CN109755616B - Hollow symmetrical structure double-cathode solid fuel cell with internal reforming characteristic and preparation method thereof - Google Patents
Hollow symmetrical structure double-cathode solid fuel cell with internal reforming characteristic and preparation method thereof Download PDFInfo
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention provides a hollow symmetrical structure double-cathode solid fuel cell with internal reforming characteristic and a preparation method thereof. The battery is characterized in that a hollow metal tube with holes in the tube wall is inserted into a hollow symmetrical solid oxide fuel battery, and the opening of the metal tube extends out of an anode layer, so that the anode current collecting area of the battery is increased, and the battery sealing at two sides of an anode is converted into the sealing of the metal tube, so that the sealing is easy; and the catalyst for reforming the natural gas is filled in the metal tube, and the natural gas can be introduced to reform, so that the reforming process is not independent of the cell reaction, the gas generated by reforming can be directly supplied to the cell, and the heat generated by the cell reaction can be directly supplied to reforming, thereby not only saving reforming equipment and heat exchange equipment which are independently equipped, but also greatly improving the use efficiency of the fuel and reducing the loss in the process.
Description
Technical Field
The invention relates to the technical field of ceramic electrolyte batteries, in particular to a hollow symmetrical structure double-cathode solid fuel battery with internal reforming characteristic and a preparation method thereof.
Background
The fuel gas which can be directly used by the solid oxide fuel cell is mainly hydrogen, carbon monoxide and other gases with reducing property, while the fuel gas which is used most in actual life is coal gas and natural gas, and the natural gas gradually replaces the coal gas to become the main domestic gas at present. The main components of natural gas are methane and a small amount of other low-carbon alkanes, which cannot be directly used for power generation of a fuel cell and can be used only after being converted into hydrogen and carbon monoxide through catalytic reforming. Therefore, when using natural gas as fuel gas, the conventional solid oxide fuel cell must be designed to prepare a reformer for reforming natural gas into hydrogen and carbon monoxide at high temperature, and the reformer is separated from the cell power generation system because the reforming process cannot be performed inside the cell due to the structure of the cell. Meanwhile, in order to fully utilize the high-temperature heat release characteristic of the fuel cell, a heat recovery system needs to be designed and prepared so as to improve the thermoelectric utilization efficiency of the fuel cell. The whole power generation system, the reforming device and the heat recovery device occupy large area, and have high consumption cost and high maintenance cost. In addition, heat generated by the power generation system needs to be led out and transferred through the device, and heat is lost in the transfer and transmission process, so that the heat recovery and utilization efficiency of the fuel cell is reduced.
Patent application No. CN201510104627.6 discloses a solid-state fuel cell supported by flat-plate electrodes, in which when the support electrode is an anode, the electrolyte and the barrier layer are symmetrically distributed on both sides of the cell substrate, the cathode layer is symmetrically distributed on both sides of the cell substrate, and the support electrode layer is provided with hollow channels for the transmission of fuel gas such as hydrogen. Compared with the traditional flat plate type anode support fuel cell, the cell with the structure has higher load strength and stronger oxidation and reduction resistance, and can ensure the integrity of the cell in the operation process; in addition, the hollow symmetrical structure gives the battery the advantage of easy sealing.
Disclosure of Invention
The invention discloses a solid fuel cell structure supported by a flat plate electrode, which is disclosed in the patent document with the patent application number of CN201510104627.6, and is improved to realize that the high-temperature reforming process of natural gas is carried out in the cell, so that the space and the cost can be saved, the energy consumption can be reduced, and the power generation efficiency of the cell can be improved.
The technical scheme of the invention is as follows: a double-cathode solid fuel cell with a hollow symmetrical structure and internal reforming characteristics is disclosed, wherein an anode layer is a support electrode layer, an electrolyte layer and a cathode layer are vertically stacked along the thickness direction, the electrolyte layer comprises a first electrolyte layer and a second electrolyte layer, the first electrolyte layer is positioned on the upper surface of the anode layer, and the second electrolyte layer is positioned on the lower surface of the anode; the cathode layer comprises a first cathode layer and a second cathode layer, the first cathode layer is positioned on the upper surface of the first electrolyte layer, and the second cathode layer is positioned on the lower surface of the second electrolyte layer; the method is characterized in that: the anode layer is internally provided with a hollow metal tube, the opening of the metal tube extends out of the anode layer, and the tube wall of the part of the metal tube positioned in the anode layer is provided with a plurality of holes.
