CN115224335A - Solid-state oxidation galvanic pile and galvanic pile sealing method thereof - Google Patents

Solid-state oxidation galvanic pile and galvanic pile sealing method thereof Download PDF

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Publication number
CN115224335A
CN115224335A CN202210112908.6A CN202210112908A CN115224335A CN 115224335 A CN115224335 A CN 115224335A CN 202210112908 A CN202210112908 A CN 202210112908A CN 115224335 A CN115224335 A CN 115224335A
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China
Prior art keywords
main body
layer
body layer
preparing
galvanic pile
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CN202210112908.6A
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Chinese (zh)
Inventor
常晓辉
金斌斌
官万兵
杨钧
王建新
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Zhejiang Hydrogen Technology Co ltd
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Zhejiang Hydrogen Technology Co ltd
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Priority to CN202210112908.6A priority Critical patent/CN115224335A/en
Publication of CN115224335A publication Critical patent/CN115224335A/en
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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
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2404—Processes or apparatus for grouping fuel cells
    • 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
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0276—Sealing means characterised by their form
    • 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
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/028—Sealing means characterised by their material
    • H01M8/0282—Inorganic material
    • 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
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286—Processes for forming seals
    • 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
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/2425—High-temperature cells with solid electrolytes
    • 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

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  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Fuel Cell (AREA)

Abstract

The invention discloses a solid-state oxidation battery and a galvanic pile sealing method thereof, relating to the technical field of solid-state oxidation batteries and comprising the following steps of S1: preparing a mixed solution, namely adding a solvent into sealing material powder, wherein the sealing material powder comprises silicate glass, ceramic and composite material powder thereof, and preparing the solvent and the powder into the mixed solution through a mixing process; step S2: preparing slurry, and adding an additive into the mixed solution to prepare slurry; the use proportion of the additive is 4-27 wt%; and step S3: coating of the main body layer: coating a main body layer slurry by using a first connecting piece as a substrate through screen printing, wherein the thickness of the main body layer is 50-300 mu m, and the thickness of the main body layer is matched with that of the current collecting layer within a certain range; step S4; preparing a main body layer, namely performing a static pressure equal treatment method on the first connecting piece coated with the main body layer slurry to obtain the main body layer with the thickness of 50-300 mu m. When in use, good current collecting contact is formed, and meanwhile, micro sintering shrinkage is generated, so that the current collecting contact is further optimized.

