CN1900366A - Ion diaphragm photoelectrolytic cell using solar energy directly decomposing water to make hydrogen - Google Patents

Ion diaphragm photoelectrolytic cell using solar energy directly decomposing water to make hydrogen Download PDF

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CN1900366A
CN1900366A CNA2006100201311A CN200610020131A CN1900366A CN 1900366 A CN1900366 A CN 1900366A CN A2006100201311 A CNA2006100201311 A CN A2006100201311A CN 200610020131 A CN200610020131 A CN 200610020131A CN 1900366 A CN1900366 A CN 1900366A
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chamber
acid
alkali
cathode
cell structure
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闫康平
周菊枚
鲁厚芳
王伟
田间
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Sichuan University
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Sichuan University
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Abstract

本发明是一种用于光电化学反应的离子隔膜光电解池结构，实现了无偏压直接光解水，该发明属于光电化学技术领域。该光电池结构包括：用全氟羧酸/磺酸复合离子膜将容器分为两个室，一个室盛酸溶液，为“酸室”，一个室盛碱溶液，为“碱室”。半导体光电材料固定在导电玻璃上作为光阳极，放入碱室。将一种析氢过电压低的惰性阴极材料放入酸室作为阴极。光电解池工作时将阳极和阴极短接，光从碱室侧射入到光阳极上，在阴极产生氢气。本发明的光电解池结构简单，利用电极电位随电解液pH值改变而改变，将阴极和阳极分别放入不同pH的酸和碱液中，提高了二者电位差，实现无偏压直接光解水。The invention relates to an ion-diaphragm photoelectrolytic cell structure for photoelectrochemical reactions, which realizes direct photolysis of water without bias, and belongs to the technical field of photoelectrochemistry. The photovoltaic cell structure includes: the container is divided into two chambers by a perfluorocarboxylic acid/sulfonic acid composite ion membrane, one chamber holds an acid solution and is called an "acid chamber", and the other chamber holds an alkali solution and is called an "alkali chamber". The semiconductor optoelectronic material is fixed on the conductive glass as a photoanode and placed in the alkali chamber. Put an inert cathode material with low hydrogen evolution overvoltage into the acid chamber as the cathode. When the photoelectrolytic cell is working, the anode and the cathode are short-circuited, light is incident on the photoanode from the side of the alkali chamber, and hydrogen gas is generated at the cathode. The structure of the photoelectrolytic cell of the present invention is simple, and the cathode and the anode are respectively put into acid and lye of different pH by using the change of the electrode potential with the change of the pH value of the electrolyte, so as to increase the potential difference between the two, and realize direct photoelectricity without bias. Dehydration.