When the natural gas reforming device is in a working state, the catalyst for reforming the natural gas is loaded into the metal pipe from the metal pipe opening, the natural gas is introduced into the metal pipe, the natural gas is reformed into fuel gas such as hydrogen gas, carbon monoxide gas and the like at the working temperature of the battery and under the condition of the catalyst, the fuel gas is diffused to the upper side and the lower side of the anode layer through holes in the metal pipe wall, electrochemical reaction is carried out between the fuel gas and oxidant gas introduced from the cathode at the three-phase interface of the electrode to generate electric energy and heat energy, the heat energy is continuously used for reforming the subsequent natural gas, the process of reforming discharge-heat release reforming can be continuously and repeatedly carried out along with the continuous introduction of the natural gas, and the direct use of the natural gas in the solid oxide fuel cell is indirectly realized by adopting the reforming mode.
As an implementation, the hollow metal tube comprises several, each metal tube being independent from the other and the orifice extending out of the anode layer. Preferably, the metal tubes are arranged parallel to each other.
As another way of realisation, the hollow metal tube forms a communicating channel inside the anode layer and has at least one metal spout protruding out of the anode layer.
The material of the metal tube is not limited, and comprises one or more of copper, nickel, iron, zinc and the like.
The catalyst for reforming the natural gas is not limited and comprises MgO-CaO-Ni/alpha-Al2O3、Ni/Ce-ZrO2/θ-Al2O3、Ni/γ-Al2O3And the like, or a mixture of two or more thereof.
The catalyst is made of porous materials, so that the transmission of gas in the metal tube cannot be influenced by the loading of the catalyst.
The electrolyte material is not limited, and includes YSZ, SSZ, LSGM and the like.
The anode material is not limited and comprises Ni-YSZ, LSM-YSZ, LSCF-YSZ or Cu-CeO2Etc.; when the thickness of the anode layer is increased, in order to maintain the fuel transmission effect, the anode layer material is preferably a material with high porosity, such as one or more of Ni-YSZ-C, NiO-SSZ, NiO-GDC, NiO-SDC, CuO-YSZ, etc. Preferably, the anode layer comprises a substrate anode layer and an active anode layer, the active anode layer comprises a first active anode layer and a second active anode layer, the first active anode layer is positioned on the upper surface of the substrate anode layer,the second active anode layer is positioned on the lower surface of the substrate anode layer, the first electrolyte layer is positioned on the surface of the first active anode layer, and the second electrolyte layer is positioned on the surface of the second active anode layer.
The cathode material is not limited and includes LSM, LSCF, BSFC, etc.
Preferably, the first electrolyte layer and the second electrolyte layer are symmetrically distributed around the anode layer, that is, the shapes, thicknesses, and the like of the first electrolyte layer and the second electrolyte layer are completely consistent.
Preferably, the first cathode layer and the second cathode layer are symmetrically distributed with the anode layer as the center, that is, the shapes, thicknesses, and the like of the first cathode layer and the second cathode layer are completely consistent.
When the thickness of the anode layer is increased, in order to maintain the fuel transmission effect, the anode layer material is preferably a material with high porosity, such as porous NiO-YSZ, LSM, LSCF and the like, and the porosity is preferably more than 50%.
