WO2021109721A1 - 一种熔融碳酸盐燃料电池堆电解质补充方法 - Google Patents
一种熔融碳酸盐燃料电池堆电解质补充方法 Download PDFInfo
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- WO2021109721A1 WO2021109721A1 PCT/CN2020/121292 CN2020121292W WO2021109721A1 WO 2021109721 A1 WO2021109721 A1 WO 2021109721A1 CN 2020121292 W CN2020121292 W CN 2020121292W WO 2021109721 A1 WO2021109721 A1 WO 2021109721A1
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- electrolyte
- fuel cell
- battery stack
- molten carbonate
- cell stack
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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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04276—Arrangements for managing the electrolyte stream, e.g. heat exchange
- H01M8/04283—Supply means of electrolyte to or in matrix-fuel cells
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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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04276—Arrangements for managing the electrolyte stream, e.g. heat exchange
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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
- H01M8/14—Fuel cells with fused electrolytes
- H01M8/144—Fuel cells with fused electrolytes characterised by the electrolyte material
- H01M8/145—Fuel cells with fused electrolytes characterised by the electrolyte material comprising carbonates
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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
- H01M8/2457—Grouping of fuel cells, e.g. stacking of fuel cells with both reactants being gaseous or vaporised
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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
- H01M8/14—Fuel cells with fused electrolytes
- H01M2008/147—Fuel cells with molten carbonates
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0048—Molten electrolytes used at high temperature
- H01M2300/0051—Carbonates
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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
Definitions
- the invention relates to the technical field of molten carbonate fuel cells, in particular to an electrolyte supplement method for a molten carbonate fuel cell stack.
- the fuel cell is a new power source with high efficiency and clean characteristics that integrates new technologies such as energy, chemical industry, materials and automatic control.
- Molten carbonate fuel cells are composed of key components such as electrodes, electrolyte membranes, carbonate sheets, and bipolar plates.
- the electrolyte diaphragm and the carbonate sheet are sintered together during the operation of the battery stack, and the molten carbonate penetrates into the pores of the sintered electrolyte diaphragm by capillary action, which acts as a gas barrier and conducts carbonate ions.
- the electrolyte membrane must have the function of storing the molten carbonate electrolyte in the battery for a long time, but in the actual operation of the battery stack, there is a problem of electrolyte loss, which greatly affects the life and stable operation of the battery stack.
- the loss of electrolyte is mainly due to corrosion reaction with metal parts, evaporation and migration of electrolyte, etc.
- the loss of electrolyte causes the internal resistance of the battery to increase, and the coarse pores of the electrolyte diaphragm plate reduce the retention of the electrolyte and accelerate the loss of the electrolyte. Therefore, in order to ensure the long life and stable operation of the molten carbonate fuel cell stack, the electrolyte replenishment technology during operation can extend the service life of the molten carbonate fuel cell and increase the competitiveness of the molten carbonate fuel cell power generation technology.
- the method for replenishing the electrolyte of a molten carbonate fuel cell stack includes the following steps:
- Step 1 Prepare an electrolyte gel solution containing 10%-20% electrolyte, wherein the viscosity of the electrolyte gel solution is 200-800 Pa ⁇ s;
- Step 2 Use the electrolyte gel solution prepared in Step 1 to supplement the battery stack electrolyte, so that the electrolyte adheres to the electrodes and the internal flow channels of the battery stack;
- Step 4 Dry the moisture or organic solvent in the battery stack under the inert gas condition to discharge the battery stack electrolyte, and then perform the discharge performance test.
- the preparation method of the electrolyte gel solution includes the following steps:
- electrolyte gel solution containing 10% to 20% electrolyte.
- the viscosity of the electrolyte gel solution is 200-800 Pa ⁇ s.
- step 2 the electrolyte gel solution prepared in step 1 is used to supplement the battery stack electrolyte, the specific method is:
- the anode or cathode inlet of the molten carbonate fuel cell, the container containing the electrolyte colloid solution prepared in step 1, the circulating pump, and the anode or cathode outlet of the molten carbonate fuel cell constitute a circulating loop for supplementing electrolyte;
- the circulation pump is started to fully circulate the electrolyte gel solution in the internal flow channel of the battery stack, so that part of the electrolyte adheres to the electrodes and the internal flow channel of the battery stack during the circulation process.
- step 3 the excess electrolyte colloid solution in the battery stack is discharged, and the specific method is:
- Air or nitrogen with a cathode flow rate of 15%-30% of the full power of the battery stack is used to pass into the battery stack from the cathode or anode inlet on the upper part of the battery stack, and the excess electrolyte colloid solution in the battery stack is completely discharged from the cathode or anode outlet on the lower part of the battery stack .
