CN108417872B - Composite YSZ electrolyte of solid oxide fuel cell and preparation method thereof - Google Patents
Composite YSZ electrolyte of solid oxide fuel cell and preparation method thereof Download PDFInfo
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- CN108417872B CN108417872B CN201810448929.9A CN201810448929A CN108417872B CN 108417872 B CN108417872 B CN 108417872B CN 201810448929 A CN201810448929 A CN 201810448929A CN 108417872 B CN108417872 B CN 108417872B
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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
- H01M8/1253—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 zirconium oxide
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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
- H01M2008/1293—Fuel cells with solid oxide electrolytes
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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
Abstract
The invention provides a composite YSZ electrolyte of a solid oxide fuel cell and a preparation method thereof, wherein the composite YSZ electrolyte is formed by sequentially laminating a first YSZ tape casting sheet, a second YSZ tape casting sheet and a first YSZ tape casting sheet; through holes are distributed in an array mode on the first YSZ casting sheet, and grooves are distributed in an array mode on the upper surface and the lower surface of the second YSZ casting sheet. The invention can reduce the thickness of the SOFC electrolyte and ensure that the cell has enough mechanical strength, thereby reducing the ohmic resistance of the cell. In addition, the electrolyte with the novel structure can enlarge the interface area of the electrode/electrolyte and provide more active reaction points for electrochemical reaction, thereby reducing the polarization resistance of the battery.
Description
Technical Field
The invention relates to the field of solid oxide fuel cells, in particular to a composite YSZ electrolyte of a solid oxide fuel cell and a preparation method thereof.
Technical Field
Energy is an important foundation on which human society relies to survive and develop. Fossil energy, coal, oil and natural gas, remain the most important energy resources in today's society, but these energy resources will be depleted continuously with the rapid development of human society. Moreover, fossil energy emits a large amount of waste water and waste gas in the combustion process, which aggravates environmental pollution and greenhouse effect. Therefore, in order to realize sustainable development of human society, it is urgent to find a new energy technology. A Solid Oxide Fuel Cell (SOFC), which is an all-solid-state power generation device, can directly convert chemical energy in fuel into electric energy without being limited by the carnot cycle, and thus has very high energy conversion efficiency. With the development of cell thin film preparation technology, an electrode-supported SOFC is gradually becoming a hot point of research, and the greatest advantage of the electrode-supported SOFC compared with the traditional electrolyte support is that the thickness of the electrolyte can be reduced to 10-30 μm, thereby greatly reducing the ohmic resistance of the cell. However, the electrode-supported SOFC still has many problems in practical use, such as instability in an oxidation-reduction atmosphere, limited gas transport inside the electrode, and the like. In contrast, electrolyte-supported SOFCs are very stable under redox atmospheres and are not limited by electrode mass transfer processes. Therefore, it is necessary to design a battery structure to have both electrolyte supporting and electrode supporting advantages.
Disclosure of Invention
The invention aims to provide a composite YSZ electrolyte of a solid oxide fuel cell and a preparation method thereof, which can greatly reduce the ohmic resistance and the polarization resistance of the traditional electrolyte-supported SOFC cell and improve the output performance of a single cell.
In order to achieve the purpose, the invention adopts the following technical scheme:
a composite YSZ electrolyte of a solid oxide fuel cell is formed by sequentially laminating a first YSZ tape casting sheet, a second YSZ tape casting sheet and a first YSZ tape casting sheet; through holes are distributed in an array mode on the first YSZ casting sheet, and grooves are distributed in an array mode on the upper surface and the lower surface of the second YSZ casting sheet.
Further, the through holes are square through holes which are formed through a laser micromachining technology, wherein the size of each through hole is 0.5-1 mm, and the number of the through holes is 4-400; the grooves are circular grooves which are formed by a laser micromachining technology and have the size of 10-100 mu m and the number of 5000-20000.
