CN107768690A - A kind of semiconductive thin film Electrolyte type fuel cell and preparation method thereof - Google Patents
A kind of semiconductive thin film Electrolyte type fuel cell and preparation method thereof Download PDFInfo
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- CN107768690A CN107768690A CN201710754210.3A CN201710754210A CN107768690A CN 107768690 A CN107768690 A CN 107768690A CN 201710754210 A CN201710754210 A CN 201710754210A CN 107768690 A CN107768690 A CN 107768690A
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- thin film
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
- H01M4/8825—Methods for deposition of the catalytic active composition
- H01M4/8864—Extrusion
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
- H01M8/126—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing cerium oxide
-
- 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
- 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
- Y02E60/50—Fuel cells
-
- 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The invention provides a kind of semiconductive thin film Electrolyte type fuel cell and preparation method thereof, structure is cathode layer, dielectric substrate, anode layer；Wherein, cathode layer materials ABO3Type perovskite oxide material or stratiform lithium-containing oxides material, or its composite with 0 50wt.% doped cerium oxides；Electrolyte layer is binary oxide semi-conducting material；Anode layer material is stratiform lithium-containing oxides material or nickel, cobalt/cobalt oxide material, or its composite with 0 50wt.% doped cerium oxides.Making step is：Pressed-powder anode potsherd, then prepares thin film shape dielectric substrate at a surface thereof, re-compacted cathodic ceramic piece, then with dielectric substrate fitting that cathodic ceramic piece and anode potsherd is compressed together and carry out high temperature sintering, that is, obtains product of the present invention.Electrolytic thin-membrane thinner thickness of the present invention and adjustable controllable, electrolyte composition is simple, preparation temperature is low, cheap；Battery has the characteristics of operation temperature is low.
Description
Technical field
The invention belongs to field of solid oxide fuel, and in particular to a kind of semiconductive thin film electrolyte-type fuel electricity
Pond and preparation method thereof.
Background technology
SOFC is a kind of clean energy resource conversion equipment with high conversion efficiency.Soild oxide fires
Expect that battery so far, had gone through the developing history of more than 170 years in invention in 1839.Traditional SOFC master
To be made up of trilaminate material：Anode, electrolyte, negative electrode.Its core component dielectric substrate is mainly yttrium stable zirconium oxide material.Should
Material needs that 0.1S/cm ionic conductivity can be obtained at a high temperature of more than 1000 DEG C.Therefore, solid oxide fuel electricity
Pond generally requires to work under higher operating temperatures, and still, caused by high temperature thus various problems produce.Such as anode, electricity
Xie Zhi, negative electrode trilaminate material thermal coefficient of expansion matching problem, and the high temperature tolerance sex chromosome mosaicism of seal and connector；Cause
This operation temperature for reducing SOFC always is the emphasis of research.At present, using doped cerium oxide or
Proton-conductive electrolyte substitutes traditional yttrium stable zirconium oxide electrolyte, can effectively reduce solid oxide fuel electricity
The operating temperature in pond.Meanwhile the catalytic activity of low temperature lower electrode material is also to influence the key factor of battery performance output.
In recent years, there are some researches show, the electrode material of conventional solid oxide fuel cells is mixed with electrolyte,
The fuel cell being prepared at low temperature there is higher performance to export.This battery is referred to as " electroless matter barrier film fuel
Battery ", also referred to as " single part fuel cell ".In the battery, conduct ion is not the pure ionic conduction to electronic isolation
Electrolyte, but the composite with Mixed electronic- ionic conduction.The working mechanism of the battery does not obtain yet so far
It is extensive to understand.At present, a kind of explain is in the type battery, due to the presence of semiconductor pn junction or schottky junction, is avoided
The short circuit of inside battery.This battery has good catalytic performance and power output at low temperature, is to solve soild oxide
The important measure of fuel cell low temperature.
Oxide semiconductor is functional material widely studied at present, has many excellent performances.Oxide semiconductor
The defects of can as a kind of important carrier of conduction ion, therefore semiconductor Electrolyte type fuel cell of the present invention,
It is in the scientific basic of single part battery, the electrolysis of SOFC is used as using oxide semiconductor sill
Matter, to promote the low temperature of SOFC.
The content of the invention
The purpose of the present invention is to be directed to limitation of the existing SOFC technology to dielectric substrate, there is provided a kind of
Semiconductive thin film Electrolyte type fuel cell, without the pure ion conductor to electronic isolation as electrolyte, and partly led with having
The sull of body conductive characteristic is as dielectric substrate, selection model of the increase SOFC to electrolyte
Enclose, reduce the operation temperature of battery.