Description

Utilize the ion diaphragm photoelectrolytic cell of the direct hydrogen production by water decomposition of sun power
One, technical field
The present invention relates to a kind of ion diaphragm photoelectrolytic cell structure that is used for the photoelectrochemistry reaction, this invention belongs to photoelectrochemistry
Technical field.
Two, background technology
Fujishima in 1972 and Honda publish an article at nature first, have described semi-conductor TiO 2The electrochemical cell that electrode is formed, it is converted into luminous energy by the method for photoelectrolysis water the chemical energy of hydrogen and oxygen.This photoelectrocatalysis hydrogen production by water decomposition utilizes sun power and water to make hydrogen, does not have byproduct, and is pollution-free.Compare with photocatalysis hydrogen production in addition, reduced the compound of electron-hole pair, make the separation efficiency of electron-hole pair improve, can on the two poles of the earth, obtain hydrogen and oxygen respectively.
But generally speaking, the light anode material can not provide the voltage of enough water of decomposition, need add a bias voltage in addition, the method that applies bias voltage mainly contains (1) external power and applies that bias voltage, (2) utilize optical device to apply internal bias voltage, (3) utilize the inside that do not coexist of negative and positive the two poles of the earth concentration that the concentration difference bias voltage is provided.Therefore the structure of photoelectrochemical cell also mainly contains single pool structure, laminated structure and two pool structure.
Laminated structure gathers into folds the semiconductor layer of different band gap, is placed on the upper strata than the material of broad-band gap, absorbs the photon of shorter wavelength, and energy can pass less than the photon of band gap and be absorbed by the bottom semi-conductor.Improved the specific absorption of light like this, also improved the total voltage of solar cell, can reach more than the 2.0V, but the electrode materials of studying suitable this structure at present there is very strong light dissolubility.Two pool structures can add different electrolytic solution respectively at the anode chamber and the cathode chamber, utilize electrode that different redox couple current potentials is arranged in different electrolytes, and its potential difference is as bias voltage.
What two pool structures were more is that the centre is divided into two compartments with dividing plate with container.Fujishima mentions what use between two compartments in " Electrochemicalphotolysis of water at a semiconductor electrode " literary composition be porous barrier.The two-spacer photolytic cell of describing for Chinese patent 89-1036994 number is fixed on the composite spacer with the semiconductor light partition, is bonded on the wall of container again.O.N.Srivastava etc. are with semi-conductor TiO in " Semiconductor-septum photo-electrochemical cellfor solar hydrogen production " literary composition 2Be fixed on the Ti plate, with TiO 2/ Ti plate separates.This separating with dividing plate is unfavorable for the solution conducting, increased the volts lost of electrolytic solution; Poor sealing; Dividing plate does not have selectivity to the infiltration of solution, can cause the neutralization of soda acid.
Three, summary of the invention
The present invention has designed a kind of perfluorocarboxylic acid/sulfonic acid composite ionic membrane photoelectrochemistrpool pool that does not apply bias voltage, has solved problems such as solution conductivity, pressure drop and acid-base neutralisation.This structure comprises:
(1) with perfluorocarboxylic acid/sulfonic acid composite ionic membrane container is divided into two chambers, acid solution is contained in a chamber, is called " sour chamber ", and alkaline solution is contained in a chamber, is called " alkali chamber ".
(2) photoelectric semiconductor material is fixed on the conductive glass,, puts into the alkali chamber of (1) as the light anode.
(3) sunlight is injected on the light anode from alkali chamber side.
(4) the low inert cathode material of a kind of liberation of hydrogen superpotential is put into sour chamber, as the negative electrode of liberation of hydrogen.
(5) with light anode and negative electrode lead short circuit.
Perfluorocarboxylic acid/sulfonic acid composite ionic membrane is because R f-COOH exists, and can stop OH -Ion is moved back to the original place of residence and is moved, and has slowed down acid-base neutralisation effectively, and its membrane resistance is lower in addition, good endurance.Can keep two electrolyte phs in the chamber that bigger difference is arranged so for a long time, then the potential difference of anode and cathode also can remain on maximum.Conductive glass has good light transmittance and low face resistance.Therefore photoelectric semiconductor material is fixed thereon, the two is in conjunction with getting well, and light anodic resistance is less.The electronics that photoelectric semiconductor material is inspired by illumination just can pass on the negative electrode by conductive glass and external circuit well.Oxidizing reaction takes place on anode, in negative electrode generation reduction reaction.Need not bias voltage just can photolysis water.
The present invention has the following advantages:
(1) photoelectrolytic cell need not to apply bias voltage,
(2) utilize the direct water of decomposition of sunlight,
(3) negative electrode prepares hydrogen, anode preparation oxygen,
