CN107634229B - Membrane electrode for fuel cell stack - Google Patents
Membrane electrode for fuel cell stack Download PDFInfo
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- CN107634229B CN107634229B CN201710709684.6A CN201710709684A CN107634229B CN 107634229 B CN107634229 B CN 107634229B CN 201710709684 A CN201710709684 A CN 201710709684A CN 107634229 B CN107634229 B CN 107634229B
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- Y02E60/30—Hydrogen technology
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Abstract
A membrane electrode for a fuel cell stack, the membrane electrode comprising: a cathode catalyst layer, a perfluorosulfonic acid membrane and an anode catalyst layer; a metal organic framework material is added in the membrane electrode catalyst layer, and the metal organic framework material has a hollow spherical structure and can improve the porosity of the catalyst layer. The metal organic framework material has high proton conductivity and can provide certain moisture retention capability for the catalytic layer. The membrane electrode for the proton exchange membrane fuel cell stack provided by the invention can improve the performance of the stack, improve the adaptability of the stack in dry weather and improve the energy density of the stack. Meanwhile, the consumption of the noble metal catalyst is reduced by improving the reaction activity of the catalyst layer, and the cost of the galvanic pile is greatly reduced.
Description
Technical Field
The invention belongs to the technical field of fuel cells, relates to a fuel cell stack, and particularly relates to a membrane electrode for the fuel cell stack.
Background
The proton exchange membrane fuel cell is a novel clean energy conversion device with high efficiency, environmental protection, no pollution and zero emission. Can be widely applied to the industries of aviation, war industry, traffic, civil use and the like.
The device adopts hydrogen as fuel and air containing oxygen as oxidant. The hydrogen gas is oxidized at the anode catalytic layer side of the membrane electrode, electrons are lost and become protons, the electrons are transmitted to the cathode catalytic layer side of the membrane electrode through an external circuit, and the protons are transmitted to the cathode catalytic layer through a proton exchange membrane of the membrane electrode. The oxygen is subjected to reduction reaction by electrons transmitted from an external circuit on the cathode catalytic layer side of the membrane electrode, and is combined with protons transmitted from the anode through the proton exchange membrane to generate water. The membrane electrode is used as a place for chemical reaction, and the material performance, the composition ratio and the structure of the membrane electrode have obvious influence on the membrane electrode performance.
However, the existing membrane electrode has poor performance, weak adaptability and low energy density. In view of the above, there is an urgent need to design a new membrane electrode to overcome the above-mentioned defects of the existing membrane electrode.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: the membrane electrode for fuel cell stack can raise the performance of the stack, raise the adaptability of the stack in dry weather and raise the energy density of the stack.
In order to solve the technical problems, the invention adopts the following technical scheme:
a membrane electrode for a fuel cell stack, the membrane electrode comprising: the device comprises a cathode catalyst layer, a perfluorosulfonic acid membrane and an anode catalyst layer, wherein a metal organic framework material is added into the anode catalyst layer and the cathode catalyst layer;
quantitative metal organic framework materials are added in the cathode catalyst layer, and the metal organic framework materials can improve the mesoporous porosity of the cathode catalyst layer in the cathode catalyst layer, so that reaction gas can enter the catalyst layer for reaction;
quantitative organic framework materials are added in the anode catalyst layer, and the metal organic framework materials can improve the anode moisture retention performance and reduce the proton transfer resistance in the anode catalyst layer;
the addition amounts of the metal organic framework materials in the cathode catalyst layer and the anode catalyst layer are different; or, the metal organic framework material is not added into the anode catalyst layer, and only the metal organic framework material is added into the cathode catalyst layer;
the membrane electrode can be used for pretreating the metal organic framework material before adding the metal organic framework material into the catalyst layer, but the physical structure of the metal organic framework material is not changed by the pretreatment; the purpose of this pretreatment is to improve the conductivity of the metal organic framework material;
the membrane electrode does not need to be pretreated before the metal organic framework material is added into the catalyst layer, and the unsaturated metal of the metal organic framework material provides an active site energy which can efficiently adsorb toxic carbon monoxide in reaction gas and provides the membrane electrode with anti-poisoning capability;
the metal organic framework materials of the membrane electrode are respectively reduced in gradient in the catalytic layer, and the distribution of the metal organic framework materials on the side close to the gas diffusion layer is higher than the density of the metal organic framework materials on the side close to the proton exchange membrane;
the metal organic framework material of the membrane electrode is added into the slurry according to the proportion of 0.5 to 10 percent of the catalyst and the binder, and is uniformly mixed and then coated on the surface of the perfluorosulfonic acid membrane;
the concentration of the slurry adopting the spraying mode is lower than that of the slurry adopting the blade coating mode;
and obtaining uniform slurry by adopting an ultrasonic dispersion mode or obtaining uniform slurry by adopting a ball milling mode.