In order to solve the above technical problems, the present invention adopts the following technical scheme that：
1) a kind of semiconductive thin film Electrolyte type fuel cell, it includes cathode layer (1), the electrolyte being in close contact successively
Layer (2), anode layer (3)；
Described cathode layer (1) material is ABO3Type perovskite oxide material or stratiform lithium-containing oxides LiNixCo1-x- yAlyO2(0≤x≤0.8,0≤y≤0.5,0≤x+y≤1, material, or its composite with 0-50wt.% doped cerium oxides；
The ABO3Type perovskite oxide material refers to ABO3The oxide material of type perovskite structure, including
MxSr1-xCo0.2Fe0.8O3(M=La, Ba；X=0.7,0.6), La0.7Sr0.3MxMn1-xO3(M=Cr, Fe；0≤x≤0.2)、
Sr2FexMo2-xO6(0≤x≤1.5) etc. but not limited to this.
Described dielectric substrate (2) material is titanium dioxide, zinc oxide, alundum (Al2O3), ceria, tungstic acid etc.
Binary oxide semi-conducting material；
Described anode layer (3) material is stratiform lithium-containing oxides LiNixCo1-x-yAlyO2(0≤x≤0.8,0≤y≤
The material of 0.5,0≤x+y≤1 or nickel, cobalt/cobalt oxide material, or its composite with 0-50wt.% doped cerium oxides.
2) a kind of preparation method of semiconductive thin film Electrolyte type fuel cell, it is characterised in that specific make step is such as
Under：
(a) powdered anode material is pressed into the thick potsherd of 100-1500 microns；
(b) film-shaped electrolyte layer of one layer of 50-2000 nanometer thickness is prepared on the anode potsherd of above-mentioned acquisition；
(c) powdered cathode material is pressed into the thick potsherd of 50-1000 microns by support of nickel foam；
(d) dielectric substrate on the face where the cathode material of above-mentioned cathodic ceramic piece and anode potsherd is compressed on one
Rise, carry out high temperature sintering in 450-650 DEG C, obtain semiconductive thin film Electrolyte type fuel cell.
Above-mentioned steps (b) the film-shaped electrolyte matter can pass through the tape casting, slurry cladding process, sol-gal process, magnetic control
The methods of sputtering method, atomic layer deposition method, obtains.
It is using beneficial effect caused by above-mentioned technical proposal：The invention provides a kind of brand-new fuel cell electricity
Solve material system of selection and build the thinking of fuel cell；
From conductor oxidate as electrolyte, can be avoided from the angle of semiconductor energy band structure in battery
Short circuit occurs for portion；
From binary semiconductor oxide as electrolyte, the composition and material preparation process of material are enormously simplify, is dropped
Low cost of manufacture；
From the dielectric substrate of film-form, the Ohmic resistance of dielectric substrate can be effectively reduced, reduces battery operational temperatures.
The electrolytic thin-membrane thinner thickness of a kind of semiconductive thin film Electrolyte type fuel cell provided by the invention and adjustable
Controllable, electrolyte composition is simple, preparation temperature is low, cheap；Battery has the characteristics of operation temperature is low.
Brief description of the drawings
Fig. 1 is a kind of structural representation of semiconductive thin film Electrolyte type fuel cell；
Fig. 2 is the microcosmic surface of the titanium deoxid film obtained on anode potsherd using slurry cladding process；
Fig. 3 is a kind of microscopic cross of semiconductive thin film Electrolyte type fuel cell；
Fig. 4 is to use LiNi0.8Co0.15Al0.05O2As cathode material and anode material, titanium dioxide as electrolysis material
Chemical property curve of the fuel cell of material at 550 degrees Celsius.
Embodiment
Embodiment 1：
By powdered anode material LiNi0.8Co0.2O2(Al hereiny, y=0) and it is pressed into 1500 microns of thick potsherds；
Then, the film-form cerium oxide electricity of one layer of 500 nanometer thickness is prepared using magnetron sputtering method on the anode potsherd of above-mentioned acquisition
Solve matter layer；Then, by powdered cathode material La0.6Sr0.4Co0.2Fe0.8O3500 microns of thickness are pressed into by support of nickel foam
Potsherd；Finally, the dielectric substrate on the face where the cathode material of above-mentioned cathodic ceramic piece and anode potsherd is suppressed
High temperature sintering is carried out under 500 degrees Celsius together, obtains semiconductive thin film Electrolyte type fuel cell.
