CN107768690B - Semiconductor film electrolyte type fuel cell and its making method - Google Patents
Semiconductor film electrolyte type fuel cell and its making method Download PDFInfo
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- CN107768690B CN107768690B CN201710754210.3A CN201710754210A CN107768690B CN 107768690 B CN107768690 B CN 107768690B CN 201710754210 A CN201710754210 A CN 201710754210A CN 107768690 B CN107768690 B CN 107768690B
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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
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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
- 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
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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
- 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
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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
- 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 semiconductor film electrolyte type fuel cell and a manufacturing method thereof, and the structure is a cathode layer, an electrolyte layer and an anode layer; wherein the cathode layer is made of ABO3Perovskite oxide materials or layered lithium-containing oxide materials, or composites thereof with 0-50 wt.% doped ceria; the electrolyte layer material is a binary oxide semiconductor material; the anode layer material is a layered lithium-containing oxide material or a nickel-cobalt oxide material, or a composite material of the layered lithium-containing oxide material and 0-50 wt.% of doped cerium oxide. The manufacturing steps are as follows: pressing the anode ceramic chip, preparing a film-shaped electrolyte layer on one surface of the anode ceramic chip, pressing the cathode ceramic chip, adhering the electrolyte layer to the cathode ceramic chip and the anode ceramic chip, pressing the cathode ceramic chip and the anode ceramic chip together, and sintering at high temperature to obtain the product of the invention. The electrolyte film has the advantages of thin thickness, adjustability, controllability, simple components of electrolyte materials, low preparation temperature and low price; the battery has the characteristic of low operating temperature.
Description
Technical Field
The invention belongs to the field of solid oxide fuel cells, and particularly relates to a semiconductor thin film electrolyte type fuel cell and a manufacturing method thereof.
Background
Solid oxide fuel cells are a clean energy conversion device with high conversion efficiency. Solid oxide fuel cells, invented to date in 1839, have experienced over 170 years of development. Conventional solid oxide fuel cells are mainly composed of three layers of materials: anode, electrolyte, cathode. The electrolyte layer of the core component is mainly yttrium-stabilized zirconia material. The material needs to obtain the ionic conductivity of 0.1S/cm at the high temperature of more than 1000 ℃. Therefore, the solid oxide fuel cell generally needs to operate at a higher operating temperature, but various problems caused by the high temperature are caused thereby. For example, matching of thermal expansion coefficients of anode, electrolyte and cathode three-layer materials, and high temperature resistance of seals and connectors; therefore, reducing the operating temperature of solid oxide fuel cells has been the focus of research. At present, the doped cerium oxide or proton conductive electrolyte is adopted to replace the traditional yttrium-stabilized zirconia electrolyte material, so that the working temperature of the solid oxide fuel cell can be effectively reduced. Meanwhile, the catalytic activity of the electrode material at low temperature is also a key factor influencing the performance output of the battery.
In recent years, research shows that the fuel cell prepared by mixing the electrode material and the electrolyte material of the traditional solid oxide fuel cell has higher performance output at low temperature. Such cells are known as "electrolyte-free membrane fuel cells", also known as "single component fuel cells". In this battery, the ion-conducting is not a pure ion-conducting electrolyte material insulating from electrons, but a composite material having electron-ion mixed conductivity. The mechanism of operation of the cell has not been widely understood to date. One explanation is that, at present, in this type of battery, short circuits inside the battery are avoided due to the presence of a semiconductor pn-or schottky-junction. The battery has good catalytic performance and power output at low temperature, and is an important measure for solving the problem of low temperature of the solid oxide fuel battery.
Oxide semiconductors are currently widely studied as functional materials with many excellent properties. The defects in the oxide semiconductor can be used as important carriers for conducting ions, so the invention relates to a semiconductor electrolyte type fuel cell, which is based on the science of a single-component cell and takes an oxide semiconductor-based material as an electrolyte of the solid oxide fuel cell so as to promote the low temperature of the solid oxide fuel cell.
Disclosure of Invention
The invention aims to provide a semiconductor thin film electrolyte type fuel cell aiming at the limitation of the existing solid oxide fuel cell technology on an electrolyte layer, which does not use a pure ion conductor insulated from electrons as an electrolyte, but uses an oxide thin film with semiconductor conductive characteristics as the electrolyte layer, thereby increasing the selection range of the solid oxide fuel cell on the electrolyte material and reducing the operation temperature of the cell.
In order to solve the technical problems, the invention adopts the following technical scheme:
1) a semiconductor thin film electrolyte type fuel cell includes a cathode layer (1), an electrolyte layer (2), and an anode layer (3) which are in close contact in this order;
the cathode layer (1) is made of ABO3Perovskite oxide material or layered lithium-containing oxide LiNixCo1-x- yAlyO2(x is more than or equal to 0 and less than or equal to 0.8, y is more than or equal to 0 and less than or equal to 0.5, and x + y is more than or equal to 0 and less than or equal to 1) or a composite material of the material and 0-50 wt.% of doped cerium oxide;
the ABO3Perovskite oxide material refers to perovskite oxide material having ABO3An oxide material of perovskite structure comprising 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. ltoreq. x. ltoreq.1.5), and the like, but are not limited thereto.