A membrane electrode for a fuel cell stack, the membrane electrode comprising: the proton exchange membrane comprises a cathode catalyst layer, an anode catalyst layer and a proton exchange membrane, wherein a metal organic framework material is added in the cathode catalyst layer and the anode catalyst layer;
the metal organic framework material has a hollow-out-like spherical structure and mesoporous channels of 2nm to 4 nm.
The metal organic framework material has sulfonic acid groups, and has good proton conductivity and certain moisture retention capacity;
the metal organic framework material is added into the catalyst layer according to the proportion of 2.5 percent of the total amount of the catalyst layer substances;
the metal organic framework material can be sulfonated MIL-101;
the metal organic framework material is firstly mixed with a catalyst, and then a binder and a solvent are added for ultrasonic dispersion or ball milling to obtain uniformly dispersed catalyst slurry;
the cathode catalyst slurry can be divided into A, B two parts, wherein, part A is not added with metal organic framework materials, and part B is added with metal organic framework materials;
the cathode catalyst slurry may not be divided into A, B two parts;
the cathode catalyst slurry is sequentially coated on one side of a proton exchange membrane, the part A is coated on one side of the proton exchange membrane, and the part B is coated on the coating of the part A after drying;
the catalyst ratio in the cathode catalyst slurry A, B portion is between 2:1 and 5: 1;
the anode catalyst slurry can be divided into A, B parts, wherein, part A is not added with metal organic framework materials, and part B is added with metal organic framework materials;
the anode catalyst slurry may not be divided into A, B two parts;
the anode catalyst slurry is sequentially coated on one side of a proton exchange membrane, the part A is coated on one side of the proton exchange membrane, and the part B is coated on the coating of the part A after drying;
the catalyst ratio in the anode catalyst slurry A, B portion is between 2:1 and 5: 1.
A membrane electrode for a proton exchange membrane fuel cell stack, the membrane electrode comprising: the metal-organic composite membrane comprises a cathode catalyst layer, a perfluorosulfonic acid membrane and an anode catalyst layer, wherein a metal-organic framework material is added into the anode catalyst layer and the cathode catalyst layer.
In a preferred embodiment of the present invention, a metal organic framework material is added to the anode catalyst layer.
In a preferred embodiment of the present invention, a metal organic framework material is added to the cathode catalyst layer.
In a preferred embodiment of the present invention, the anode catalyst layer is divided into two layers, and the catalyst layer near the gas diffusion layer is added with a metal-organic framework material and is not added near the proton exchange membrane.
In a preferred embodiment of the present invention, the cathode catalyst layer is divided into two layers, and the catalyst layer near the gas diffusion layer is added with a metal-organic framework material, but not near the proton exchange membrane.
As a preferred scheme of the invention, the preparation of the catalyst slurry adopts an ultrasonic dispersion or ball milling mode.
The membrane electrode serves as a chemical reaction site for energy conversion of the fuel cell, and a reduction reaction occurs in the cathode catalyst layer and an oxidation reaction occurs in the anode catalyst layer. Hydrogen is oxidized in the anode catalyst layer to lose electrons and then becomes protons, and the protons are transferred to the cathode catalyst layer side through the perfluorosulfonic acid membrane; the oxygen gets electrons in the cathode catalyst layer which are transferred by an external circuit and are reduced to be combined with the protons transferred from the anode to become water. The chemical reaction is generated in a solid-liquid-gas three-phase region, so that the catalyst layer needs to be provided with an electronic channel, a proton transmission channel and a gas transmission channel at the same time. Part of the way to increase these active sites in the solid-liquid-gas three-phase region is to increase the number of channels.
The preparation of the membrane electrode catalyst layer generally has two forms, one is that the membrane electrode catalyst layer is coated on a gas diffusion layer and then is hot-pressed with a proton exchange membrane; firstly, the membrane is coated on a proton exchange membrane and then is pressed with a gas diffusion layer. The coating process generally comprises three modes of blade coating, silk screen printing and spraying.