Description

Solid-state oxidation galvanic pile and galvanic pile sealing method thereof
Technical Field
The invention relates to the technical field of solid oxide batteries, in particular to a solid oxide galvanic pile and a galvanic pile sealing method thereof.
Background
Generally, a solid oxide battery (SOC) is an energy conversion device that converts chemical energy in fuel into electrical energy through oxidation-reduction reaction to supply power to the outside, and also stores the electrical energy in the chemical fuel through electrolysis. A planar solid oxide fuel cell/electrolyser (SOFC/SOEC) is a typical SOC. Taking a thin plate type SOFC/SOEC and a flat tube type SOFC/SOEC as examples, the fuel cell mainly comprises an anode, an electrolyte and a cathode;
an SOFC/SOEC in the form of a thin plate, about 0.5mm thick anode support coated with a dense Yttria Stabilised Zirconia (YSZ) electrolyte layer, over which is coated a cathode layer of about 30 μm;
in the other, a flat tube SOFC/SOEC, the fuel gas channels run through an anode support of about 5mm thickness, which is coated with a dense Yttria Stabilised Zirconia (YSZ) electrolyte layer, over which is coated a cathode layer of about 30 μm;
in the power generation mode, for example, the two types of cells need to pass air to the cathode (white region) and fuel gas, such as hydrogen, to the anode (green region) during operation, so that the cathode and the anode need to be sealed respectively to ensure that the air and the fuel gas are confined in the cathode and the anode regions respectively for electrochemical reaction, and to prevent explosion caused by direct contact. Generally, since the SOC has a full ceramic or metal-ceramic composite structure and has a small amount of compressive deformation, the surface sealing of the negative and positive collectors is difficult due to the fluctuation of parameters such as thickness, flatness, warp degree and the like of the battery and the connector.
Meanwhile, the prior art mainly has the following defects:
1. is not suitable for batteries with poor deformability or low mechanical strength;
2. the battery has high manufacturing cost, high brittleness and easy damage;
3. the battery has complex manufacturing process, great difficulty and high cost;
4. conventional current collecting layers with high requirements on high-temperature compressibility of the current collecting layer and poor compressibility may result in poor current collecting contact. For the integration of the electric pile, the poor contact of local current collection can lead to the shortening of the service life and even the failure.
Disclosure of Invention
The invention aims to provide a solid-state oxidation galvanic pile and a galvanic pile sealing method thereof, which are used for solving the technical problems.
The technical scheme adopted by the invention is as follows:
a method of sealing a stack comprising the steps of:
step S1: preparing a mixed solution, namely adding a solvent into sealing material powder, wherein the sealing material powder comprises silicate glass, ceramic and composite material powder thereof, and preparing the mixed solution from the solvent and the powder through a mixing process;
step S2: preparing slurry, and adding an additive into the mixed solution to prepare slurry; the additive can be polyvinyl alcohol, polyvinyl pyrrolidone solution, polyvinyl butyral solution, ethyl cellulose solution or ethylene diamine tetraacetic acid solution, and the use ratio of the additive is 4-27 wt%;
and step S3: coating of the main body layer: coating a main body layer slurry by using a first connecting piece as a substrate through screen printing, or dispensing, or suspension coating, or physical deposition, or mould pressing, wherein the thickness of the main body layer is 50-300 mu m, and the thickness of the main body layer is matched with that of the current collecting layer in a certain range;
step S4; preparing a main body layer, namely air-drying, or dry-pressing, or static-pressing the first connecting piece coated with the main body layer slurry to obtain the main body layer with the thickness of 50-300 mu m;
step S5: preparing a modification layer, namely coating modification layer slurry on the main layer through screen printing, or dispensing, or suspension coating, or physical deposition; obtaining a second connecting piece by a preparation means;
step S6: preparing a battery unit; assembling the solid-state oxidation battery coated with the current collecting layer and a second connecting piece to obtain a pile integrated battery unit;
step S7: integrating the electric pile; the cell units are used as components to perform galvanic pile integration according to requirements, and the number of the galvanic pile units is 1-100 and can be adjusted;
step S8: sintering the integrated galvanic pile for 2-6 h at 700-850 ℃ to obtain the double-layer sealed galvanic pile unit.
In step 2, the shape of the decorative layer is preferably linear, parallel linear, cross linear, or S-shaped linear layer.
Preferably, the coating means in step S1 is screen printing, dispensing, suspension coating, physical deposition, thermal spraying, vapor deposition, or liquid deposition.
Preferably, the preparation method in step S3 is to air dry, dry press, or static press the main layer coated with the finishing layer slurry.
As further preferred, the mixing process may be roller ball milling, or planetary ball milling, or mechanical intervention stirring, or centrifugal stirring, or ultrasonic vibration stirring.
A solid oxide galvanic pile is prepared by the galvanic pile sealing method. As a further preference.
The technical scheme has the following advantages or beneficial effects:
in the invention, the battery has certain deformability, and the component errors are counteracted through deformation.
In the invention, the electrolyte sheet with the thickness of 200-300 mu m is used as a support body, so that the high-precision requirement and strict control of the thickness, the flatness and the warping tolerance are realized.
In the invention, in the production process of the battery, the electronic ceramic is adopted to directly seal the surface of the anode, and the fuel gas flow channel is sealed in the anode of the battery, so that the cathode does not need to be strictly sealed.
The structure of the invention mainly comprises a main body layer with negligible normal temperature compression deformation and a normal temperature compressible modification layer. The main body layer is coated on the battery or the connecting piece through methods such as screen printing, suspension coating, dispensing and the like to serve as a substrate, the thickness of the main body layer is matched with that of the current collecting layer, the modification layer is coated on the main body layer through methods such as dispensing, suspension coating and the like, and the thickness of the modification layer is matched with the comprehensive error of the element parameters. When the device is assembled at normal temperature, the modification layer is deformed under the action of the dead weight of the element component or external pressure to counteract the parameter error of the element component, and good current collection contact is formed at the same time. After high-temperature sintering, the densification of the main body layer achieves a good sealing effect, and simultaneously, trace sintering shrinkage is generated to further optimize current collection contact.
Drawings
Fig. 1 is a flow chart of a method of stack sealing of a solid oxide cell;
FIG. 2 is a first schematic diagram of a solid oxide cell according to the present invention;
