CN102280675A - Selfbias photoelectrochemical cell for hydrogen production with solar energy - Google Patents
Selfbias photoelectrochemical cell for hydrogen production with solar energy Download PDFInfo
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Abstract
The invention which discloses a selfbias photoelectrochemical cell for hydrogen production with solar energy and relates to the selfbias photoelectrochemical cell which comprises semiconductor photoelectrodes and can truly realize the conversion of solar energy-electric energy-chemical energy belongs to the field of clean and renewable new energy utilization and new material preparation. The selfbias photoelectrochemical cell for the hydrogen production with the solar energy comprises a photoanode with the photoelectric response capability, a photocathode with the photoelectric response capability, an electrolyte and an external circuit, and the connection relation is that: parts of the photoanode and the photocathode are immersed in the electrolyte, and exposed parts of the photoanode and the photocathode are connected by the external circuit. A work process of the cell of the invention is that: when sunlight irradiates the cell, an electric potential difference which is generated between the photoanode and the photocathode allows a photogenerated current to be generated in a case that the external circuit is connected. The photoelectrochemical cell, which allows energy conversion to be successfully realized by completely depending on the solar energy in the invention, and has the advantages of simple structure, cost saving, and easy scale production, has good application prospects.
Description
Technical field
The present invention relates to a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making, especially relate to the automatic bias photoelectrochemical cell that a kind of semiconductor photoelectrode that can realize really that solar-electrical energy-chemical energy (hydrogen, oxygen) transforms is formed, belong to renewable utilization of new energy resources of cleaning and field of new material preparation.
Background technology
The ultimate challenge of mankind nowadays social development----energy crisis and environmental pollution.Through twice industrial revolution in 19th century and 20th century, the mankind have entered advanced industry and culturally advanced modern society.Yet industrial society develops a large amount of consumption that also caused the energy rapidly.It is estimated, the energy system that the world today relies on, just fossil energy (comprising coal, oil, natural gas) only can be kept only century-old.And along with the continuous rareness of the energy, exploitation difficulty of new forms of energy and cost also increase greatly, institute's consumed energy even can approach or surmount the energy energy that is obtained.Moreover the burning fossil energy causes a large amount of carbon emissions and other harmful substances, air pollution, and global warming has badly influenced human own inhabitation and life.
Unique solution route utilizes the renewable new forms of energy of cleaning exactly.Hydrogen Energy is considered to the alternative energy source of most possible development of future generation, and it contains can be high, and be convenient for carrying and use, and pollution-free, zero carbon emission.Along with the development of technology, except the traditional large-scale application in industrial production, hydrogen also more and more has been applied in such as people's livelihood fields such as fuel cell, hydrogen energy source automobiles.Yet present 96% Hydrogen Energy in the world derives from the consumption of non-regenerative resources such as natural gas, oil equally and transforms, and produces by the steam methane transformation technology such as the annual hydrogen output 95% of the present U.S..Water is composed of hydrogen and oxygen, hydrogen content is abundant, and water is bulky on earth, make hydrogen and oxygen is a kind of desirable approach by brine electrolysis, yet global at present only 3.9% hydrogen is to be obtained by water electrolysis, and the prior art power consumption is huge, and required electric energy is produced by fossil energy equally, and development potentiality is limited.So utilize clean reproducible energies such as solar energy, wind energy, from the water that earth content enriches, obtain the preferred approach that electric energy or Hydrogen Energy are considered to sustainable development from now on, also become one of focus of current science industrial quarters research.
Photoelectrochemical cell (PEC) promptly is the device that utilizes the hydrogen manufacturing of sunlight electrolysis water.Photoelectrochemical cell is generally by optoelectronic pole, form electrode and electrolyte.Utilization has the semiconductor of photocatalytic activity and does optoelectronic pole, it is right to produce light induced electron-hole under rayed, produces photogenerated current and photovoltage then, makes hydrone that redox reaction take place on positive and negative electrode respectively, make hydrogen and oxygen, finish solar energy-chemical transformation of energy.The semi-conducting material that is fit to do optoelectronic pole must satisfy several necessary conditions simultaneously: suitable can be with position, carrier mobility that chemical stability is good and enough.Yet most of semiconductor can not satisfy above several conditions simultaneously.Therefore, up to the present, most of research has concentrated on the n N-type semiconductor N light anode, comprises TiO
2, SrTiO
3, ZnO, Fe
2O
3Deng.Do the light anode with these n N-type semiconductor Ns, negative electrode is then generally selected noble metal electrode for use, as platinum electrode.