The invention also provides a method for preparing the hollow symmetrical structure double-cathode solid fuel cell with the internal reforming characteristic, which comprises the following steps:
(1) preparing a half cell with a pore structure
Taking an anode material as a raw material, burying a high-temperature volatile object with a certain shape as a pore-forming object, and obtaining a battery substrate by a forming technology; preparing electrolyte layers on the upper surface and the lower surface of a battery matrix respectively by coating, dipping, screen printing and other methods, and then sintering to obtain a half battery comprising a first electrolyte layer and a second electrolyte layer; preparing a first non-support electrode layer on the upper surface of the first electrolyte layer by adopting methods such as coating, dipping and screen printing, preparing a second non-support electrode layer on the lower surface of the second electrolyte layer by adopting methods such as coating, dipping and screen printing, and sintering to obtain a half cell comprising a first cathode layer and a second cathode layer;
in the sintering process, volatilizing the pore-forming object to obtain a pore channel in the shape of the pore-forming object, wherein the pore channel is provided with an opening end on the side surface of the support electrode layer;
(2) a hollow metal pipe is inserted into the pore channel, the opening of the metal pipe extends out of the pore channel, the surface of the hollow metal pipe is matched with the inner surface of the pore channel and can be matched in the pore channel, and a plurality of holes are formed in the pipe wall of the part of the metal pipe positioned in the anode layer.
Preferably, in the step (1), the cathode buffer layer is prepared on the upper surface of the first cathode layer and the lower surface of the second cathode layer by coating, dipping, screen printing and the like, and is used for buffering and collecting current without sintering.
The material of the pore-forming object is not limited, and includes carbon rods, carbon materials with other shapes such as graphite, carbon nanotubes and the like.
The molding method is not limited, and includes hot pressing, casting and the like.
In summary, the metal tube with the hollow holes in the wall is inserted into the hollow symmetrical solid oxide fuel cell, and the invention has the following advantages:
(1) on one hand, the current collecting area of the anode of the hollow symmetrical solid oxide fuel cell is increased, and on the other hand, the cell sealing on the two sides of the anode is converted into the sealing of the metal tube, so that the sealing is easier to carry out.
(2) The hollow symmetrical solid oxide fuel cell with the structure can directly use natural gas, a catalyst for reforming the natural gas is filled in the metal tube, and reforming can be carried out after the natural gas is introduced, so that the reforming process is not independent of cell reaction any more, but the natural gas and the catalyst are combined into a whole, on one hand, reforming equipment and heat exchange equipment which are required to be independently equipped for the existing solid oxide fuel cell are omitted, on the other hand, gas generated by reforming is directly supplied to the cell, heat generated by cell reaction is directly supplied to reforming, the use efficiency of the fuel is greatly improved, and the loss in the process is reduced.
(3) The hollow metal pipe is inserted into the pore canal, so that the surface of the hollow metal pipe is matched with the inner surface of the pore canal and can be inosculated in the pore canal, and the metal pipe can be effectively protected when being stressed.
Drawings
Fig. 1 is a schematic side view of a hollow symmetric double cathode solid state fuel cell according to example 1 of the present invention;
fig. 2 is a schematic top view of a double-cathode solid-state fuel cell of hollow symmetrical structure according to example 1 of the present invention;
fig. 3 is a schematic structural view of the metal pipe in fig. 2.
Detailed Description
The invention will be described in further detail below with reference to the embodiments of the drawing, which are intended to facilitate the understanding of the invention and are not intended to limit the invention in any way.
The reference numerals in fig. 1-3 are: 3-metal tube, 20-anode layer, 21-first electrolyte layer, 22-second electrolyte layer, 31-first cathode layer, 32-second cathode layer and 33-holes of metal tube wall.
Example 1:
in this embodiment, a schematic structural diagram of a hollow symmetric dual-cathode solid-state fuel cell is shown in fig. 2, where an anode layer is a supporting electrode layer, an electrolyte layer and a cathode layer are stacked up and down along a thickness direction, the electrolyte layer includes a first electrolyte layer and a second electrolyte layer, the first electrolyte layer is located on an upper surface of the anode layer, and the second electrolyte layer is located on a lower surface of the anode; the cathode layer comprises a first cathode layer and a second cathode layer, the first cathode layer is positioned on the upper surface of the first electrolyte layer, and the second cathode layer is positioned on the lower surface of the second electrolyte layer; as shown in fig. 2 and 3, a hollow metal tube is disposed inside the anode layer, the metal tube is made of copper, a metal tube opening extends out of the anode layer, and a plurality of holes are disposed on a tube wall of the metal tube portion inside the anode layer.