fig. 3 is a schematic diagram of a solid oxide cell structure according to the present invention.
Fig. 4 is a schematic view of the structure of the stack of the present invention.
In the figure: 1. a solid state oxidation cell; 2. a cathode layer; 3. and (4) passing fuel gas.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention comprehensible, embodiments accompanied with figures are described in detail below.
In the description of the present invention, it should be understood that the terms "upper", "lower", "front", "rear", and the like indicate orientations or positional relationships based on the orientations or positional relationships shown in the drawings, and are only for convenience in describing the present invention and simplifying the description, but do not indicate or imply that the device or element referred to must have a specific orientation, be constructed in a specific orientation, and operate, and thus should not be construed as limiting the present invention.
The terms "first", "second" and "first" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one such feature.
Referring to fig. 1 to 3, a method for sealing a solid oxide cell stack includes the following steps:
step S1: preparing a mixed solution, namely adding a solvent into sealing material powder, wherein the sealing material powder comprises silicate glass, ceramic and composite material powder thereof, and preparing the solvent and the powder into the mixed solution through a mixing process;
step S2: preparing slurry, and adding an additive into the mixed solution to prepare slurry; the additive can be polyvinyl alcohol, polyvinyl pyrrolidone, polyvinyl butyral, ethyl cellulose, ethylene diamine tetraacetic acid and solution thereof, and the use proportion of the additive is 4-27 wt%;
and step S3: coating of the main body layer: coating the main body layer slurry by using a first connecting piece as a substrate through screen printing, or dispensing, or suspension coating, or physical deposition, or mould pressing and other methods, wherein the thickness of the main body layer is 50-300 mu m, and the thickness of the main body layer is matched with that of the current collecting layer in a certain range;
step S4; preparing a main body layer, namely performing air drying, dry pressing, isostatic pressing and other treatment methods on the first connecting piece coated with the main body layer slurry to obtain the main body layer with the thickness of 50-300 mu m
Step S5: preparing a modification layer, namely coating modification layer slurry on the main layer by screen printing, dispensing, suspension coating, physical deposition (including thermal spraying, vapor deposition and liquid deposition) and other methods; obtaining a second connecting piece through a certain preparation means;
step S6: preparing a battery unit; assembling the solid-state oxidation battery 1 coated with the current collecting layer and a second connecting piece to obtain a pile integrated battery unit;
step S7: integrating the electric pile; the cell units are used as components to perform galvanic pile integration according to requirements, and the number of the galvanic pile units is 1-100 and can be adjusted;
step S8: sintering the integrated galvanic pile for 2-6 h at 700-850 ℃ to obtain the double-layer sealed galvanic pile unit.
Further, as a preferred embodiment, in step 2, the shape of the decorative layer coating may be linear, parallel linear, cross linear, S-shaped linear, layered, etc.
Further, as a preferred embodiment, the step S of coating the main body layer includes: screen printing, dispensing, suspension coating, physical deposition (including thermal spraying, vapor deposition, liquid deposition), and the like.
Further, as a preferred embodiment, the preparation means in step S3 includes a processing method of air drying, dry pressing, isostatic pressing, etc. of the main layer coated with the slurry of the finishing layer.
Further, as a preferred embodiment, the mixing process may be roller ball milling, planetary ball milling, mechanical intervention type stirring, centrifugal type stirring, ultrasonic vibration stirring, etc.
A solid-state oxidation galvanic pile is prepared by any one of the galvanic pile sealing methods.
The first embodiment is as follows: coating the main body layer slurry by using a first connecting piece as a substrate through a screen printing method, wherein the thickness of the main body layer slurry is 100 mu m; air-drying the main layer product; coating an S-shaped linear modification layer on the main body layer by using the main body layer as a substrate through a suspension coating method; attaching and assembling the battery coated with the current collecting layer and a second connecting piece coated with a modification layer to obtain a galvanic pile integrated unit; the 'unit' is used as a component to carry out galvanic pile integration according to the requirement, and the number of the 'unit' is 20; and sintering the 5-cell or the electric pile at 800 ℃ for 3h to obtain the product.
In the second embodiment, the battery is used as a substrate, and the slurry of the main body layer is coated by a dispensing method, wherein the thickness of the slurry is 300 mu m; drying the main body layer product; coating a laminated modification layer on the main body layer by a screen printing method by taking the main body layer as a substrate; attaching and assembling the battery coated with the current collecting layer and a second connecting piece coated with a modification layer to obtain a galvanic pile integrated unit; the 'unit' is taken as a component to carry out galvanic pile integration according to the requirement, and the number of the 'unit' is 50; and sintering the 5-element battery or the electric pile for 6 hours at 750 ℃ to obtain the product.
Example three, a bulk layer was coated by thermal spraying on a first connector as a substrate to a thickness of 100 μm; air-drying the main body layer product; coating a parallel linear modification layer on the main body layer by using the main body layer as a substrate through a dispensing method; attaching and assembling the battery coated with the current collecting layer and the second connecting piece coated with the modification layer 5 to obtain a galvanic pile integrated galvanic pile unit; the galvanic pile units are used as element parts to carry out galvanic pile integration according to the needs, and the number of the galvanic pile units is 100; and sintering the 5-element battery or the electric pile at 800 ℃ for 2h to obtain the product.
Example four, a bulk layer was coated by vapor deposition on a cell substrate to a thickness of 60 μm;
drying the main layer product, and performing isostatic pressing for 60s under the pressure of 100 MPa; coating a double-S-shaped linear modification layer on the main body layer by using the main body layer as a substrate through a glue dispensing method; attaching and assembling the battery coated with the current collecting layer and the second connecting piece coated with the modification layer 5 to obtain a galvanic pile integrated galvanic pile unit; the galvanic pile units are taken as components to carry out galvanic pile integration according to the needs, and the number of the galvanic pile units is 40; and sintering the 5-cell or the electric stack at 750 ℃ for 4h to obtain the product.
While the invention has been described with reference to a preferred embodiment, it will be understood by those skilled in the art that various changes in form and detail may be made without departing from the spirit and scope of the invention.

