CN101629300A - Method for separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis - Google Patents
Method for separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis Download PDFInfo
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- CN101629300A CN101629300A CN200910039641A CN200910039641A CN101629300A CN 101629300 A CN101629300 A CN 101629300A CN 200910039641 A CN200910039641 A CN 200910039641A CN 200910039641 A CN200910039641 A CN 200910039641A CN 101629300 A CN101629300 A CN 101629300A
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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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
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Abstract
The invention provides a method for separating and preparing hydrogen by decomposing water in a fuel cell through photocatalysis according to the inverse principle of the hydrogen fuel cell, aiming to avoiding the current separation problem of hydrogen and oxygen prepared by decomposing water through solar energy photocatalysis. The method adopts the inverse principle of the hydrogen fuel cell and uses photocatalyst as raw material for a photoanode, and platinum, nickel or carbon electrode as a cathode; an ion film is used between the two electrodes to transfer protons or hydroxyl ions, circuit is formed by connecting the photoanode and the cathode with a lead; sunlight or simulated sunlight is used as a light source, the light directly shines down upon the photoanode; and hydrogen is generated on the cathode and an oxidation reaction is performed on the anode so as to realize the aim of separating and preparing hydrogen by decomposing water through photocatalysis. In the method of the invention, no sacrifice agent or inhibitor is needed to add for adjusting the pH value of the electrolyte solution, an external power source can be added as additional bias so as to directly separate and prepare hydrogen by decomposing water through photocatalysis, and the separation problem of hydrogen and oxygen in practical technology development for decomposing water through solar energy photocatalysis is successfully solved.
Description
Technical field
The present invention relates to chemistry and photochemical catalysis subject and technical field of solar utilization technique, relate in particular to a kind of method of separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis.
Technical background
Fujishima had found optically catalytic TiO 2 water of decomposition effect in 1972, after this be mainly used in the research of hydrogen production by water decomposition aspect to photochemical catalysis at the beginning of the eighties, although on methods such as titanium dioxide/Pt microelectrode preparation, interpolation biomass, improve the hydrogen rate of producing, but, be not subjected to extensive concern because the productive rate of hydrogen is too low.Through the research in surplus 30 years, obtained progress at full speed with multiphase photocatalysis (heterogeneous photocatalysis) technology of conductor photocatalysis hydrogen production by water decomposition.Calendar year 2001 Zou Zhi just, leaf golden flower etc. is at Nature 2001,414 (6864): delivered the article that is entitled as Direct splitting of water under visible lightirradiation with an oxide semiconductor photocatalyst on the 625-627, reported the research of visible light catalyst aspect photo catalytic reduction hydrogen manufacturing, the solar energy photocatalytic hydrogen production by water decomposition obtains people's attention again.
The subject matter that solar energy photocatalytic hydrogen manufacturing is at present used is the difficult problem of separating of low hydrogen that makes with photodissociation water of photocatalysis efficiency and oxygen, wherein the hydrogen-oxygen separation is that the solar energy photocatalytic hydrogen production by water decomposition is used the subject matter that will solve, and the photocatalysis efficiency influence is the scale that solar hydrogen making is used.Under the situation that photocatalysis efficiency is low at present, solve separating of hydrogen that photodissociation water makes and oxygen effectively, can be with this technology and the integrated exploitation light of nickel metal hydride battery rechargeable battery, has the potential application market at aspects such as portable type electronic product, military communication equipment, toy cars, thereby the utilization that is sun power is opened up the effective way that solar energy-chemical energy utilizes except photovoltaic, photo-thermal.
Aspect the hydrogen and oxygen separation that makes in photochemical catalyzing, mainly be to adopt chemical reagent at present such as I
-/ I
2And Fe
2+/ Fe
3+Suppress the generation of oxygen and hydrogen respectively as sacrifice agent, this method is not had a practicality.The pH value such as the positive column that also have simultaneously employing to regulate positive column and cathodic area are that NaOH solution, cathodic area are H
2SO
4The method of solution generates O in positive column and cathodic area respectively
2And H
2This method is also restricted when practicality.
Summary of the invention
The present invention is directed to the difficult problem of separating of hydrogen that present solar energy photocatalytic water of decomposition makes and oxygen, a kind of photochemical catalysis fuel cell (Photocatalyitc Fuel Cell that adopts the hydrogen fuel cell inverse principle has been proposed, PFC) method of the direct separating and preparing hydrogen of technology water of decomposition is researched and solved the hydrogen and the oxygen separation difficult problem of the technological development of sun power photodissociation water practicability.