In this embodiment, the hollow metal tubes include a plurality of metal tubes, each of the metal tubes is independent of the other metal tubes, and the tube openings extend out of the anode layer, and the metal tubes are arranged in parallel at intervals.
In this embodiment, the electrolyte material may be YSZ, SSZ, LSGM, or the like.
In this embodiment, the anode material may be Ni-YSZ, LSM-YSZ, LSCF-YSZ, or Cu-CeO2Etc.; when the thickness of the anode layer is increased, in order to maintain the fuel transmission effect, the anode layer material is preferably made of a material with higher porosity, such as Ni-YSZ-CNiO-SSZ, NiO-GDC, NiO-SDC, CuO-YSZ, and the like.
The anode layer comprises a substrate anode layer and an active anode layer, the active anode layer comprises a first active anode layer and a second active anode layer, the first active anode layer is positioned on the upper surface of the substrate anode layer, the second active anode layer is positioned on the lower surface of the substrate anode layer, the first electrolyte layer is positioned on the surface of the first active anode layer, and the second electrolyte layer is positioned on the surface of the second active anode layer.
In this embodiment, the cathode material may be LSM, LSCF, BSFC, or the like.
In this embodiment, the first electrolyte layer and the second electrolyte layer are symmetrically distributed with the anode layer as the center, that is, the shapes, thicknesses, and the like of the first electrolyte layer and the second electrolyte layer are completely consistent.
In this embodiment, the anode layer is used as a center, and the first cathode layer and the second cathode layer are symmetrically distributed, that is, the shapes, thicknesses, and the like of the first cathode layer and the second cathode layer are completely the same.
The preparation method of the hollow symmetrical structure double-cathode solid fuel cell comprises the following steps:
(1) preparing a half cell with a pore structure
Taking an anode material as a raw material, burying a carbon rod in the anode material, and obtaining a battery matrix through a forming technology; preparing electrolyte layers on the upper surface and the lower surface of a battery matrix respectively by coating, dipping, screen printing and other methods, and then sintering to obtain a half battery comprising a first electrolyte layer and a second electrolyte layer; preparing a first non-support electrode layer on the upper surface of the first electrolyte layer by adopting methods such as coating, dipping and screen printing, preparing a second non-support electrode layer on the lower surface of the second electrolyte layer by adopting methods such as coating, dipping and screen printing, and sintering to obtain a half cell comprising a first cathode layer and a second cathode layer;
in the sintering process, volatilizing the carbon rods to obtain a pore canal with a carbon rod shape, wherein the pore canal is provided with an opening end on the side surface of the support electrode layer;
(2) a hollow metal pipe is inserted into the pore channel, the opening of the metal pipe extends out of the pore channel, the surface of the hollow metal pipe is matched with the inner surface of the pore channel and can be matched in the pore channel, and a plurality of holes are arranged on the pipe wall of the part of the metal pipe positioned in the anode layer.
Preferably, in the step (1), the cathode buffer layer is prepared on the upper surface of the first cathode layer and the lower surface of the second cathode layer by coating, dipping, screen printing and the like, and is used for buffering and collecting current without sintering.
Catalysts for reforming natural gas, e.g. MgO-CaO-Ni/alpha-Al, in operation2O3、Ni/Ce-ZrO2/θ-Al2O3、Ni/γ-Al2O3And loading the natural gas into the metal pipe from the metal pipe opening and introducing the natural gas into the metal pipe. Because the catalyst is made of porous materials, the loading of the catalyst does not influence the transmission of gas. The natural gas is reformed into fuel gas such as hydrogen, carbon monoxide gas and the like at the working temperature of the cell and under the condition of a catalyst, the fuel gas is diffused to the upper side and the lower side of the anode layer through holes of the metal tube wall, electrochemical reaction is carried out between the fuel gas and oxidant gas introduced from the cathode at the three-phase interface of the electrode to generate electric energy and heat energy, the heat energy is continuously used for reforming the subsequent natural gas, the process of 'reforming discharge-heat release reforming' can be continuously and repeatedly carried out along with the continuous introduction of the natural gas, and the direct use of the natural gas in the solid oxide fuel cell is indirectly realized by adopting the reforming mode.