(4) equipment is simple, easy to prepare,
(5) electrolysis need not other sacrifice agent, and other side reaction does not take place.
Four, embodiment
Below by embodiment the present invention is specifically described; be necessary to be pointed out that at this present embodiment only is used for the present invention is further specified; can not be interpreted as limiting the scope of the invention, the person skilled in the art in this field can make some nonessential improvement and adjustment according to the content of the invention described above.
Embodiment 1:
1, the semiconductor optoelectronic anode material adopts the good TiO of fast light burn into chemical stability 2Adopt sol/gel+powder method with TiO 2Be fixed on conductive glass surface.
TiO 2The colloidal sol preparation flow: distilled water adds an amount of concentrated nitric acid, is heated to 70 ℃ with water bath with thermostatic control.Get 1: 3 Virahol: after butyl (tetra) titanate solution mixes, slowly be added drop-wise in the homothermic distilled water and stirring, continuation constant temperature stirs 2h, makes to contain TiO 2TiO for 27g/L 2Colloidal sol, sealing is preserved.Flow process is seen accompanying drawing 1.
TiO 2Pulp preparation flow process: get an amount of TiO 2Colloidal sol adds nano-TiO 2Powder (nano-TiO 2Powder is pressed TiO in the slip 2Total amount is that 120g/L calculates adding), grinding, ultrasonic dispersing make TiO 2Slurry.
TiO 2Coating preparation flow process: with TiO 2Slurry evenly is coated on the conducting surface of clean ITO conductive glass, puts into 450 ℃ of sintering 30min of High Temperature Furnaces Heating Apparatus, naturally cooling.Repeat above operation repeatedly, prepare TiO 2/ ito thin film electrode.
2, test TiO 2The relation of/ito thin film electropotential and electrolyte ph.Initial electrolysis liquid pH value adjusts to 1, regulates the pH value with the 4mol/L KOH aqueous solution.As reference electrode, treat the stable back of electropotential reading (being converted into hydrogen mark electropotential) with saturated calomel electrode, gained the results are shown in Figure 2.
Fig. 2 as seen, TiO 2/ ito thin film electropotential is the same as pH increases and negative moving with hydrogen electrode.Current potential is negative more, and is favourable more to making the light anode, so TiO 2/ ito thin film electrode is put into the alkali chamber.
3, used ionic membrane is perfluorocarboxylic acid/sulfonic acid composite ionic membrane.
4, perfluorocarboxylic acid/sulfonic acid composite ionic membrane is sealed in the middle of two blocks of " U " shape plates, and is divided into two chambers with the thin plate envelope.One of them contains acid solution as " sour chamber ", and another one is contained alkaline solution as " alkali chamber ".The photoelectrolytic cell structure is seen Fig. 3.
5, with TiO 2/ ito thin film electrode is put into the alkali chamber of containing alkaline solution (the KOH solution of 1mol/L), as the light anode.
6, the liberation of hydrogen superpotential is low inert cathode material (platinum) is put into the Sheng acid solution (H of 1mol/L 2SO 4Solution) sour chamber is as the negative electrode of liberation of hydrogen.
7, sunlight shines TiO from alkali chamber one side 2/ ITO photoanode surface.
8, with lead above-mentioned smooth anode and negative electrode are connect, form electron channel.
9, with the direct water of decomposition of photoelectrolytic cell of said structure, adopt the exhaust gas collection method to collect hydrogen, obtain the result and list table 1 (fix for making each test light intensity, sunlight is simulated with the xenon lamp of 350W) at negative electrode.
Embodiment 2: condition is with embodiment 1, and light source is urban district, the Chengdu sunlight at high noon in June.
Comparative example 1: negative electrode and anode are with embodiment 1, and single-chamber photoelectric Xie Chi, solution are the KOH solution of 1mol/L; Illumination is the xenon lamp of 350W, apart from TiO 2Plate is 70mm.Adopt the exhaust gas collection method to collect hydrogen, obtain the result and list table 1 at negative electrode.
Comparative example 2: negative electrode and anode are with embodiment 1, and single-chamber photoelectric Xie Chi, solution are the KOH solution of 1mol/L; Add the bias voltage of 0.6V.Illumination is the xenon lamp of 350W, apart from TiO 2Plate is 70mm.Adopt the exhaust gas collection method to collect hydrogen, obtain the result and list table 1 at negative electrode.
The liberation of hydrogen of table 1 ion diaphragm photoelectrolytic cell of the present invention and single-chamber photoelectric Xie Chi relatively
Figure A20061002013100071
Table 1 as seen, single-chamber photoelectric Xie Chi is when no-bias, the negative electrode no hydrogen produces.And the ion diaphragm photoelectrolytic cell can make hydrogen by direct water of decomposition under no-bias.And along with light anode TiO 2Area increase, hydrogen output increases.At comparative example 2, the 0.6V bias voltage produces hydrogen 2.0Lm down -2H -1, embodiment 1, and no-bias produces hydrogen 3.34Lm -2H -1, bigger than comparative example 2 amounts.The light anode that area is identical is described, the cell voltage of ion diaphragm photoelectrolytic cell is far above the cell voltage of single-chamber photoelectric Xie Chi.
Description of drawings of the present invention:
Fig. 1 sol/gel+powder method schema.
Fig. 2 TiO 2The relation of/ito thin film electropotential and electrolyte ph.
Fig. 3 ion diaphragm photoelectrochemistrpool pool synoptic diagram.

