catalytic fuel cell system produces are seen table 1.
As reference examples, under identical condition, respectively with TiO
2Nano-pipe array thin film (TNA) or conventional Ti O
2Film is the light anode; With simulated wastewater 0.05 M phenol, 0.22 mM tetracycline, 0.27 mM is Congo red is that substrate generates electricity; Measure through electrochemical workstation, open circuit voltage, short circuit current and maximum power density that the visible light catalytic fuel cell system produces are seen table 1.
Visible by table 1 data, TiO
2Nano-pipe array thin film is than traditional T iO
2Film has higher battery performance under simulated solar irradiation; In addition, via Cu
2The combination electrode material of O or CdS modified has the TiO of ratio
2The battery performance that nano-pipe array thin film obviously improves.
With the TiO that makes among the embodiment 1
2Nano-tube array film electrode is an anode, and Pt is to electrode, and Ag/AgCl is a reference electrode; In the electrolyte solution that contains sodium acetate 0.1 M, Schweinfurt green 0.02 M, apply bias voltage-0.25 V; Deposition process continues 5 min, and it is ultrasonic that whole process adopts ultrasonic wave to continue, and can obtain Cu
2O/TiO
2The nano-tube array combination electrode.
With Cu
2O/TiO
2The nano-tube array combination electrode is a light anode 1, and the platinized platinum that plated platinum black is a negative electrode 2.Negative electrode, anode are inserted respectively in phenol (0.05 M) solution that contains 0. 5 M sodium sulphate, and be communicated with through external circuit 3.(light intensity is 100 mW cm to open the simulated solar light source
-2) the irradiates light anode, and near negative electrode, continue bubbling air, and this moment, phenol was oxidized near the light anode, and the electronics of generation to negative electrode, by near the oxygen reduction the negative electrode, can be realized the purpose of the degraded and the generating of phenol through the external circuit load transfer simultaneously.Measure through electrochemical workstation, the open circuit voltage that this visible light catalytic fuel cell system produces is 0.91V, short circuit current 1.30 mA cm
-2With maximum power density 0.43 mW cm
-2
With the TiO that makes among the embodiment 1
2Nano-tube array film electrode is a negative electrode, and platinized platinum is an anode, is containing 0.05 M CdCl
2With apply bias voltage 0.44 V in the dimethyl sulfoxide solution of 0.1 M elemental sulfur, electro-deposition 10 min, it is ultrasonic that whole process adopts ultrasonic wave to continue, and can obtain CdS/TiO
2The nano-tube array combination electrode.
With CdS/TiO
2The nano-tube array combination electrode is a light anode 1, and the platinized platinum that plated platinum black is a negative electrode 2.Cathode and anode is inserted respectively in acetate (0.3 mM) solution that contains 0.25 M sodium sulphate, and be communicated with through external circuit 3.Utilize nature solar light irradiation light anode 1; And near negative electrode 2, continue bubbling air, and this moment, acetate was oxidized near the light anode, and the electronics of generation passes through the external circuit load transfer to negative electrode; Near the negative electrode oxygen is reduced, and can realize the purpose of the degraded and the generating of acetate simultaneously.Measure through electrochemical workstation, the open circuit voltage that this visible light catalytic fuel cell system produces is 0.88 V, short circuit current 0.57 mA cm
-2With maximum power density 0.31 mW cm
-2
Table 1 has provided that (light intensity is 100 mW cm under simulated solar irradiation
-2) test, three kinds of simulative organic wastewaters are matrix, the open circuit voltage (V) of the fuel cell system of the anode material of not sharing the same light, short circuit current (mA cm
-2) and power density (mW cm
-2), visible by table 1, TiO
2Nanometer pipe array electrode shows than conventional Ti O
2The battery performance that the powder membrane electrode is more excellent; The battery performance of complex light anode material is then than TiO
2Nanometer pipe array electrode is better.
Claims (8)
1. visible light-responded nano-tube array fuel cell; Comprise light anode (1), negative electrode (2), organic wastewater, light source, electrolyte and quartz reaction pond; Described negative electrode (2), light anode (1) insert respectively and contain in the electrolytical organic wastewater; And, it is characterized in that described smooth anode (1) is by having visible light-responded TiO through external circuit (3) connection
2Nano-pipe array thin film is processed.
2. visible light-responded nano-tube array fuel cell according to claim 1 is characterized in that the described visible light-responded TiO that has
2Nano-pipe array thin film is via CdS or Cu
2The TiO of O modified
2Nano-pipe array thin film.
3. visible light-responded nano-tube array fuel cell according to claim 1 is characterized in that described light source is the simulated solar light source, or natural sunlight.
4. visible light-responded nano-tube array fuel cell according to claim 1 is characterized in that described negative electrode (2) is the platinized platinum electrode that plated platinum black.
5. visible light-responded nano-tube array fuel cell according to claim 1 is characterized in that described electrolyte is the metabisulfite solution of concentration 0.1-0.5 M.
6. visible light-responded nano-tube array fuel cell according to claim 1 is characterized in that described TiO
2The preparation method of nano-pipe array thin film is: at first with the metallic titanium plate cleaned as anode; Place the aqueous solution that contains 0.5% hydrofluoric acid; With platinum electrode for being 20V to electrode regulating voltage; Reaction system is being carried out under the lasting ultrasonic situation of ultrasonic wave; Metallic titanium plate was carried out anodic oxidation 30 minutes; Obtain the titanium based titanium oxide nano-tube array material that the titanium oxide by Titanium and titanium surface constitutes, described then titanium based titanium oxide nano-tube array material is through 450
°Behind the C high temperature sintering 3 hours, obtain having the TiO of anatase phase
2The nano-pipe array thin film material.