For chemical reaction: aA+bB=cC+dD
Gibbs free energy is: Δ G=Δ G
0-RTln K, K are the equilibrium constant
Cell voltage under the situation of not considering kinetics of electrode process
In theory, the redox chemistry reaction of most of Δ G＜0 can be used for designing fuel cell, for photodissociation water, because extraneous luminous energy enters reaction system, water decomposition can be subjected to carry out under the optical excitation on the semi-conductor of band-gap energy greater than 1.23eV in theory, become spontaneous reaction (Δ G＜0), and confirmed by practice, therefore on principle, can be used for designing the photochemical catalysis fuel cell fully.Because redox reaction is independently carried out on the electrode at two respectively, therefore can realize separating of photodissociation aquatic products thing oxygen and hydrogen.
The present invention adopts photochemical catalysis fuel cell (PFC) technology of the inverse principle of hydrogen fuel cell to solve the hydrogen that photodissociation water makes and the separation problem of oxygen, and its principle and structural representation are respectively as attached illustrated in figures 1 and 2.Among attached Fig. 1 and 2, light anode (anode) is with the photocatalyst such as the TiO of burst of ultraviolel
2The perhaps photocatalyst of excited by visible light such as InVO
4, MBi
2O
4(M=Mg, Ca, Sr, Ba), Bi
2WO
6Be raw material, described smooth anodic preparation method adopts the powder coating method; Negative electrode (cathode) is platinum (Pt) electrode or carbon, nickel electrode.Two electrodes are immersed in the electrolyte solution, the inorganic salt electrolyte solution of described electrolyte solution prior art.Separate with ionic membrane (cationic exchange membrane Proton Exchange Membrane/ anion-exchange membrane Anion Exchange Membrane) between two electrodes, light anode and negative electrode are connected to form circuit with lead.Electrode can not add by biasing yet, and biased mode has and directly adds external direct current power supply, drying battery, dye sensitization solar battery, various fuel cell power source.As light source, light directly impinges upon on the light anode with sunlight or solar simulated; Adopt drainage, or the direct collecting method of airbag is collected the gas oxygen of positive column and the gas hydrogen in cathodic area.
Photochemical catalysis fuel cell of the present invention is as the light anode material with photocatalyst, with Pt, carbon, nickel electrode is negative electrode, its similar is in the chemical reaction equipment of hydrogen fuel cell, because luminous energy enters reaction system, water decomposition hydrogen manufacturing can be carried out in the photochemical catalysis fuel cell, is the converse process of hydrogen fuel cell principle.Because water decomposition is carried out liberation of hydrogen and oxygen evolution reaction respectively on two isolating electrodes of photochemical catalysis fuel cell, and two reactions are carried out in two enclosed spaces that separated by the proton film respectively, generate hydrogen and oxygen respectively, therefore, PFC technology water of decomposition is separating and preparing hydrogen directly.
Described photocatalyst is that the photocatalyst of burst of ultraviolel comprises TiO by the photocatalyst of burst of ultraviolel or the photocatalyst of excited by visible light
2Deng, the photocatalyst of excited by visible light comprises SrBi
2O
4Or InVO
4InVO
4, Mg Bi
2O
4, Ca Bi
2O
4, SrBi
2O
4, Ba Bi
2O
4, Bi
2WO
6Deng.
The reaction of the direct separating and preparing hydrogen photochemical catalysis of water of decomposition fuel cell electrode is as follows:
The cationic exchange film system
anode：H
2O+h
+→O
2+H
+
cathode：H
++e→H
2
The anionresin film system
anode：OH
-+h
+→O
2+H
2O
cathode：H
2O+e→H
2+OH
-
Technique effect of the present invention is: do not needing to add sacrifice agent or inhibitor, adjusting electrolyte solution pH value, can add external source and do under the situation of additional bias, make directly separating and preparing hydrogen of photochemical catalyzing, successfully solve the hydrogen and the oxygen separation difficult problem of solar energy photocatalytic water of decomposition practicability technological development.