Example 2:
in this example, the structure of a hollow symmetrical double-cathode solid fuel cell is basically the same as that of the cell in example 1, except that a cathode buffer layer is provided on the upper surface of the first cathode layer and the lower surface of the second cathode layer for buffering and current collection.
The preparation method of the hollow symmetrical structure double-cathode solid fuel cell is basically the same as that in the embodiment 1, except that in the step (1), the cathode buffer layer is prepared on the upper surface of the first cathode layer and the lower surface of the second cathode layer by adopting the methods of coating, dipping, screen printing and the like, and the layer is used for buffering and current collection and does not need to be sintered.
Catalysts for reforming natural gas, e.g. MgO-CaO-Ni/alpha-Al, in operation2O3、Ni/Ce-ZrO2/θ-Al2O3、Ni/γ-Al2O3And loading the natural gas into the metal pipe from the metal pipe opening and introducing the natural gas into the metal pipe. Because the catalyst is made of porous materials, the loading of the catalyst does not influence the transmission of gas. The natural gas is reformed into fuel gas such as hydrogen, carbon monoxide gas and the like at the working temperature of the cell and under the condition of a catalyst, the fuel gas is diffused to the upper side and the lower side of the anode layer through holes of the metal tube wall, electrochemical reaction is carried out between the fuel gas and oxidant gas introduced from the cathode at the three-phase interface of the electrode to generate electric energy and heat energy, the heat energy is continuously used for reforming the subsequent natural gas, the process of 'reforming discharge-heat release reforming' can be continuously and repeatedly carried out along with the continuous introduction of the natural gas, and the direct use of the natural gas in the solid oxide fuel cell is indirectly realized by adopting the reforming mode.
Example 3:
in this embodiment, a structure of a hollow symmetric dual-cathode solid fuel cell is substantially the same as that of the cell in embodiment 1, except that the anode layer includes a substrate anode layer and an active anode layer, the active anode layer includes a first active anode layer and a second active anode layer, the first active anode layer is located on the upper surface of the substrate anode layer, the second active anode layer is located on the lower surface of the substrate anode layer, the first electrolyte layer is located on the surface of the first active anode layer, and the second electrolyte layer is located on the surface of the second active anode layer.
The preparation method of the hollow symmetrical structure double-cathode solid fuel cell is basically the same as that in the example 1, except that in the step (1), the active anode layer and the electrolyte layer are respectively prepared on the upper surface and the lower surface of the cell substrate by coating, dipping, screen printing and the like, and then sintered.
Catalysts for reforming natural gas, e.g. MgO-CaO-Ni/alpha-Al, in operation2O3、Ni/Ce-ZrO2/θ-Al2O3、Ni/γ-Al2O3And loading the natural gas into the metal pipe from the metal pipe opening and introducing the natural gas into the metal pipe. Because the catalyst is made of porous materials, the loading of the catalyst does not influence the transmission of gas. In the electricityThe natural gas is reformed into fuel gas such as hydrogen, carbon monoxide gas and the like at the working temperature of the cell and under the condition of a catalyst, the fuel gas is diffused to the upper side and the lower side of the anode layer through holes of the metal tube wall, electrochemical reaction is carried out between the fuel gas and oxidant gas introduced from the cathode at the three-phase interface of the electrode to generate electric energy and heat energy, the heat energy is continuously used for reforming the subsequent natural gas, the process of 'reforming discharge-heat release reforming' can be continuously and repeatedly carried out along with the continuous introduction of the natural gas, and the direct use of the natural gas in the solid oxide fuel cell is indirectly realized by adopting the reforming mode.
The above embodiments are provided to explain the technical solutions of the present invention in a detailed manner, and it should be understood that the above examples are only specific embodiments of the present invention, and are not intended to limit the present invention. Any modification, addition or equivalent substitution made within the scope of the present invention shall be included within the protection scope of the present invention.