Embodiment 2：
By powdered anode material LiNi0.8Co0.15Al0.05O2It is pressed into 100 microns of thick potsherds；Then, upper
State the film-form titanium dioxide dielectric substrate for preparing one layer of 50 nanometer thickness on the anode potsherd of acquisition using sol-gal process；Connect
, by powdered cathode material LiNi0.8Co0.15Al0.05O21000 microns of thick potsherds are pressed into by support of nickel foam；
Finally, by the dielectric substrate on the face where the cathode material of above-mentioned cathodic ceramic piece and anode potsherd it is compressed together in
High temperature sintering is carried out under 650 degrees Celsius, obtains semiconductive thin film Electrolyte type fuel cell.
Embodiment 3：
By powdered anode material LiNi0.8Co0.15Al0.05O2With weight than being mixed for 50wt.% samarium doping cerium oxide
Merging is pressed into 800 microns of thick potsherds；Then, one layer is prepared using the tape casting on the anode potsherd of above-mentioned acquisition
The film-form zinc oxide dielectric substrate of 2000 nanometer thickness；Then, by powdered cathode material LiNi0.8Co0.15Al0.05O2With again
Measure than the samarium doping cerium oxide mixing for 50wt.% and be pressed into 50 microns of thick potsherds by support of nickel foam；Finally, will
Face where the cathode material of above-mentioned cathodic ceramic piece and the dielectric substrate on anode potsherd are compressed together in 600 degrees Celsius
Lower carry out high temperature sintering, obtains semiconductive thin film Electrolyte type fuel cell.
Embodiment 4：
By powdered anode material NiO2It is pressed into 1000 microns of thick potsherds；Then, in the anode of above-mentioned acquisition
The film-form alundum (Al2O3) dielectric substrate of one layer of 100 nanometer thickness is prepared on potsherd using atomic layer deposition method；Then, by powder
The cathode material LiCoO of last shape2With weight than mixing for 20wt.% samarium doping cerium oxide and being pressed into by support of nickel foam
800 microns of thick potsherds；Finally, by the electrolysis on the face where the cathode material of above-mentioned cathodic ceramic piece and anode potsherd
Matter is laminated together to carry out high temperature sintering under 450 degrees Celsius, obtains semiconductive thin film Electrolyte type fuel cell.
Embodiment 5：
By powdered anode material LiCo0.5Al0.5O2With weight than mixing compacting for 30wt.% samarium doping cerium oxide
The potsherd thick into 900 microns；Then, prepared one layer 800 and received using silk screen print method on the anode potsherd of above-mentioned acquisition
The thick film-form tungstic acid dielectric substrate of rice；Then, by powdered cathode material Sr2Fe1.5Mo0.5O6Using nickel foam as branch
200 microns of thick potsherds are made in bulging；Finally, by the face where the cathode material of above-mentioned cathodic ceramic piece and anode potsherd
On dielectric substrate it is compressed together high temperature sintering is carried out under 550 degrees Celsius, obtain semiconductive thin film electrolyte-type fuel electricity
Pond.
The foregoing is only presently preferred embodiments of the present invention, all equivalent changes done according to scope of the present invention patent with
Modification, it should all belong to the covering scope of the present invention.
Claims (3)
1. a kind of semiconductive thin film Electrolyte type fuel cell, it includes cathode layer (1), the dielectric substrate being in close contact successively
(2), anode layer (3), it is characterised in that：
Described cathode layer (1) material is ABO3Type perovskite oxide material or stratiform lithium-containing oxides LiNixCo1-x-yAlyO2
Material, 0≤x≤0.8,0≤y≤0.5,0≤x+y≤1, or its composite with 0-50wt.% doped cerium oxides；
The ABO3Type perovskite oxide material refers to ABO3The oxide material M of type perovskite structurexSr1- xCo0.2Fe0.8O3, M=La, Ba, x=0.7,0.6；Either La0.7Sr0.3MxMn1-xO3, M=Cr, Fe, 0≤x≤0.2；Or
It is Sr2FexMo2-xO6, 0≤x≤1.5；
Described dielectric substrate (2) material is titanium dioxide, zinc oxide, alundum (Al2O3), ceria, tungstic acid binary oxygen
Compound semi-conducting material；
Described anode layer (3) material is stratiform lithium-containing oxides LiNixCo1-x-yAlyO2, 0≤x≤0.8,0≤y≤0.5,0≤
The material of x+y≤1 or nickel, cobalt/cobalt oxide material, or its composite with 0-50wt.% doped cerium oxides.