Description of drawings
Fig. 1 is the separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis principle schematic, (a) is the cationic exchange film system, (b) is the anionresin film system;
Fig. 2 is a photochemical catalysis fuel cell water of decomposition separating and preparing hydrogen apparatus structure synoptic diagram, (a) is the proton film system, (b) is the anionresin film system;
Fig. 3 is the gas gas-chromatography qualitative analysis figure that the embodiment negative electrode is collected
Embodiment
The assembling of separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis device mainly divides two portions: first part is light anode, negative electrode, the preparation of electrolyte solution and the pre-treatment of proton film of PFC; Second section is according to accompanying drawing 2 assemblings and collects cathodic area gas and carry out qualitative analysis.
1, light anodic preparation
Make 3g by oneself visible light catalyst (as: InVO
4, MBi
2O
4(M=Mg, Ca, Sr, Ba), Bi
2WO
6) put into mortar, add the ethanol solution of 1ml 10% methyl ethyl diketone again, grind 30min; Add 4.5ml water afterwards, the mixing solutions of 0.1mlTriton X-100 and 30%wt (0.9g) polyoxyethylene glycol (molecular weight 20000) grinds 30min, adjusts suitable concn, adopts coating process, draws two-layer TiO
2Preparation visible light catalytic agent film on the FTO glass conducting surface of film.Vertically be attached to FTO conductive glass (6 * 8cm) both sides of membrane with scotch tape (about 40 μ m are thick), add a certain amount of visible light catalyst slurry by method preparation noted earlier, with glass stick roller coating film forming, equidirectional one-pass film-forming effect is best, and film size is about 5 * 6cm
2Membrane electrode is positioned in the retort furnace, 600 ℃ of following thermal treatment one hour, naturally cool to 80 ℃ standby.
2, the preparation of negative electrode
The self-control platinized platinum (20mm * 20mm).Carbon or nickel electrode also can be used.
3, the preparation of electrolyte solution
Concentration is the Na of 0.01-1mol/L
2SO
4Solution.
4, the pre-treatment of proton film
Under 70 ℃, with the H of lower concentration
2O
2Solution-treated proton film 3h;
Then under 70 ℃, with the H of lower concentration
2SO
4Solution is handled proton film 3h again;
Clean with distilled water at last and be soaked in the distilled water standby.
5, assembling and collection cathodic area gas carry out gas chromatographic detection
Assemble the photochemical catalysis fuel cells and adopt drainage to collect the gas in cathodic area according to accompanying drawing 2; Adopt the GC9800 of Shanghai Kechuang Chromatograph Instruments Co., Ltd. type gas chromatograph to carry out off-line analysis to collecting gas, (3mm * 3m), He is carrier gas to the TDX-01 chromatographic column, and TCD detects.The gas that the employing drainage is collected has apparent in view hydrogen peak through the gas chromatographic detection result as shown in Figure 3 about 1.5min.Because the selective permeation effect of proton film, this result shows has hydrogen to produce in the cathodic area.
Embodiment 2
1, light anodic preparation
Make 3g by oneself TiO
2Nano material is put into mortar, adds the ethanol solution of 1ml 10% methyl ethyl diketone again, grinds 30min; Add 4.5ml water afterwards, the mixing solutions of 0.1mlTriton X-100 and 30%wt (0.9g) polyoxyethylene glycol (molecular weight 20000) grinds 30min, adjusts suitable concn, adopts coating process, draws two-layer TiO
2Prepare TiO on the FTO glass conducting surface of film
2Film.(6 * 8cm) both sides add a certain amount of TiO by method preparation noted earlier vertically to be attached to the FTO conductive glass of membrane with scotch tape (about 40 μ m are thick)
2Slurry, with glass stick roller coating film forming, equidirectional one-pass film-forming effect is best, and film size is about 5 * 6cm
2Membrane electrode is positioned in the retort furnace, 500 ℃ of following thermal treatment one hour, naturally cool to 80 ℃ standby.
2, the preparation of negative electrode
The self-control platinized platinum (20mm * 20mm).
3, the preparation of electrolyte solution
Concentration is the NaNO of 0.1mol/L
3Solution
4, the pre-treatment of Nafion117 proton film
Under 70 ℃, the H with 5%
2O
2Solution-treated Nafion117 proton film 3h;
Then under 70 ℃, the H with 10%
2SO
4Solution is handled Nafion117 proton film 3h again;
Clean with distilled water at last and be soaked in the distilled water standby.