Another object of the present invention is to provide a method for preparing the composite YSZ electrolyte, which comprises the following steps:
(1) preparing a YSZ electrolyte tape casting sheet by adopting a tape casting method:
(2) processing square through holes distributed in an array on a batch of YSZ electrolyte casting sheets as first YSZ casting sheets by a laser micromachining technology; processing the upper and lower surfaces of another YSZ electrolyte casting sheet into circular grooves distributed in an array to serve as a second YSZ casting sheet;
(3) sequentially overlapping and placing a first YSZ cast sheet, a second YSZ cast sheet and a first YSZ cast sheet together, and then pressurizing on a tablet press to obtain a YSZ electrolyte green sheet;
(4) and putting the YSZ electrolyte green sheet into a high-temperature furnace for calcining to prepare the SOFC electrolyte with the novel structure.
Further, the preparation process of the YSZ electrolyte casting sheet in the step (1) is as follows: mixing YSZ (yttria-stabilized zirconia) powder with triethanolamine, dissolving in mixed solution of alcohol and xylene, and ball-milling to obtain slurry; adding an organic additive into the slurry, adding alcohol and xylene, and continuing ball milling; then putting the YSZ slurry into a vacuum pump for vacuumizing and defoaming treatment; finally, casting the YSZ slurry subjected to bubble removal onto a polyester film, and drying to obtain a YSZ electrolyte casting sheet;
according to a further scheme, the mass ratio of alcohol to xylene in the mixed solution is 1: 1-3: 1;
the organic additive is one or more of polyvinyl butyral, polyethylene glycol, dibutyl phthalate and the like;
the vacuumizing and defoaming treatment time is 10-60 min;
the drying temperature is room temperature, and the drying time is 1-2 days.
Further, the thickness of the YSZ electrolyte tape-casting sheet in the step (1) is 100-150 μm.
In a further scheme, the pressure of the tablet press in the step (3) is 20-100 MPa, and the pressure maintaining time is 5-10 min.
In a further scheme, the calcining temperature in the step (4) is 1300-1600 ℃, and the calcining time is 1-5 h.
According to the invention, the second YSZ tape casting sheet with the groove on the surface is placed between the two first YSZ tape casting sheets with the through holes to form the SOFC electrolyte in a sandwich type lamination mode, wherein the through hole structure of the first YSZ tape casting sheet can ensure that the cell has enough mechanical strength while the thickness of the SOFC electrolyte is reduced, so that the ohmic resistance of the cell is reduced. The groove structure of the second YSZ tape-casting sheet can enlarge the interface area of the electrode-electrolyte, and provide more active reaction points for electrochemical reaction, thereby reducing the polarization resistance of the cell.
Therefore, the composite YSZ electrolyte not only can reduce the polarization resistance of the traditional electrolyte supported SOFC, but also can reduce the ohmic resistance of the cell under the condition of ensuring that the cell has enough mechanical strength; the output power of the single battery can be greatly improved, and the power assisting effect is provided for the commercialization process of the SOFC.
Drawings
FIG. 1 is a schematic diagram of the resolution of a composite YSZ electrolyte according to the invention;
FIG. 2 is an AC impedance spectrum at 800 ℃ in an open circuit state after four examples and comparative examples of the present invention are prepared as a single cell.
Detailed Description
In order to make the objects, technical solutions and advantageous technical effects of the present invention more clear, the present invention is further described in detail with reference to the following embodiments.
As shown in fig. 1, a composite YSZ electrolyte of a solid oxide fuel cell is formed by sequentially laminating a first YSZ cast sheet 1, a second YSZ cast sheet 3 and a first YSZ cast sheet 1; through holes 2 are arranged on the first YSZ casting sheet 1 in an array mode, and grooves 4 are arranged on the upper surface and the lower surface of the second YSZ casting sheet 3 in an array mode.
Further, the through holes 2 are square through holes which are formed through a laser micromachining technology, wherein the size of each through hole is 0.5-1 mm, and the number of the through holes is 4-400; the grooves 4 are circular grooves with the size of 10-100 mu m and the number of 5000-20000 formed by a laser micromachining technology.