In order to make the catalytic layer porous, it is common to apply the catalytic layer in batches and in many times, but the coating time increases and the production efficiency decreases.
By adding the pore-forming agent into the catalyst layer, the catalyst is generally damaged by volatile gas generated after the pore-forming agent is decomposed, or residual inorganic ions after decomposition occupy the position of protons on the sulfonic acid group, and the residual inorganic ions need to be cleaned, so that the process is complicated.
The lateral conductivity of the catalyst layer can be improved by adding graphene into the catalyst layer, and the catalyst layer does not contribute to porosity.
The invention has the beneficial effects that: the membrane electrode for the fuel cell stack can increase energy density, and improve energy conversion efficiency and stack performance; the method is favorable for improving the gas transmission capacity in the catalyst layer of the membrane electrode, guiding the excessive water generated by the cathode to permeate into the anode to improve the water management capacity of the membrane electrode, and the added sulfonic acid group of the metal organic framework material can serve as a proton transfer channel. The invention is helpful to solve the problems of large gas diffusion resistance inside the catalyst layer and untimely material transmission under the condition of large current, and reduces concentration polarization. Compared with the existing membrane electrode design, the method is beneficial to improving the performance of the galvanic pile, reducing the gas back pressure and improving the energy density of the galvanic pile.
Because the gas diffusion speed of the traditional fuel cell bipolar plate is too low under the condition of large current, concentration polarization is easy to occur, the power is too low, and the like, the limit current is small, the long-time constant current discharge is difficult, and the like.
In contrast, the membrane electrode of the present disclosure improves catalytic layer microporosity, wherein the simultaneous addition of metal organic framework materials can improve water transport capacity and improve water management. The reactant gas can be uniformly dispersed within the catalytic layer to help provide fuel cell stack efficiency and provide power density. The consumption of the platinum catalyst in the catalyst layer can be reduced, and the cost of the galvanic pile is greatly reduced.
Drawings
FIG. 1 is a schematic diagram of a membrane electrode dual-catalyst layer structure.
FIG. 2 is a schematic diagram of a single catalytic layer structure of a membrane electrode.
FIG. 3 is a partial schematic view of a membrane electrode catalyst layer.
Detailed Description
Preferred embodiments of the present invention will be described in detail below with reference to the accompanying drawings.
Example one
Referring to fig. 1, the present invention discloses a membrane electrode for a fuel cell stack, the membrane electrode comprising: the cathode catalysis layer and the anode catalysis layer are added with hollow metal organic framework materials to enhance the gas transmission capability of the catalysis layer and enhance the water management capability of the catalysis layer.
In fig. 1, a metal-organic framework material 1 and a catalyst 2 are distributed on the near-gas diffusion layer side of the catalytic layer by a binder 3.
In fig. 1, a catalyst 2 is distributed on the catalytic layer near the perfluorosulfonic acid membrane 4 side by a binder 3.
Example two
Referring to fig. 2, the present invention discloses a membrane electrode for a fuel cell stack, the membrane electrode comprising: the cathode catalysis layer and the anode catalysis layer are added with hollow metal organic framework materials to enhance the gas transmission capability of the catalysis layer and enhance the water management capability of the catalysis layer.
In fig. 2, the metal-organic framework material 1a and the catalyst 2a are uniformly distributed on the perfluorosulfonic acid membrane side 4a via the binder 3 a.
In fig. 3, the metal-organic framework material 1b and the catalyst 2b are uniformly distributed on the perfluorosulfonic acid membrane side 4b through the binder 3 b. The reaction gas can diffuse to the catalyst in the inner layer through the hollow metal organic framework material pore channel to participate in the reaction.
In summary, the membrane electrode for a proton exchange membrane fuel cell stack provided by the invention can improve the gas transmission efficiency of the catalyst layer and improve the water management capability of the catalyst layer, thereby reducing the consumption of the noble metal catalyst in the catalyst layer and reducing the cost of the fuel cell stack due to the energy conversion efficiency and the performance of the fuel cell stack. The invention is helpful to solve the problems of difficult reaction gas transmission and difficult water management of the membrane electrode catalyst layer of the fuel cell. Compared with the existing membrane electrode preparation scheme, the method is beneficial to improving the performance of the fuel cell stack, reducing the requirement of the back pressure of the reaction gas of the membrane fuel cell stack, improving the energy density of the fuel cell stack, reducing the cost of the fuel cell stack and realizing the rapid commercialization of the fuel cell stack.