Claims (8)

1.一种用于光电化学反应的离子隔膜光电解池结构，该结构包括：1. A kind of ion diaphragm photoelectrolytic cell structure for photoelectrochemical reaction, this structure comprises: (1)用全氟羧酸/磺酸复合离子膜将容器分为两个室，一个室盛酸溶液，为“酸室”，一个室盛碱溶液，为“碱室”。(1) The container is divided into two chambers with perfluorocarboxylic acid/sulfonic acid composite ionic membrane, one chamber holds acid solution, which is called "acid chamber", and the other chamber holds alkali solution, which is called "alkali chamber". (2)将半导体光电材料固定在导电玻璃上，作为光阳极，放入(1)中的碱室。(2) Fix the semiconductor optoelectronic material on the conductive glass as a photoanode and put it into the alkali chamber in (1). (3)将一种析氢过电压低的惰性阴极材料放入(1)中的酸室。(3) Put an inert cathode material with low hydrogen evolution overvoltage into the acid chamber in (1). (4)将(2)、(3)的光阳极和阴极短接。(4) Short-circuit the photoanode and cathode of (2) and (3). (5)光从碱室侧射入到光阳极上。(5) Light is incident on the photoanode from the alkali chamber side. 2.按权利要求1所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：将容器分为了两个室。一个室装酸溶液，一个室装碱溶液，保证二者pH值之间足够大，并且导电性好。2. A kind of ion diaphragm photoelectrolytic cell structure for photoelectrochemical reaction according to claim 1, characterized in that: the container is divided into two chambers. One chamber is filled with acid solution, and the other chamber is filled with alkali solution to ensure that the pH value between the two is large enough and the conductivity is good. 3.按权利要求1所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：步骤(1)中所述全氟羧酸/磺酸复合离子膜能阻挡OH-离子迁移到酸室，防止酸碱的中和，至少能大大减缓，且有较低的膜电阻和耐久性。3. a kind of ion membrane photoelectrolytic cell structure for photoelectrochemical reaction according to claim 1, is characterized in that: perfluorocarboxylic acid/sulfonic acid composite ion membrane described in step (1) can block OH - ion Migrating to the acid chamber, preventing the neutralization of acid and alkali, can at least be greatly slowed down, and has lower membrane resistance and durability. 4.按权利要求1所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：步骤(2)中所述半导体光电材料固定在导电玻璃的导电面，固定方法可以是溶胶凝胶涂敷法或其它。4. a kind of ion membrane photoelectrolytic cell structure for photoelectrochemical reaction by claim 1, is characterized in that: semiconductor photoelectric material described in the step (2) is fixed on the conductive surface of conductive glass, and fixing method can be Sol gel coating method or other. 5.按权利要求1所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：步骤(2)中所述半导体光电材料能耐碱，耐光腐蚀，与导电玻璃之间的结合性好，在碱中不会脱落。5. a kind of ionic membrane photoelectrolytic cell structure for photoelectrochemical reaction according to claim 1, is characterized in that: the semiconductor photoelectric material energy alkali resistance described in the step (2), photocorrosion resistance, and the gap between the conductive glass Good combination, will not fall off in alkali. 6.按权利要求1所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：步骤(2)中所述光阳极可以是独立活动的，插入到碱室中，也可以是直接将固定有半导体光电材料的导电玻璃粘在容器壁上，有半导体光电材料一面朝向溶液。