Yet, because the reduction potential of hydrogen is mostly approached in the conduction band position of n N-type semiconductor N, utilize this n type unijunction photoelectrochemical cell to come photolysis water hydrogen under applied voltage, just can carry out, this just makes it become a kind of is not truly solar hydrogen making device, has reduced its attraction yet.An optimal approach that addresses this problem is to adopt a kind of new-type battery structure, and anode and negative electrode all adopt optoelectronic pole to form, and promptly the n N-type semiconductor N is as the light anode, and the p N-type semiconductor N is as photocathode.This battery structure operation does not need applied voltage, even it is also passable to be lower than the hydrogen reduction current potential in the flat rubber belting position, this just makes it become photoelectrochemical cell real Driven by Solar Energy, automatic bias.
Summary of the invention
The objective of the invention is to realize the conversion of solar energy-Hydrogen Energy, and a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making is provided in order to solve under the situation that does not need external energy fully.
The objective of the invention is to realize by following technical proposals:
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making is made up of the light anode with photoelectric respone ability, the photocathode with photoelectric respone ability, electrolyte and external circuit.
Its annexation is: the light anode with photoelectric respone ability partly immerses electrolyte with the photocathode with photoelectric respone ability, immerses part and is formed by connecting by external circuit.
The described automatic bias photoelectrochemical cell that is used for solar hydrogen making, the time that wherein has a photoelectric respone ability, is p N-type semiconductor N material photocathode very, comprises p type gallium phosphide, p type copper indium diselenide, p type cuprous oxide, p type silicon, p type silicon nanowires.
The described automatic bias photoelectrochemical cell that is used for solar hydrogen making, the light anode that wherein has the photoelectric respone ability are n N-type semiconductor N material light anode, comprise n type titanium oxide, n type zinc oxide, n type iron oxide, n type tungsten oxide, n p type gallium arensidep or n type silicon.
The described automatic bias photoelectrochemical cell that is used for solar hydrogen making, wherein electrolyte is the aqueous solution with conductivity, comprises acidic aqueous solution, neutral aqueous solution, alkaline aqueous solution or seawater.
The described automatic bias photoelectrochemical cell that is used for solar hydrogen making, wherein external circuit has the conductive path of the conducting medium composition of the light anode of photoelectric respone ability and the photocathode with photoelectric respone ability for connection.
Its course of work is: when this battery of solar light irradiation, have the light anode of photoelectric respone ability and have between the photocathode of photoelectric respone ability and produce electrical potential difference, can produce photogenerated current under the situation that external circuit is connected.
Its operation principle is: electric current comes from the electron exchange of optoelectronic pole and electrolyte, and being about to water decomposition is hydrogen and oxygen, so just under the situation of no applied voltage homenergic, realizes the conversion of solar energy and Hydrogen Energy.
Its preparation method is as follows: with selected photocathode with photoelectric respone ability, be that 3: 1 the sulfuric acid and the mixed solution of hydrogen peroxide clean successively through acetone, alcohol, volume ratio, put into the mixed solution that moves into hydrofluoric acid and silver nitrate after the hydrofluoric acid dips of dilution again and carry out hydro-thermal reaction, under 5-50 ℃, leave standstill reaction.Cooling is taken out the back and is fallen the surface porosity attachment with a large amount of deionized water rinsings, immerses red fuming nitric acid (RFNA) then and removes impurity silver, dries up at last.Select suitable light anode and electrolyte in addition, be assembled into the automatic bias photoelectrochemical cell with photoelectric respone ability.