7. visible light-responded nano-tube array fuel cell according to claim 6 is characterized in that the described TiO that modifies through CdS
2The preparation method of nano-tube array film electrode adopts ultrasonic electro-deposition techniques to prepare, and its concrete preparation method is: with described TiO
2Nano-pipe array thin film is a negative electrode, and platinized platinum is an anode, is containing 0.05 M CdCl
2With apply bias voltage 0.44 V in the dimethyl sulfoxide solution of 0.1 M simple substance S, electro-deposition 10 minutes, it is ultrasonic that whole process adopts ultrasonic wave to continue.
8. visible light-responded nano-tube array fuel cell according to claim 6 is characterized in that described through Cu
2The TiO that O modifies
2The preparation method of nano-tube array film electrode prepares for adopting ultrasonic electro-deposition techniques, and its concrete preparation method is: with described TiO
2Nano-tube array film electrode is an anode, and Pt is to electrode, and Ag/AgCl is a reference electrode, in the electrolyte solution that contains sodium acetate 0.1 M, Schweinfurt green 0.02 M, applies bias voltage-0.25 V, and deposition process continues 5 minutes, and it is ultrasonic that whole process adopts ultrasonic wave to continue.
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103367759A (en) * | 2013-07-15 | 2013-10-23 | 上海交通大学 | Visible-light response type photocatalysis wastewater fuel cell, manufacture method thereof and application thereof |
| CN103762086A (en) * | 2014-02-13 | 2014-04-30 | 河海大学 | Dye-sensitized solar cell for recovering energy from sewage |
| CN103928690A (en) * | 2014-04-10 | 2014-07-16 | 华中科技大学 | Visible light photocatalytic fuel cell and preparation method thereof |
| CN104009123A (en) * | 2014-05-26 | 2014-08-27 | 上海交通大学 | Visible-light response type automatic-bias photoelectrical catalytic water decomposition hydrogen production and electricity generation system |
| CN104393309A (en) * | 2014-11-24 | 2015-03-04 | 哈尔滨工业大学 | Photocatalysis and microorganism composite anode fuel battery system |
| CN104638276A (en) * | 2014-12-03 | 2015-05-20 | 南京大学 | Photoelectrochemical battery and preparation method thereof |
| CN106169632A (en) * | 2016-06-22 | 2016-11-30 | 重庆大学 | Visible light photocatalysis fuel cell based on membrane electrode and preparation method thereof |
| CN109767921A (en) * | 2019-01-17 | 2019-05-17 | 辽宁大学 | A kind of photochemical cell and preparation method thereof and the application in circulation degradating organic dye |
| CN112759035A (en) * | 2021-01-11 | 2021-05-07 | 中国环境科学研究院 | Resource recovery mobile photoelectrochemical system in high-salinity wastewater |
| CN114804285A (en) * | 2022-05-23 | 2022-07-29 | 安徽农业大学 | Double-electrode mobile phase photocatalysis organic wastewater degradation device driven by sunlight |
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2011
- 2011-07-20 CN CN201110203146A patent/CN102306802A/en active Pending
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|---|---|---|---|---|
| CN103367759B (en) * | 2013-07-15 | 2015-04-22 | 上海交通大学 | Visible-light response type photocatalysis wastewater fuel cell, manufacture method thereof and application thereof |
| CN103367759A (en) * | 2013-07-15 | 2013-10-23 | 上海交通大学 | Visible-light response type photocatalysis wastewater fuel cell, manufacture method thereof and application thereof |
| CN103762086A (en) * | 2014-02-13 | 2014-04-30 | 河海大学 | Dye-sensitized solar cell for recovering energy from sewage |
| CN103928690A (en) * | 2014-04-10 | 2014-07-16 | 华中科技大学 | Visible light photocatalytic fuel cell and preparation method thereof |
| CN103928690B (en) * | 2014-04-10 | 2016-03-02 | 华中科技大学 | A kind of visible light photocatalysis fuel cell and preparation method thereof |
| CN104009123B (en) * | 2014-05-26 | 2017-01-04 | 上海交通大学 | Visible light-responded automatic bias photoelectrocatalysis decomposes Aquatic product hydrogen the system generated electricity |
| CN104009123A (en) * | 2014-05-26 | 2014-08-27 | 上海交通大学 | Visible-light response type automatic-bias photoelectrical catalytic water decomposition hydrogen production and electricity generation system |
| CN104393309A (en) * | 2014-11-24 | 2015-03-04 | 哈尔滨工业大学 | Photocatalysis and microorganism composite anode fuel battery system |
| CN104638276A (en) * | 2014-12-03 | 2015-05-20 | 南京大学 | Photoelectrochemical battery and preparation method thereof |
| CN106169632A (en) * | 2016-06-22 | 2016-11-30 | 重庆大学 | Visible light photocatalysis fuel cell based on membrane electrode and preparation method thereof |
| CN106169632B (en) * | 2016-06-22 | 2018-12-18 | 重庆大学 | Visible light photocatalysis fuel cell based on membrane electrode and preparation method thereof |
| CN109767921A (en) * | 2019-01-17 | 2019-05-17 | 辽宁大学 | A kind of photochemical cell and preparation method thereof and the application in circulation degradating organic dye |
| CN112759035A (en) * | 2021-01-11 | 2021-05-07 | 中国环境科学研究院 | Resource recovery mobile photoelectrochemical system in high-salinity wastewater |
| CN114804285A (en) * | 2022-05-23 | 2022-07-29 | 安徽农业大学 | Double-electrode mobile phase photocatalysis organic wastewater degradation device driven by sunlight |
| CN114804285B (en) * | 2022-05-23 | 2024-01-16 | 安徽农业大学 | Sunlight-driven double-electrode mobile phase photocatalytic organic wastewater degradation device |
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Application publication date: 20120104 |