Claims (8)
1. A preparation method of a double-cathode solid fuel cell with a hollow symmetrical structure and internal reforming characteristics is disclosed, wherein an anode layer is a support electrode layer, an electrolyte layer and a cathode layer are vertically stacked along the thickness direction, the electrolyte layer comprises a first electrolyte layer and a second electrolyte layer, the first electrolyte layer is positioned on the upper surface of the anode layer, and the second electrolyte layer is positioned on the lower surface of the anode layer; the cathode layer comprises a first cathode layer and a second cathode layer, the first cathode layer is positioned on the upper surface of the first electrolyte layer, and the second cathode layer is positioned on the lower surface of the second electrolyte layer; the method is characterized in that: the anode layer is internally provided with a hollow metal tube, the opening of the metal tube extends out of the anode layer, and the tube wall of the metal tube part positioned in the anode layer is provided with a plurality of holes;
the method comprises the following steps:
(1) preparing a half cell with a pore structure
Taking an anode material as a raw material, burying a high-temperature volatile object with a certain shape as a pore-forming object, and obtaining a battery substrate by a forming technology; preparing electrolyte layers on the upper surface and the lower surface of a battery matrix by coating, dipping and screen printing methods respectively, and then sintering to obtain a half battery comprising a first electrolyte layer and a second electrolyte layer; preparing a first non-support electrode layer on the upper surface of the first electrolyte layer by adopting a coating, dipping and screen printing method, preparing a second non-support electrode layer on the lower surface of the second electrolyte layer by adopting a coating, dipping and screen printing method, and sintering to obtain a half cell comprising a first cathode layer and a second cathode layer;
in the sintering process, volatilizing the pore-forming object to obtain a pore channel in the shape of the pore-forming object, wherein the pore channel is provided with an opening end on the side surface of the support electrode layer;
(2) a hollow metal pipe is inserted into the pore channel, the opening of the metal pipe extends out of the pore channel, the surface of the hollow metal pipe is matched with the inner surface of the pore channel and can be matched in the pore channel, and a plurality of holes are arranged on the pipe wall of the part of the metal pipe positioned in the anode layer;
when the natural gas reforming device is in a working state, the catalyst for reforming the natural gas is loaded into the metal pipe from the metal pipe opening, natural gas is introduced into the metal pipe, and the natural gas is reformed into fuel gas at the working temperature of the battery and under the condition of the catalyst.
2. The method of claim 1, wherein: the fuel gas is hydrogen gas or carbon monoxide gas.
3. The method of claim 1, wherein: the hollow metal tube includes a plurality of metal tubes, each of which is independent of the other and has a nozzle extending out of the anode layer.
4. The method of claim 3, wherein: the metal tubes are arranged parallel to each other.
5. The method of claim 1, wherein: the hollow metal tube forms a communication channel inside the anode layer and has at least one metal tube orifice extending out of the anode layer.
6. The method of claim 1, wherein: the metal tube is made of one or more of copper, nickel, iron and zinc.
7. The method of claim 1, wherein: the catalyst for reforming natural gas comprises MgO-CaO-Ni/alpha-Al2O3、Ni/Ce-ZrO2/θ- Al2O3、Ni/γ- Al2O3One or a mixture of two or more of them.
8. The method of claim 1, wherein: in the step (1), the cathode buffer layer is prepared on the upper surface of the first cathode layer and the lower surface of the second cathode layer by a coating, dipping or screen printing method.
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| WO2021262219A1 (en) * | 2020-06-25 | 2021-12-30 | Shell Oil Company | Exhaust gas emissions abatement system |
| CN113381048B (en) * | 2021-05-28 | 2022-11-11 | 山东工业陶瓷研究设计院有限公司 | Solid oxide fuel cell and preparation method thereof |
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| CN105161743A (en) * | 2015-10-14 | 2015-12-16 | 中国科学院宁波材料技术与工程研究所 | Anode of high-temperature solid-state fuel cell and cell stack unit |
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