Beneficial effect
1, the present invention has successfully realized relying on solar energy to carry out the photoelectrochemical cell of Conversion of energy fully; Described automatic bias photoelectrochemical cell need not applying bias under illumination can produce short circuit current, be that decomposition water begins to produce hydrogen, how many this size of current is directly proportional with product hydrogen, short-circuit photocurrent density can reach 10 microamperes more than every square centimeter, the open circuit voltage scope is greater than 100 millivolts, and the phototranstormation efficiency scope is greater than 0.01%.
2, a kind of this battery structure of automatic bias photoelectrochemical cell that is used for solar hydrogen making of the present invention is simple, saves cost, is easy to large-scale production, has a good application prospect.
Description of drawings
Fig. 1 is prepared solar hydrogen making automatic bias photoelectrochemical cell structural representation;
Fig. 2 is the short circuit current curve of embodiment 6 prepared automatic bias photoelectrochemical cells.
Wherein: light anode, the 2-that 1-has a photoelectric respone ability has photocathode, 3-electrolyte, the 4-external circuit of photoelectric respone ability.
Embodiment
The present invention will be further described below in conjunction with drawings and Examples.
Embodiment 1
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making mainly is made up of the light anode 1 with photoelectric respone ability, the photocathode 2 with photoelectric respone ability, electrolyte 3 and external circuit 4.Photocathode 2 the selection of materials with photoelectric respone ability are p type gallium phosphide; Light anode 1 the selection of material with photoelectric respone ability is a n type silicon; Electrolyte 3 the selection of materials are acidic aqueous solution.External circuit 4 is to have the light anode 1 of photoelectric respone ability and to have the conductive path that the photocathode 2 usefulness leads of photoelectric respone ability connect to form.
The annexation of this battery is that n type silicon and p type gallium phosphide partly immerse in the acidic aqueous solution, does not immerse part and by lead n type silicon and p type gallium phosphide is connected to form conductive path.
The course of work of this battery is for when the solar light irradiation battery, has the light anode 1 of photoelectric respone ability and have between the photocathode 2 of photoelectric respone ability to produce electrical potential difference, can produce photogenerated current under the situation of external circuit 4 connections, at 100mW/cm
2Record the battery short circuit current density under the illumination and reach 10 μ A/cm
2
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making mainly is made up of the light anode 1 with photoelectric respone ability, the photocathode 2 with photoelectric respone ability, electrolyte 3 and external circuit 4.Described photocathode 2 the selection of materials with photoelectric respone ability are p type copper indium diselenide; Described light anode 1 the selection of material with photoelectric respone ability is a n type zinc oxide; Described electrolyte 3 the selection of materials are the aqueous solution.Described external circuit 4 is to have the light anode 1 of photoelectric respone ability and to have the conductive path that the photocathode 2 of photoelectric respone ability directly connects to form.
The annexation of this battery is that n type zinc oxide and p type copper indium diselenide partly immerse in the aqueous solution, does not immerse part n type zinc oxide and p type copper indium diselenide are connected to form conductive path.
The course of work of this battery is for when the solar light irradiation battery, has the light anode 1 of photoelectric respone ability and have between the photocathode 2 of photoelectric respone ability to produce electrical potential difference, can produce photogenerated current under the situation of external circuit 4 connections, at 100mW/cm
2Record the battery short circuit current density under the illumination and reach 320 μ A/cm
2
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making mainly is made up of the light anode 1 with photoelectric respone ability, the photocathode 2 with photoelectric respone ability, electrolyte 3 and external circuit 4.Described photocathode 2 the selection of materials with photoelectric respone ability are p type cuprous oxide; Described light anode 1 the selection of material with photoelectric respone ability is a n type iron oxide; Described electrolyte 3 the selection of materials are alkaline aqueous solution.Described external circuit 4 is conductive paths that the light anode 1 that will have the photoelectric respone ability, the photocathode 2 usefulness leads with photoelectric respone ability and load connect to form
The annexation of this battery is that n type iron oxide and p type cuprous oxide partly immerse in the acidic aqueous solution, immerses part and by lead n type iron oxide and p type cuprous oxide and load is connected to form conductive path.