The electrolyte layer (2) is made of binary oxide semiconductor materials such as titanium dioxide, zinc oxide, aluminum oxide, cerium dioxide and tungsten trioxide;
the anode layer (3) is made of layered lithium-containing oxide LiNixCo1-x-yAlyO2(x is more than or equal to 0 and less than or equal to 0.8, y is more than or equal to 0 and less than or equal to 0.5, and x + y is more than or equal to 0 and less than or equal to 1 material or nickel and cobalt oxide material, or composite material of the nickel and cobalt oxide material and 0-50 wt.% of doped cerium oxide.
2) A preparation method of a semiconductor film electrolyte type fuel cell is characterized by comprising the following specific manufacturing steps:
(a) pressing the powdery anode material into a ceramic sheet with the thickness of 100 and 1500 microns;
(b) preparing a film-shaped electrolyte layer with the thickness of 50-2000 nm on the obtained anode ceramic sheet;
(c) pressing the powdery cathode material into a ceramic sheet with the thickness of 50-1000 microns by taking foamed nickel as a support;
(d) and pressing the surface of the cathode material of the cathode ceramic piece and the electrolyte layer on the anode ceramic piece together, and sintering at the temperature of 450-650 ℃ to obtain the semiconductor thin film electrolyte type fuel cell.
The film-like electrolyte in the step (b) can be obtained by a casting method, a slurry coating method, a sol-gel method, a magnetron sputtering method, an atomic layer deposition method, or the like.
Adopt the produced beneficial effect of above-mentioned technical scheme to lie in: the invention provides a novel fuel cell electrolyte material selection method and a fuel cell construction idea;
the semiconductor oxide is selected as the electrolyte material, so that the short circuit in the battery can be avoided from the perspective of a semiconductor energy band structure;
the binary semiconductor oxide is selected as the electrolyte, so that the components of the material and the preparation process of the material are greatly simplified, and the manufacturing cost is reduced;
the thin-film electrolyte layer is selected, so that the ohmic resistance of the electrolyte layer can be effectively reduced, and the operating temperature of the battery can be reduced.
The electrolyte film of the semiconductor film electrolyte type fuel cell provided by the invention has the advantages of thin thickness, adjustability, controllability, simple electrolyte material components, low preparation temperature and low price; the battery has the characteristic of low operating temperature.
Drawings
Fig. 1 is a schematic view of the structure of a semiconductor thin film electrolyte type fuel cell;
FIG. 2 is a microscopic surface of a titanium dioxide film obtained by a slurry coating method on an anode ceramic sheet;
FIG. 3 is a microscopic cross section of a semiconductor thin film electrolyte type fuel cell;
FIG. 4 is a schematic representation of the use of LiNi0.8Co0.15Al0.05O2The electrochemical performance curve at 550 degrees celsius for a fuel cell with titanium dioxide as the electrolyte material, as the cathode material and the anode material.
Detailed Description
Example 1:
mixing anode material LiNi in powder form0.8Co0.2O2(Here, Al is present)yY is 0) is pressed into a ceramic sheet with the thickness of 1500 microns; then, preparing a film-shaped cerium oxide electrolyte layer with the thickness of 500 nanometers on the obtained anode ceramic sheet by a magnetron sputtering method; then, the powdered cathode material La was added0.6Sr0.4Co0.2Fe0.8O3Pressing into a ceramic sheet with the thickness of 500 microns by taking foamed nickel as a support; and finally, pressing the surface of the cathode material of the cathode ceramic piece and the electrolyte layer on the anode ceramic piece together, and sintering at the high temperature of 500 ℃ to obtain the semiconductor thin film electrolyte type fuel cell.
Example 2:
mixing anode material LiNi in powder form0.8Co0.15Al0.05O2Pressing into a ceramic sheet with the thickness of 100 microns; then, preparing a 50 nanometer thick film-shaped titanium dioxide electrolyte layer on the obtained anode ceramic sheet by a sol-gel method; then, a powdery cathode material LiNi was added0.8Co0.15Al0.05O2Pressing foamed nickel as a support into a ceramic sheet with the thickness of 1000 microns; and finally, pressing the surface of the cathode material of the cathode ceramic piece and the electrolyte layer on the anode ceramic piece together, and sintering at the high temperature of 650 ℃ to obtain the semiconductor thin film electrolyte type fuel cell.
Example 3:
mixing anode material LiNi in powder form0.8Co0.15Al0.05O2Mixing with samarium-doped cerium oxide in a weight ratio of 50 wt.% and pressing into a ceramic sheet with a thickness of 800 microns; then, preparing a 2000 nm-thick film zinc oxide electrolyte layer on the obtained anode ceramic sheet by using a tape casting method; then, a powdery cathode material LiNi was added0.8Co0.15Al0.05O2Mixing with samarium-doped cerium oxide in a weight ratio of 50 wt.% and pressing into a ceramic sheet with a thickness of 50 microns by using foamed nickel as a support; finally, the surface of the cathode ceramic piece where the cathode material is positioned and the anode ceramic piece are electrolyzedThe layers are pressed together and sintered at 600 c to obtain a semiconductor thin film electrolyte type fuel cell.