The thickness of the first YSZ casting sheet 1 and the second YSZ casting sheet 3 is 100-150 μm.
The preparation process of the YSZ electrolyte tape-casting sheet of the invention is as follows: mixing YSZ (yttria-stabilized zirconia) powder with triethanolamine, and dissolving the mixture in alcohol and xylene in a mass ratio of 1: 1-3: 1, ball-milling the mixed solution into slurry; adding an organic additive into the slurry, adding alcohol and xylene, and continuing ball milling; then putting the YSZ slurry into a vacuum pump for vacuumizing and defoaming for 10-60 min; finally, casting the YSZ slurry subjected to bubble removal onto a polyester film, and drying for 1-2 days at room temperature to obtain a YSZ electrolyte casting sheet;
wherein the organic additive is one or more of polyvinyl butyral, polyethylene glycol, dibutyl phthalate and the like.
In a further scheme, the pressure of the tablet press in the step (3) is 20-100 MPa, and the pressure maintaining time is 5-10 min.
In a further scheme, the calcining temperature in the step (4) is 1300-1600 ℃, and the calcining time is 1-5 h.
Example 1:
a method for preparing a composite YSZ electrolyte, comprising the steps of:
(1) preparing a YSZ electrolyte tape casting sheet by adopting a tape casting method:
(2) cutting and processing a batch of YSZ electrolyte casting sheets into square through holes distributed in a 4 multiplied by 4 array by a laser micromachining technology, wherein the side length of each square through hole is 0.8mm, and the distance between every two adjacent through holes is 2.26mm, so that the square through holes are used as first YSZ casting sheets; the square via area accounts for 10% of the area of the first YSZ cast sheet.
Processing the upper and lower surfaces of another YSZ electrolyte casting sheet into circular grooves distributed in an array to serve as a second YSZ casting sheet;
(3) sequentially overlapping and placing a first YSZ cast sheet, a second YSZ cast sheet and a first YSZ cast sheet together, and then pressurizing to 50MPa on a tablet press and maintaining the pressure for 8min to obtain a YSZ electrolyte green sheet;
(4) and (3) putting the YSZ electrolyte green sheet into a high-temperature furnace to be calcined for 2 hours at 1500 ℃ to prepare the SOFC electrolyte with the novel structure.
Example 2:
a method for preparing a composite YSZ electrolyte, comprising the steps of:
(1) preparing a YSZ electrolyte tape casting sheet by adopting a tape casting method:
(2) cutting and processing a batch of YSZ electrolyte casting sheets into square through holes distributed in a 6 x 6 array by a laser micromachining technology, wherein the side length of each square through hole is 0.8mm, and the distance between every two adjacent through holes is 1.04mm, so that the square through holes are used as first YSZ casting sheets; the square via area accounted for 23% of the area of the first YSZ cast sheet.
Processing the upper and lower surfaces of another YSZ electrolyte casting sheet into circular grooves distributed in an array to serve as a second YSZ casting sheet;
(3) sequentially overlapping and placing a first YSZ cast sheet, a second YSZ cast sheet and a first YSZ cast sheet together, and then pressurizing to 20MPa on a tablet press and maintaining the pressure for 10min to obtain a YSZ electrolyte green sheet;
(4) and (3) putting the YSZ electrolyte green sheet into a high-temperature furnace to be calcined for 2 hours at 1500 ℃ to prepare the SOFC electrolyte with the novel structure.
Example 3:
a method for preparing a composite YSZ electrolyte, comprising the steps of:
(1) preparing a YSZ electrolyte tape casting sheet by adopting a tape casting method:
(2) cutting and processing a batch of YSZ electrolyte casting sheets into square through holes distributed in an 8 multiplied by 8 array by a laser micromachining technology, wherein the side length of each square through hole is 0.8mm, and the distance between every two adjacent through holes is 0.51mm, so that the square through holes are used as first YSZ casting sheets; the square via area accounted for 41% of the area of the first YSZ cast sheet.