The course of work of this battery is for when the solar light irradiation battery, has the light anode 1 of photoelectric respone ability and have between the photocathode 2 of photoelectric respone ability to produce electrical potential difference, can produce photogenerated current under the situation of external circuit 4 connections, at 100mW/cm
2Record the battery short circuit current density under the illumination and reach 2mA/cm
2
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making mainly is made up of the light anode 1 with photoelectric respone ability, the photocathode 2 with photoelectric respone ability, electrolyte 3 and external circuit 4.Described photocathode 2 the selection of materials with photoelectric respone ability are p type silicon; Described light anode 1 the selection of material with photoelectric respone ability is a n type tungsten oxide; Described electrolyte 3 the selection of materials are seawater.Described external circuit 4 is conductive paths that light anode 1, photocathode 2 usefulness leads and load are connected to form
The annexation of this battery is that n type tungsten oxide and p type silicon partly immerse in the acidic aqueous solution, immerses part and by lead n type tungsten oxide and p type silicon and load is connected to form conductive path.
The course of work of this battery is for when the solar light irradiation battery, has the light anode 1 of photoelectric respone ability and have between the photocathode 2 of photoelectric respone ability to produce electrical potential difference, can produce photogenerated current under the situation of external circuit 4 connections, at 100mW/cm
2Record the battery short circuit current density under the illumination and reach 5mA/cm
2
Embodiment 5
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making mainly is made up of the light anode 1 with photoelectric respone ability, the photocathode 2 with photoelectric respone ability, electrolyte 3 and external circuit 4.Described photocathode 2 the selection of materials with photoelectric respone ability are p type silicon nanowires; Described light anode 1 the selection of material with photoelectric respone ability is the n p type gallium arensidep; Described electrolyte 3 the selection of materials are seawater.Described external circuit 4 is conductive paths that light anode 1, photocathode 2 usefulness leads and load are connected to form
The annexation of this battery is that n p type gallium arensidep and p type silicon nanowires partly immerse in the acidic aqueous solution, immerses part and by lead n p type gallium arensidep and p type silicon nanowires and load is connected to form conductive path.
The course of work of this battery is for when the solar light irradiation battery, has the light anode 1 of photoelectric respone ability and have between the photocathode 2 of photoelectric respone ability to produce electrical potential difference, can produce photogenerated current under the situation of external circuit 4 connections, at 100mW/cm
2Record the battery short circuit current density under the illumination and reach 10mA/cm
2
Embodiment 6
A kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making mainly is made up of the light anode 1 with photoelectric respone ability, the photocathode 2 with photoelectric respone ability, electrolyte 3 and external circuit 4, as shown in Figure 1.Described photocathode 2 the selection of materials with photoelectric respone ability are p type silicon nanowires; Described light anode 1 the selection of material with photoelectric respone ability is a n type titanium oxide; Described electrolyte 3 the selection of materials are aqueous sodium persulfate solution.Described external circuit 4 is conductive paths that light anode 1, photocathode 2 usefulness leads are connected to form
The annexation of this battery is that n type titanium oxide and p type silicon nanowires partly immerse in the acidic aqueous solution, does not immerse part and by lead n type titanium oxide and p type silicon nanowires is connected to form conductive path.
P type silicon chip is that 3: 1 the sulfuric acid and the mixed solution of hydrogen peroxide clean through acetone, alcohol, volume ratio successively, puts into the mixed solution that moves into hydrofluoric acid and silver nitrate after the hydrofluoric acid dips of dilution again and carries out hydro-thermal reaction, leaves standstill reaction under 50 ℃.Cooling is taken out the back and is fallen the surface porosity attachment with a large amount of deionized water rinsings, immerses red fuming nitric acid (RFNA) then and removes impurity silver, dries up at last, makes p type silicon nanowires, is assembled into the automatic bias photoelectrochemical cell with n type titanium oxide and acidic aqueous solution.
The course of work of this battery is for when the solar light irradiation battery, has the light anode 1 of photoelectric respone ability and have between the photocathode 2 of photoelectric respone ability to produce electrical potential difference, can produce photogenerated current under the situation of external circuit 4 connections.