6. A kind of ion membrane photoelectrolytic cell structure for photoelectrochemical reaction according to claim 1, characterized in that: the photoanode described in the step (2) can be independently movable, inserted in the alkali chamber, also It may be that the conductive glass fixed with the semiconductor optoelectronic material is directly glued to the container wall, and the side with the semiconductor optoelectronic material faces the solution. 7.按权利要求1所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：用于光分解水时，步骤(3)中所述惰性阴极材料具有低析氢过电位，可以是Pt，NiOx等。7. A kind of ion membrane photoelectrolyte cell structure for photoelectrochemical reaction according to claim 1, characterized in that: when used for photolysis of water, the inert cathode material described in step (3) has a low hydrogen evolution overpotential , can be Pt, NiOx, etc. 8.按权利要求1、2、3、4、5、6、7所述的一种用于光电化学反应的离子隔膜光电解池结构，其特征在于：按步骤(4)中所述将(2)、(3)的阳极和阴极短接，按步骤(5)中所述光从碱室侧射入到光阳极上后，阳极和阴极之间电位差较单室电池升高。无需外加电源，即可分解水。8. according to claim 1, 2, 3, 4, 5, 6, 7 described a kind of ionic membrane photoelectrolytic cell structure for photoelectrochemical reaction, it is characterized in that: by described in step (4) will ( 2), the anode and the cathode of (3) are short-circuited, and after the light is incident on the photoanode from the side of the alkali chamber according to the step (5), the potential difference between the anode and the cathode is higher than that of the single-chamber battery. Water can be decomposed without external power supply.
CNA2006100201311A 2006-01-10 2006-01-10 Ion diaphragm photoelectrolytic cell using solar energy directly decomposing water to make hydrogen Pending CN1900366A (en)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101608316B (en) * 2009-07-27 2011-09-07 新奥科技发展有限公司 Device for producing hydrogen through decomposing water
CN101629300B (en) * 2009-05-21 2012-01-18 中国科学院广州能源研究所 Method for separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis
CN102482789A (en) * 2009-09-09 2012-05-30 三井化学株式会社 Gas generator and method for generating gas
CN107740133A (en) * 2017-10-19 2018-02-27 杭州泰博科技有限公司 The devices and methods therefor of photocatalysis cathode electrode hydrogen production by water decomposition gas
CN113529115A (en) * 2020-04-16 2021-10-22 中国科学院大连化学物理研究所 A dual-cell high-voltage electrochemical reaction device

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101629300B (en) * 2009-05-21 2012-01-18 中国科学院广州能源研究所 Method for separating and preparing hydrogen by decomposing water in fuel cell through photocatalysis
CN101608316B (en) * 2009-07-27 2011-09-07 新奥科技发展有限公司 Device for producing hydrogen through decomposing water
CN102482789A (en) * 2009-09-09 2012-05-30 三井化学株式会社 Gas generator and method for generating gas
CN102482789B (en) * 2009-09-09 2014-10-01 三井化学株式会社 Gas generator and method for generating gas
CN107740133A (en) * 2017-10-19 2018-02-27 杭州泰博科技有限公司 The devices and methods therefor of photocatalysis cathode electrode hydrogen production by water decomposition gas
CN113529115A (en) * 2020-04-16 2021-10-22 中国科学院大连化学物理研究所 A dual-cell high-voltage electrochemical reaction device
CN113529115B (en) * 2020-04-16 2022-09-16 中国科学院大连化学物理研究所 Double-cell high-voltage electrochemical reaction device

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