Processing the upper and lower surfaces of another YSZ electrolyte casting sheet into circular grooves distributed in an array to serve as a second YSZ casting sheet;
(3) sequentially overlapping and placing a first YSZ cast sheet, a second YSZ cast sheet and a first YSZ cast sheet together, and then pressurizing to 100MPa on a tablet press and maintaining the pressure for 5min to obtain a YSZ electrolyte green sheet;
(4) and (3) calcining the YSZ electrolyte green sheet in a high-temperature furnace at 1300 ℃ for 5h to prepare the SOFC electrolyte with the novel structure.
Example 4:
a method for preparing a composite YSZ electrolyte, comprising the steps of:
(1) preparing a YSZ electrolyte tape casting sheet by adopting a tape casting method:
(2) cutting and processing a batch of YSZ electrolyte casting sheets into square through holes distributed in a 10 multiplied by 10 array by a laser micromachining technology, wherein the side length of each square through hole is 0.8mm, and the distance between every two adjacent through holes is 0.22mm, so that the square through holes are used as first YSZ casting sheets; the square via area accounted for 64% of the area of the first YSZ cast sheet.
Processing the upper and lower surfaces of another YSZ electrolyte casting sheet into circular grooves distributed in an array to serve as a second YSZ casting sheet;
(3) sequentially overlapping and placing a first YSZ cast sheet, a second YSZ cast sheet and a first YSZ cast sheet together, and then pressurizing to 80MPa on a tablet press and maintaining the pressure for 5min to obtain a YSZ electrolyte green sheet;
(4) and (3) putting the YSZ electrolyte green sheet into a high-temperature furnace to calcine for 1h at 1600 ℃ to prepare the SOFC electrolyte with the novel structure.
The same positive and negative electrode materials were coated on both sides of the SOFC electrolyte prepared in examples 1 to 5 and the electrolyte of the conventional structure, respectively, and the resulting product was calcined to obtain a single cell. The impedance of each single cell in an open circuit state is analyzed by electrochemical alternating current impedance spectroscopy (EIS), and the test temperature is 800 ℃. The test result is shown in fig. 2, the ohmic resistance of the single cell made of the SOFC electrolyte in the embodiment 1 of the present application at 800 ℃ is reduced by 4.15%, and the polarization resistance is reduced by 29.7%; the ohmic resistance of a single cell made of the SOFC electrolyte in the example 2 at 800 ℃ is reduced by 12.4 percent, and the polarization resistance is reduced by 32.7 percent; the ohmic resistance of a single cell made of the SOFC electrolyte in the example 3 at 800 ℃ is reduced by 24.4 percent, and the polarization resistance is reduced by 36.2 percent; the ohmic resistance of the single cell made of the SOFC electrolyte in example 4 was reduced by 40.9% at 800 ℃, and the polarization resistance was reduced by 45.3%. From the above analysis, the composite YSZ electrolyte prepared by the present invention greatly reduces the ohmic resistance and polarization resistance of the battery.
It is to be understood that the invention is not limited to the specific embodiments disclosed and described above, and that modifications and variations may be made thereto without departing from the scope of the invention as defined in the appended claims.
Claims (7)
1. A composite YSZ electrolyte for a solid oxide fuel cell, comprising: the composite YSZ electrolyte is formed by sequentially laminating a first YSZ tape casting sheet, a second YSZ tape casting sheet and a first YSZ tape casting sheet; through holes are distributed in an array mode on the first YSZ casting sheet, and grooves are distributed in an array mode on the upper surface and the lower surface of the second YSZ casting sheet;
the through holes are square through holes which are formed through a laser micromachining technology, have the size of 0.5-1 mm and are 4-400 in number; the grooves are circular grooves which are formed by a laser micromachining technology and have the size of 10-100 mu m and the number of 5000-20000.