2. a kind of preparation method of semiconductive thin film Electrolyte type fuel cell, it is characterised in that specific make step is as follows：
(a) powdered anode material is pressed into the thick potsherd of 100-1500 microns；
(b) film-shaped electrolyte layer of one layer of 50-2000 nanometer thickness is prepared on the anode potsherd of above-mentioned acquisition；
(c) powdered cathode material is pressed into the thick potsherd of 50-1000 microns by support of nickel foam；
It is (d) face where the cathode material of above-mentioned cathodic ceramic piece and the dielectric substrate on anode potsherd is compressed together,
High temperature sintering is carried out in 450-650 DEG C, obtains semiconductive thin film Electrolyte type fuel cell.
A kind of 3. preparation method of semiconductive thin film Electrolyte type fuel cell according to claim 2, it is characterised in that
Prepared on step (b) Anodic potsherd the method for the film-shaped electrolyte layer of one layer of 50-2000 nanometer thickness for the tape casting or
Slurry cladding process or silk screen print method or sol-gal process or magnetron sputtering method or atomic layer deposition method.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109360991A (en) * | 2018-11-01 | 2019-02-19 | 东北大学 | A kind of low-temperature solid oxide fuel cell composite cathode and preparation method thereof |
| CN109524675A (en) * | 2018-11-15 | 2019-03-26 | 辽宁石油化工大学 | A kind of solid oxide fuel cell and preparation method thereof |
| CN109671958A (en) * | 2018-11-02 | 2019-04-23 | 全球能源互联网研究院有限公司 | A kind of solid oxide fuel cell and preparation method thereof |
| CN110021771A (en) * | 2019-04-23 | 2019-07-16 | 湖北大学 | Based on SnO2The preparation method of-SDC semiconductor-ion conductor schottky junction fuel cell |
| CN112687929A (en) * | 2020-12-29 | 2021-04-20 | 东北大学 | Lithium oxide electrode micro-molten salt ceramic fuel cell and preparation method thereof |
| CN113782794A (en) * | 2021-08-30 | 2021-12-10 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
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| CN101523645A (en) * | 2006-08-02 | 2009-09-02 | 康宁股份有限公司 | A solid oxide fuel cell device with an elongated seal geometry |
| CN105006580A (en) * | 2014-04-22 | 2015-10-28 | 南京蕴纳纳米科技有限公司 | Manufacturing of low-temperature solid oxide fuel cell with cobalt-nickel- aluminum-lithium oxide and doped cerium oxide composite material |
| CN105140526A (en) * | 2015-07-22 | 2015-12-09 | 中国地质大学（武汉） | Fuel cell and manufacturing method of fuel cell |
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Patent Citations (4)
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| US4032694A (en) * | 1976-08-26 | 1977-06-28 | General Electric Company | Fuel cell with hydronium beta-alumina electrolyte |
| CN101523645A (en) * | 2006-08-02 | 2009-09-02 | 康宁股份有限公司 | A solid oxide fuel cell device with an elongated seal geometry |
| CN105006580A (en) * | 2014-04-22 | 2015-10-28 | 南京蕴纳纳米科技有限公司 | Manufacturing of low-temperature solid oxide fuel cell with cobalt-nickel- aluminum-lithium oxide and doped cerium oxide composite material |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109360991A (en) * | 2018-11-01 | 2019-02-19 | 东北大学 | A kind of low-temperature solid oxide fuel cell composite cathode and preparation method thereof |
| CN109360991B (en) * | 2018-11-01 | 2021-12-14 | 东北大学 | Low-temperature solid oxide fuel cell composite cathode and preparation method thereof |
| CN109671958A (en) * | 2018-11-02 | 2019-04-23 | 全球能源互联网研究院有限公司 | A kind of solid oxide fuel cell and preparation method thereof |
| CN109524675A (en) * | 2018-11-15 | 2019-03-26 | 辽宁石油化工大学 | A kind of solid oxide fuel cell and preparation method thereof |
| CN110021771A (en) * | 2019-04-23 | 2019-07-16 | 湖北大学 | Based on SnO2The preparation method of-SDC semiconductor-ion conductor schottky junction fuel cell |
| CN112687929A (en) * | 2020-12-29 | 2021-04-20 | 东北大学 | Lithium oxide electrode micro-molten salt ceramic fuel cell and preparation method thereof |
| CN113782794A (en) * | 2021-08-30 | 2021-12-10 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
| CN113782794B (en) * | 2021-08-30 | 2024-03-08 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
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