EXAMPLE III
A membrane electrode for a fuel cell stack, the membrane electrode comprising: the proton exchange membrane comprises a cathode catalyst layer, an anode catalyst layer and a proton exchange membrane, wherein a metal organic framework material is added in the cathode catalyst layer and the anode catalyst layer.
The metal organic framework material has a hollow-out-like spherical structure and mesoporous channels of 2nm to 4 nm.
The metal organic framework material has sulfonic acid groups, and has good proton conductivity and certain moisture retention capacity; the metal organic framework material is added into the catalyst layer according to the proportion of 2.5 percent of the total amount of the catalyst layer substances.
The metal organic framework material can be sulfonated MIL-101; other metal organic framework materials are also possible.
The metal organic framework material is firstly mixed with the catalyst, and then the binder and the solvent are added for ultrasonic dispersion or ball milling to obtain the uniformly dispersed catalyst slurry.
The cathode catalyst slurry can be divided into A, B two parts, wherein part A is not added with metal organic framework materials, and part B is added with metal organic framework materials. Of course, the cathode catalyst slurry may not be divided into A, B portions.
The cathode catalyst slurry is sequentially coated on one side of the proton exchange membrane, the part A is coated on one side of the proton exchange membrane, and the part B is coated on the coating of the part A after drying.
In this embodiment, the catalyst ratio of the cathode catalyst slurry A, B is between 2:1 and 5:1 (other ratios are also possible).
The anode catalyst slurry can be divided into A, B parts, wherein, part A is not added with metal organic framework materials, and part B is added with metal organic framework materials. The anode catalyst slurry may not be divided into A, B portions.
The anode catalyst slurry is sequentially coated on one side of the proton exchange membrane, the part A is coated on one side of the proton exchange membrane, and the part B is coated on the coating of the part A after drying.
In this embodiment, the catalyst ratio of the anode catalyst slurry A, B is between 2:1 and 5:1 (other ratios are also possible).
The description and applications of the invention herein are illustrative and are not intended to limit the scope of the invention to the embodiments described above. Variations and modifications of the embodiments disclosed herein are possible, and alternative and equivalent various components of the embodiments will be apparent to those skilled in the art. It will be clear to those skilled in the art that the present invention may be embodied in other forms, structures, arrangements, proportions, and with other components, materials, and parts, without departing from the spirit or essential characteristics thereof. Other variations and modifications of the embodiments disclosed herein may be made without departing from the scope and spirit of the invention.
Claims (2)
1. A membrane electrode for a fuel cell stack, comprising: the device comprises a cathode catalyst layer, a perfluorosulfonic acid membrane and an anode catalyst layer, wherein a metal organic framework material is added into the anode catalyst layer and the cathode catalyst layer;
quantitative metal organic framework materials are added in the cathode catalyst layer, and the metal organic framework materials improve the mesoporous porosity of the cathode catalyst layer in the cathode catalyst layer, so that reaction gas can enter the catalyst layer for reaction;
quantitative organic framework materials are added in the anode catalyst layer, and the metal organic framework materials improve the anode moisture retention performance and reduce the proton transfer resistance in the anode catalyst layer;
the addition amounts of the metal organic framework materials in the cathode catalyst layer and the anode catalyst layer are different; the metal organic framework materials added in the cathode catalyst layer and the anode catalyst layer have sulfonic acid groups serving as proton transfer channels;
the membrane electrode can be used for pretreating the metal organic framework material before adding the metal organic framework material into the catalyst layer, but the physical structure of the metal organic framework material is not changed by the pretreatment; the purpose of this pretreatment is to improve the conductivity of the metal organic framework material;
the membrane electrode does not need to be pretreated before the metal organic framework material is added into the catalyst layer, and the unsaturated metal of the metal organic framework material provides an active site which can efficiently adsorb toxic carbon monoxide in the reaction gas and provides the membrane electrode with anti-poisoning capability;
the metal organic framework materials of the membrane electrode are respectively reduced in gradient in the catalytic layer, and the distribution of the metal organic framework materials on the side close to the gas diffusion layer is higher than the density of the metal organic framework materials on the side close to the proton exchange membrane;
the metal organic framework material of the membrane electrode is added into the slurry according to the proportion of 0.5 to 10 percent of the catalyst and the binder, and is uniformly mixed and then coated on the surface of the perfluorosulfonic acid membrane;
and obtaining uniform slurry by adopting an ultrasonic dispersion mode or obtaining uniform slurry by adopting a ball milling mode.