2. The method of making a composite YSZ electrolyte according to claim 1, wherein: the method comprises the following steps:
(1) preparing a YSZ electrolyte tape casting sheet by adopting a tape casting method:
(2) processing square through holes distributed in an array on a batch of YSZ electrolyte casting sheets as first YSZ casting sheets by a laser micromachining technology; processing the upper and lower surfaces of another YSZ electrolyte casting sheet into circular grooves distributed in an array to serve as a second YSZ casting sheet;
(3) sequentially overlapping and placing a first YSZ cast sheet, a second YSZ cast sheet and a first YSZ cast sheet together, and then pressurizing on a tablet press to obtain a YSZ electrolyte green sheet;
(4) and putting the YSZ electrolyte green sheet into a high-temperature furnace for calcining to obtain the composite YSZ electrolyte.
3. The method of claim 2, wherein: the preparation process of the YSZ electrolyte tape-casting sheet in the step (1) is as follows: mixing YSZ powder and triethanolamine, dissolving in mixed solution of alcohol and xylene, and ball-milling to obtain slurry; adding an organic additive into the slurry, adding alcohol and xylene, and continuing ball milling; then putting the YSZ slurry into a vacuum pump for vacuumizing and defoaming treatment; finally, casting the YSZ slurry subjected to bubble removal onto a polyester film, and drying to obtain a YSZ electrolyte casting sheet;
the organic additive is one or more of polyvinyl butyral, polyethylene glycol and dibutyl phthalate.
4. The production method according to claim 3, characterized in that: the mass ratio of alcohol to xylene in the mixed solution is 1: 1-3: 1;
the vacuumizing and defoaming treatment time is 10-60 min;
the drying temperature is room temperature, and the drying time is 1-2 days.
5. The method of claim 2, wherein: the thickness of the YSZ electrolyte tape-casting sheet in the step (1) is 100-150 μm.
6. The method of claim 2, wherein: the pressure of the tablet press in the step (3) is 20-100 MPa, and the pressure maintaining time is 5-10 min.
7. The method of claim 2, wherein: the calcination temperature in the step (4) is 1300-1600 ℃, and the calcination time is 1-5 h.
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| CN114094123A (en) * | 2021-11-17 | 2022-02-25 | 合肥国轩高科动力能源有限公司 | Anode/electrolyte half cell, anode-supported solid oxide fuel cell and method for manufacturing the same |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1409427A (en) * | 2001-09-18 | 2003-04-09 | 中国科学技术大学 | PEN multilayer film of middle temperature solid oxide fuel cell and its producing method |
| CN101536235A (en) * | 2006-10-31 | 2009-09-16 | 康宁股份有限公司 | Micromachined electrolyte sheet, fuel cell devices utilizing such, and micromachining method for making fuel cell devices |
| CN103811789A (en) * | 2012-11-07 | 2014-05-21 | 中国科学院上海硅酸盐研究所 | Solid oxide fuel cell with symmetrical electrodes, and preparation method and application thereof |
| JP2016126884A (en) * | 2014-12-26 | 2016-07-11 | 株式会社日本触媒 | Electrolyte sheet for solid oxide fuel cell |
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| US6835488B2 (en) * | 2000-05-08 | 2004-12-28 | Honda Giken Kogyo Kabushiki Kaisha | Fuel cell with patterned electrolyte/electrode interface |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1409427A (en) * | 2001-09-18 | 2003-04-09 | 中国科学技术大学 | PEN multilayer film of middle temperature solid oxide fuel cell and its producing method |
| CN101536235A (en) * | 2006-10-31 | 2009-09-16 | 康宁股份有限公司 | Micromachined electrolyte sheet, fuel cell devices utilizing such, and micromachining method for making fuel cell devices |
| CN103811789A (en) * | 2012-11-07 | 2014-05-21 | 中国科学院上海硅酸盐研究所 | Solid oxide fuel cell with symmetrical electrodes, and preparation method and application thereof |
| JP2016126884A (en) * | 2014-12-26 | 2016-07-11 | 株式会社日本触媒 | Electrolyte sheet for solid oxide fuel cell |
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