- step 4 the process conditions for drying and discharging the moisture or organic solvent in the battery stack are:
- nitrogen or carbon dioxide inert gas is introduced into the battery stack, and heated and ventilated for 24 to 48 hours.
- the invention provides a molten carbonate fuel cell stack electrolyte replenishment method, which can make use of the good fluidity and viscosity of the electrolyte colloid solution to uniformly adhere the electrolyte to the electrode and the channel inside the flow field, and use the molten electrolyte
- the principle of capillary infiltration supplements the electrolyte loss in the stack. This method can effectively supplement the performance and lifespan of the molten carbonate fuel cell due to electrolyte loss during high-temperature operation, and is useful for improving the stability of the molten carbonate fuel cell. Performance and longevity have important guiding significance.
- the molten carbonate electrolyte is generally solid. It melts into a liquid state under high temperature conditions and relies on capillary force to inhale into the micropores of the diaphragm to isolate the two-stage gas. It is difficult for the solid electrolyte to be evenly replenished into the battery stack. It may cause blockage of the internal pipeline of the battery, and the electrolyte, the binder and the solvent are dispersed into a liquid colloid, and the electrolyte can be evenly transported into the battery and distributed evenly through the continuous flow of the circulating pump.
- the content of electrolyte supplemented to the battery stack is adjusted by adjusting the electrolyte content in the electrolyte gel, and the gel contains a small amount of binder, and the electrolyte can be evenly dispersed in the gel, ensuring that the electrolyte is evenly dispersed in the battery stack Various parts within.
- Figure 1 is an electrolyte supplement circuit device related to the present invention
- Electrolyte colloid solution container 2. Circulation pump 3. Anode or cathode inlet 4. Battery 5. Molten carbonate fuel cell 6. Anode or cathode outlet 7. Circulation pipeline.
- the specific solution of the present invention is: an electrolyte replenishment method for a molten carbonate fuel cell stack, which includes the following specific steps:
- the first is to mix lithium carbonate and sodium carbonate with a molar percentage of 53:47 to form an electrolyte
- the second method is to mix lithium carbonate and potassium carbonate with a molar percentage of 62:38 to form an electrolyte
- electrolyte gel solution aqueous solution of polyvinyl alcohol with a concentration of 0.5% to 3%, or a mixed solution formed by alcohol and polyvinyl butyral, and an electrolyte colloidal solution containing 10% to 20% electrolyte.
- the viscosity of the electrolyte gel solution is 200-800 Pa ⁇ s.
- the concentration of the mixed solution formed by alcohol and polyvinyl butyral is 3% to 5%, and the concentration of alcohol is 95%.
- the anode or cathode inlet 3 of the molten carbonate fuel cell 5, the electrolyte colloid solution container 1, the liquid circulation pump 2, and the MCFC anode or cathode outlet 6 form a circulation loop that replenishes the electrolyte, and the circulation pump 2 is started to make the electrolyte
- the colloidal solution is fully circulated in the internal flow channel of the battery stack for 24 to 48 hours to ensure that a part of the electrolyte adheres to the electrodes and the internal flow channel of the battery stack during the circulation process.
- Air or nitrogen with a cathode flow rate of 15% to 30% of the full power of the battery stack is used to pass into the battery stack from the cathode or anode inlet on the upper part of the battery stack, and the excess electrolyte colloid solution in the battery stack is removed from the cathode or anode outlet on the lower part of the battery stack.
- Exhaust, ventilation time is 24 to 48 hours; by controlling the air flow, on the one hand, the residual colloid is slowly blown out of the battery stack, and on the other hand, the electrolyte is slowly attached to the wall of the components inside the battery stack.
- the present invention is an electrolyte replenishment method for molten carbonate fuel cell stack, which has important guiding significance in the field of MCFC research and application.
- the following examples will illustrate the specific guiding effect of the present invention.
- the volume of the flow field and flow channel in the cell stack is calculated to be about 0.036m 3 .
- the amount of gel solution is the internal flow of the battery stack. 3 times the volume of field and flow channel;
- the temperature is increased to 450°C at a heating rate of 1°C/3min, and the temperature is kept for 5 hours.
- the temperature is increased to 550°C at a heating rate of 1°C/3min, and then to 650°C at a heating rate of 1°C/1min, and the anode is connected.
- air and carbon dioxide can be introduced into the cathode to perform discharge performance test.