2. A membrane electrode for a fuel cell stack, the membrane electrode comprising: the proton exchange membrane comprises a cathode catalyst layer, an anode catalyst layer and a proton exchange membrane, wherein a metal organic framework material is added in the cathode catalyst layer and the anode catalyst layer;
the metal organic framework material has a hollow-out-like spherical structure and has mesoporous channels of 2nm to 4 nm;
the metal organic framework material has sulfonic acid groups, and has good proton conductivity and certain moisture retention capacity;
the metal organic framework material is added into the catalyst layer according to the proportion of 2.5 percent of the total amount of the catalyst layer substances;
the metal organic framework material is sulfonated MIL-101;
mixing the metal organic framework material with a catalyst, and then adding a binder and a solvent to perform ultrasonic dispersion or ball milling to obtain uniformly dispersed catalyst slurry;
the cathode catalyst slurry is divided into A, B parts, wherein part A is not added with metal organic framework materials, and part B is added with metal organic framework materials;
the cathode catalyst slurry is sequentially coated on one side of a proton exchange membrane, the part A is coated on one side of the proton exchange membrane, and the part B is coated on the coating of the part A after drying;
the catalyst ratio in the cathode catalyst slurry A, B portion is between 2:1 and 5: 1;
the anode catalyst slurry is divided into A, B parts, wherein part A is not added with metal organic framework materials, and part B is added with metal organic framework materials;
the anode catalyst slurry is sequentially coated on one side of a proton exchange membrane, the part A is coated on one side of the proton exchange membrane, and the part B is coated on the coating of the part A after drying;
the catalyst ratio in the anode catalyst slurry A, B portion is between 2:1 and 5: 1.
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| CN109273748B (en) * | 2018-09-30 | 2020-09-29 | 德州新动能铁塔发电有限公司 | Membrane electrode containing porous coordination polymer and preparation method thereof |
| CN111244475B (en) * | 2018-11-28 | 2021-03-12 | 中国科学院大连化学物理研究所 | High-temperature proton exchange membrane fuel cell membrane electrode and preparation method and application thereof |
| CN109675441B (en) * | 2019-01-11 | 2020-08-11 | 浙江大学 | Heparin sodium modified metal organic framework film and preparation method and application thereof |
| CN112018415B (en) * | 2019-05-31 | 2022-01-28 | 上海汽车集团股份有限公司 | Membrane electrode and preparation method thereof |
| US11705558B2 (en) * | 2020-06-19 | 2023-07-18 | Robert Bosch Gmbh | Patterned catalyst layers in fuel cells |
| CN112117468B (en) * | 2020-08-21 | 2021-10-08 | 同济大学 | Preparation method of framework fuel cell catalyst layer |
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| CN1656632A (en) * | 2002-05-23 | 2005-08-17 | 哥伦比亚化学公司 | Proton conductive carbon material |
| CN103178273A (en) * | 2013-03-01 | 2013-06-26 | 北京化工大学常州先进材料研究院 | Electrocatalyst of MOFs (Metal-organic Frameworks)/graphene composite carrier and preparation method of electrocatalyst |
| CN103219531A (en) * | 2013-03-01 | 2013-07-24 | 北京化工大学常州先进材料研究院 | High activity electric catalyst using metal organic skeleton as carrier and preparation method thereof |
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| US9147920B2 (en) * | 2010-07-01 | 2015-09-29 | Ford Global Technologies, Llc | Metal oxygen battery containing oxygen storage materials |
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| CN1656632A (en) * | 2002-05-23 | 2005-08-17 | 哥伦比亚化学公司 | Proton conductive carbon material |
| CN103178273A (en) * | 2013-03-01 | 2013-06-26 | 北京化工大学常州先进材料研究院 | Electrocatalyst of MOFs (Metal-organic Frameworks)/graphene composite carrier and preparation method of electrocatalyst |
| CN103219531A (en) * | 2013-03-01 | 2013-07-24 | 北京化工大学常州先进材料研究院 | High activity electric catalyst using metal organic skeleton as carrier and preparation method thereof |
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