500W xenon lamp (by ultraviolet/infrared filter, the cut-off wavelength scope is 350-750nm) is adopted in the photoelectrochemical behaviour test, and as the simulated solar irradiation source of parallel light, strength control is 100mW/cm
2Photoelectrochemical cell is connected electrochemical workstation.Testing impedance shows, under the a-c cycle of 10kHz, records p type silicon nanowire array carrier concentration 10
14-10
15In the scope, flat-band potential is in 0.1～0.2V scope.Under the potential scanning speed of 5mV/s, carry out test of current-voltage (I-V) curve and short circuit current test under dark attitude and the bright attitude, record the battery short circuit current density and reach 120 μ A/cm
2, the short circuit current curve as shown in Figure 2.
Claims (6)
1. automatic bias photoelectrochemical cell that is used for solar hydrogen making, it is characterized in that: this battery mainly is made up of the light anode (1) with photoelectric respone ability, the photocathode (2) with photoelectric respone ability, electrolyte (3) and external circuit (4).
2. a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making according to claim 1 is characterized in that: described light anode (1) with photoelectric respone ability is a n N-type semiconductor N material light anode.
3. a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making according to claim 1 is characterized in that: described photocathode (2) with photoelectric respone ability is a p N-type semiconductor N material photocathode.
4. a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making according to claim 1 is characterized in that: described electrolyte (3) is for having the aqueous solution of conductivity.
5. a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making according to claim 1 is characterized in that: the conductive path that described external circuit (4) is formed for the conducting medium that connects light anode and photocathode.
6. a kind of automatic bias photoelectrochemical cell that is used for solar hydrogen making according to claim 1, it is characterized in that: the syndeton of this battery is the light anode (1) of photoelectric respone ability to be arranged and have photocathode (2) part of photoelectric respone ability to immerse in the electrolyte (3), does not immerse part and is connected by external circuit (4).
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104330153A (en) * | 2014-10-11 | 2015-02-04 | 深圳市开天源自动化工程有限公司 | Method for measuring intensity of ultraviolet light |
| CN106367775A (en) * | 2016-09-06 | 2017-02-01 | 山东大学 | Method of utilizing a built-in electric field in polar crystal to adjust and control separation efficiency and optic electrochemical activity of photon-generated carriers in photoelectrode of ZnO single crystal |
| CN108550963A (en) * | 2018-05-03 | 2018-09-18 | 南京大学 | A method of improving InGaN/GaN material multiple quantum wells solar energy electrochemical cell efficiency using polarization regulation and control |
| CN109637813A (en) * | 2018-11-12 | 2019-04-16 | 华东师范大学 | A kind of sunlight helps seawater battery and preparation method |
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| CN101853973A (en) * | 2010-05-07 | 2010-10-06 | 北京理工大学 | Photo-electrochemical cell with nanostructure for solar hydrogen production and preparation method thereof |
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| CN101853973A (en) * | 2010-05-07 | 2010-10-06 | 北京理工大学 | Photo-electrochemical cell with nanostructure for solar hydrogen production and preparation method thereof |
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| 《ELECTROCHEMICAL AND SOLID STATE LETTERS》 20060215 Ingler. WB，etal A Self-Driven p∕n-Fe2O3 Tandem Photoelectrochemical Cell for Water Splitting 第144-146页 第9卷, 第4期 * |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104330153A (en) * | 2014-10-11 | 2015-02-04 | 深圳市开天源自动化工程有限公司 | Method for measuring intensity of ultraviolet light |
| CN104330153B (en) * | 2014-10-11 | 2017-07-11 | 深圳市开天源自动化工程有限公司 | The measuring method of ultraviolet ray intensity |
| CN106367775A (en) * | 2016-09-06 | 2017-02-01 | 山东大学 | Method of utilizing a built-in electric field in polar crystal to adjust and control separation efficiency and optic electrochemical activity of photon-generated carriers in photoelectrode of ZnO single crystal |
| CN108550963A (en) * | 2018-05-03 | 2018-09-18 | 南京大学 | A method of improving InGaN/GaN material multiple quantum wells solar energy electrochemical cell efficiency using polarization regulation and control |
| CN109637813A (en) * | 2018-11-12 | 2019-04-16 | 华东师范大学 | A kind of sunlight helps seawater battery and preparation method |
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