Claims (6)

1. A method for sealing a galvanic pile is characterized by comprising the following steps:
step S1: preparing a mixed solution, namely adding a solvent into sealing material powder, wherein the sealing material powder comprises silicate glass, ceramic and composite material powder thereof, and preparing the mixed solution from the solvent and the powder through a mixing process;
step S2: preparing slurry, and adding an additive into the mixed solution to prepare slurry; the additive can be polyvinyl alcohol, polyvinyl pyrrolidone solution, polyvinyl butyral solution, ethyl cellulose solution or ethylene diamine tetraacetic acid solution, and the use ratio of the additive is 4-27 wt%;
and step S3: coating of the main body layer: coating a main body layer slurry on a first connecting piece serving as a substrate through screen printing, or dispensing, or suspension coating, or physical deposition, or mould pressing, wherein the thickness of the main body layer is 50-300 mu m, and the thickness of the main body layer is matched with that of the current collecting layer in a certain range;
step S4; preparing a main body layer, namely air-drying, or dry-pressing, or static-pressing the first connecting piece coated with the main body layer slurry to obtain the main body layer with the thickness of 50-300 mu m;
step S5: preparing a modification layer, namely coating modification layer slurry on the main layer through screen printing, or dispensing, or suspension coating, or physical deposition; obtaining a second connecting piece by a preparation means;
step S6: preparing a battery unit; assembling the solid-state oxidation battery coated with the current collecting layer and a second connecting piece to obtain a pile integrated battery unit;
step S7: integrating the electric pile; the cell units are used as components to perform galvanic pile integration according to requirements, and the number of the galvanic pile units is 1-100 and can be adjusted;
step S8: sintering the integrated galvanic pile for 2-6 h at 700-850 ℃ to obtain the double-layer sealed galvanic pile unit.
2. The stack sealing method according to claim 1, wherein in step 2, the modification layer is applied in a linear shape, a parallel linear shape, a cross linear shape, or an S-shaped linear layer shape.
3. The galvanic pile sealing method according to claim 1, wherein the coating means in step S1 is screen printing, dispensing, suspension coating, physical deposition, thermal spraying, vapor deposition, or liquid deposition.
4. The stack sealing method according to claim 1, wherein the preparing step S3 is to air dry, or dry press, or static press the main layer coated with the finishing layer slurry.
5. The method for sealing a galvanic pile according to claim 1, wherein the mixing process is roller ball milling, planetary ball milling, mechanical intrusive stirring, centrifugal stirring, or ultrasonic vibration stirring.
6. A solid oxide cell stack prepared by the cell stack sealing method according to any one of claims 1 to 5.
CN202210112908.6A 2022-01-29 2022-01-29 Solid-state oxidation galvanic pile and galvanic pile sealing method thereof Pending CN115224335A (en)

Priority Applications (1)

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CN202210112908.6A CN115224335A (en) 2022-01-29 2022-01-29 Solid-state oxidation galvanic pile and galvanic pile sealing method thereof

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Application Number Priority Date Filing Date Title
CN202210112908.6A CN115224335A (en) 2022-01-29 2022-01-29 Solid-state oxidation galvanic pile and galvanic pile sealing method thereof

Publications (1)

Publication Number Publication Date
CN115224335A true CN115224335A (en) 2022-10-21

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