5, assembling and collection cathodic area gas carry out gas chromatographic detection
According to accompanying drawing 2 assembling photochemical catalysis fuel cells, add under the 0.2V bias voltage at external direct current power supply, collect the gas in cathodic area with the gas sampling bag; Adopt the GC9800 of Shanghai Kechuang Chromatograph Instruments Co., Ltd. type gas chromatograph to carry out off-line analysis to collecting gas, (3mm * 3m), He is carrier gas to the TDX-01 chromatographic column, and TCD detects.The gas that the employing drainage is collected has apparent in view hydrogen peak through the gas chromatographic detection result as shown in Figure 3 about 1.5min.Because the selective permeation effect of proton film, this result shows has hydrogen to produce in the cathodic area.
Embodiment 3
1, light anodic preparation
Make 3g by oneself TiO
2Nano material is put into mortar, adds the ethanol solution of 1ml 10% methyl ethyl diketone again, grinds 30min; Add 4.5ml water afterwards, the mixing solutions of 0.1mlTriton X-100 and 30%wt (0.9g) polyoxyethylene glycol (molecular weight 20000) grinds 30min, adjusts suitable concn, adopts coating process, draws two-layer TiO
2Prepare TiO on the FTO glass conducting surface of film
2Film.(6 * 8cm) both sides add a certain amount of TiO by method preparation noted earlier vertically to be attached to the FTO conductive glass of membrane with scotch tape (about 40 μ m are thick)
2Slurry, with glass stick roller coating film forming, equidirectional one-pass film-forming effect is best, and film size is about 5 * 6cm
2Membrane electrode is positioned in the retort furnace, 500 ℃ of following thermal treatment one hour, naturally cool to 80 ℃ standby.
2, the preparation of negative electrode
The self-control platinized platinum (20mm * 20mm).
3, the preparation of electrolyte solution
0.01-1mol/L NaOH solution
4, the pre-treatment of anion-exchange membrane
Under 50 ℃, with the H of lower concentration
2O
2Solution-treated proton film 3h;
Under 50 ℃, handle proton film 3h more then with the NaOH solution of lower concentration;
Clean with distilled water at last and be soaked in the distilled water standby.
5, assembling and collection cathodic area gas carry out gas chromatographic detection
According to accompanying drawing 2 assembling photochemical catalysis fuel cells, add under the 0.2V bias voltage at external direct current power supply, collect the gas in cathodic area with the gas sampling bag; Adopt the GC9800 of Shanghai Kechuang Chromatograph Instruments Co., Ltd. type gas chromatograph to carry out off-line analysis to collecting gas, (3mm * 3m), He is carrier gas to the TDX-01 chromatographic column, and TCD detects.The gas that the employing drainage is collected has apparent in view hydrogen peak through the gas chromatographic detection result as shown in Figure 3 about 1.5min.Because the selective permeation effect of proton film, this result shows has hydrogen to produce in the cathodic area.
Claims (6)
1, a kind of method of separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis is characterized in that: adopt the inverse principle of hydrogen fuel cell, the light anode is raw material with the photocatalyst, and negative electrode is platinum or nickel or carbon dioxide process carbon electrode; Adopt ionic membrane to transmit proton or hydroxide ion between two electrodes, light anode and negative electrode are connected to form circuit with lead; As light source, light directly impinges upon on the light anode with sunlight or solar simulated; Produce hydrogen at negative electrode,, realize the separating and preparing hydrogen purpose of photodissociation water in anode generation oxidizing reaction.
2, the method for the described separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis of claim 1 is characterized in that: described photocatalyst is that negative electrode is platinum or carbon or nickel electrode by the photocatalyst of burst of ultraviolel or the photocatalyst of excited by visible light.
3, the method for the described separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis of claim 2 is characterized in that: the photocatalyst of described burst of ultraviolel is TiO
2
4, the method for the described separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis of claim 2 is characterized in that: the photocatalyst of described excited by visible light is SrBi
2O
4Or InVO
4, InVO
4, Mg Bi
2O
4, Ca Bi
2O
4, Sr Bi
2O
4, Ba Bi
2O
4, Bi
2WO
6
5, the method for the separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis described in the claim 1 is characterized in that: described two electrodes are immersed in the electrolyte solution, separate with ionic membrane between two electrodes.
6, the method for the described separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis of claim 1, it is characterized in that: described electrode biasing, biased mode is for directly adding external direct current power supply or drying battery, dye sensitization solar battery, various fuel cell.
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