Example 4:
NiO is added to the powdery anode material2Pressing into a ceramic sheet with the thickness of 1000 microns; then, preparing a film-shaped aluminum oxide electrolyte layer with the thickness of 100 nanometers on the obtained anode ceramic sheet by utilizing an atomic layer deposition method; then, LiCoO, a powdery cathode material2Mixing with 20 wt.% of samarium-doped cerium oxide and pressing into a ceramic sheet with the thickness of 800 microns by taking foamed nickel as a support; and finally, pressing the surface of the cathode material of the cathode ceramic piece and the electrolyte layer on the anode ceramic piece together at 450 ℃ for high-temperature sintering to obtain the semiconductor thin-film electrolyte type fuel cell.
Example 5:
preparing anode material LiCo in powder form0.5Al0.5O2Mixing with 30 wt.% samarium-doped cerium oxide, and pressing into ceramic sheet with thickness of 900 μm; then, preparing a thin film tungsten trioxide electrolyte layer with the thickness of 800 nanometers on the obtained anode ceramic sheet by a screen printing method; then, the powdery cathode material Sr is added2Fe1.5Mo0.5O6Pressing into a ceramic sheet with the thickness of 200 microns by taking foamed nickel as a support; and finally, pressing the surface of the cathode material of the cathode ceramic piece and the electrolyte layer on the anode ceramic piece together, and sintering at 550 ℃ at high temperature to obtain the semiconductor thin film electrolyte type fuel cell.
The above description is only a preferred embodiment of the present invention, and all equivalent changes and modifications made in accordance with the claims of the present invention should be covered by the present invention.
Claims (2)
1. A semiconductor thin film electrolyte type fuel cell comprising a cathode layer (1), an electrolyte layer (2), and an anode layer (3) in close contact in this order, characterized in that:
the cathode layer (1) is made of ABO3Perovskite oxide materials or layersLiNi oxide containing lithiumxCo1-x-yAlyO2X is more than or equal to 0 and less than or equal to 0.8, y is more than or equal to 0 and less than or equal to 0.5, and x + y is more than or equal to 0 and less than or equal to 1, or a composite material formed by mixing any one of the oxides and 0-50 wt.% of doped cerium oxide;
the ABO3Perovskite oxide material refers to perovskite oxide material having ABO3Oxide material M of perovskite structurexSr1- xCo0.2Fe0.8O3M = La or Ba, x =0.7, 0.6; or is La0.7Sr0.3MxMn1-xO3M = Cr or Fe, x is more than or equal to 0 and less than or equal to 0.2; or is Sr2FexMo2-xO6 ，0≤x≤1.5；
The electrolyte layer (2) is made of a binary oxide semiconductor material, and the binary oxide semiconductor material is titanium dioxide, zinc oxide, aluminum oxide or tungsten trioxide;
the electrolyte layer (2) is obtained by preparing a film-shaped electrolyte layer with the thickness of 50-2000 nm on the anode layer (3) by a slurry coating method, a sol-gel method, a magnetron sputtering method or an atomic layer deposition method;
the anode layer (3) is made of layered lithium-containing oxide LiNixCo1-x-yAlyO2X is more than or equal to 0 and less than or equal to 0.8, y is more than or equal to 0 and less than or equal to 0.5, and x + y is more than or equal to 0 and less than or equal to 1, or a composite material of the material and 0-50 wt.% of doped cerium oxide.
2. A method for manufacturing a semiconductor thin film electrolyte type fuel cell according to claim 1, characterized by comprising the steps of:
(a) pressing the powdery anode material into a ceramic sheet with the thickness of 100 and 1500 microns;
(b) preparing a film-shaped electrolyte layer with the thickness of 50-2000 nm on the obtained anode ceramic sheet;
(c) pressing the powdery cathode material into a ceramic sheet with the thickness of 50-1000 microns by taking foamed nickel as a support;
(d) and pressing the surface of the cathode material of the cathode ceramic piece and the electrolyte layer on the anode ceramic piece together, and sintering at the temperature of 450-650 ℃ to obtain the semiconductor thin film electrolyte type fuel cell.
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| CN109360991B (en) * | 2018-11-01 | 2021-12-14 | 东北大学 | Low-temperature solid oxide fuel cell composite cathode and preparation method thereof |
| CN109671958B (en) * | 2018-11-02 | 2021-04-27 | 全球能源互联网研究院有限公司 | 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 |
| CN110021771B (en) * | 2019-04-23 | 2020-07-28 | 湖北大学 | Based on SnO2Preparation method of Schottky junction fuel cell of-SDC semiconductor-ion conductor |
| 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 |
| CN113782794B (en) * | 2021-08-30 | 2024-03-08 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
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 |
| 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)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| 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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