- Lithium carbonate and sodium carbonate with a molar percentage of 53:47 were mixed, and then mixed with a 1.5% polyvinyl alcohol aqueous solution with stirring to prepare an electrolyte gel solution containing 15% electrolyte and a viscosity of 200 Pa ⁇ s.
- Lithium carbonate and sodium carbonate with a molar percentage of 53:47 were mixed, and then mixed with a 3% polyvinyl alcohol aqueous solution with stirring to prepare an electrolyte gel solution containing 20% electrolyte and a viscosity of 200 Pa ⁇ s.
- Lithium carbonate and sodium carbonate with a molar percentage of 53:47 are mixed, and then mixed with a 0.5% polyvinyl alcohol aqueous solution with stirring to prepare an electrolyte gel solution containing 13% electrolyte and a viscosity of 200 Pa ⁇ s.
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- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Fuel Cell (AREA)
Abstract
Description
Claims (6)
- 一种熔融碳酸盐燃料电池堆电解质补充方法,其特征在于,包括以下步骤:步骤1,配制含10%~20%电解质的电解质胶体溶液,其中,所述电解质胶体溶液的粘度为200~800Pa·s;步骤2,利用步骤1配制得到的电解质胶体溶液进行电池堆电解质的补充,使得电解质粘附在电极及电池堆内部流道;步骤3,将电池堆内多余的电解质胶体溶液排出;步骤4,在惰性气体条件下,将电池堆内的水分或有机溶剂烘干排出,即完成电池堆电解质的补充,之后进行放电性能测试。
- 根据权利要求1所述的一种熔融碳酸盐燃料电池堆电解质补充方法,其特征在于,步骤1中,电解质胶体溶液的配制方法,包括以下步骤:将摩尔百分比为62:38的碳酸锂和碳酸钾进行混合,形成电解质;将得到的电解质与浓度为0.5%~3%的聚乙烯醇水溶液,或与95%酒精与聚乙烯醇缩丁醛形成的混合溶液进行混合,含10%~20%电解质的电解质胶体溶液,其中,所述电解质胶体溶液的粘度为200~800Pa·s。
- 根据权利要求1所述的一种熔融碳酸盐燃料电池堆电解质补充方法,其特征在于,步骤1中,电解质胶体溶液的配制方法,包括以下步骤:将摩尔百分比为53:47的碳酸锂和碳酸钠进行混合,形成电解质;将得到的电解质与浓度为0.5%~3%的聚乙烯醇水溶液,或与95%酒精与聚乙烯醇缩丁醛形成的混合溶液进行混合,含10%~20%电解质的电解质胶体溶液,其中,所述电解质胶体溶液的粘度为200~800Pa·s。
- 根据权利要求1所述的一种熔融碳酸盐燃料电池堆电解质补充方法,其特征在于,步骤2中,利用步骤1配制得到的电解质胶体溶液进行电池堆电解质的补充,具体方法是:由熔融碳酸盐燃料电池的阳极或阴极入口、盛放有步骤1配制得到的电解质胶体溶液的容器、循环泵、以及熔融碳酸盐燃料电池的阳极或阴极出口组成补充电解质的循环回路;之后启动循环泵,使电解质胶体溶液在电池堆内部流道中充分循环,使得部分电解质在循环过程中粘附在电极及电池堆内部流道。
- 根据权利要求1所述的一种熔融碳酸盐燃料电池堆电解质补充方法,其特征在于,步骤3中,将电池堆内多余的电解质胶体溶液排出,具体方法是:采用电池堆全功率15%~30%阴极流量的空气或氮气从电池堆上部的阴极或阳极入口通入电池堆,从电池堆下部的阴极或阳极出口将电池堆内多余的电解质胶体溶液完全排出。
- 根据权利要求1所述的一种熔融碳酸盐燃料电池堆电解质补充方法,其特征在于,步骤4中,将电池堆内的水分或有机溶剂烘干排出的工艺条件是:在66~80℃加热条件下,向电池堆内通入氮气或二氧化碳惰性气体,加热通气24~48小时。
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CN110911717B (zh) * | 2019-12-03 | 2021-03-23 | 中国华能集团清洁能源技术研究院有限公司 | 一种熔融碳酸盐燃料电池堆电解质补充方法 |
CN113471500B (zh) * | 2021-07-16 | 2023-10-03 | 华能国际电力股份有限公司 | 一种熔融碳酸盐燃料电池盐膜及其制备方法 |
CN116706347B (zh) * | 2023-08-02 | 2023-10-20 | 德阳市东新机电有限责任公司 | 快速加热反应堆电解液的铝燃料电池及快速加热方法 |
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US11728502B2 (en) | 2023-08-15 |
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JP7170909B2 (ja) | 2022-11-14 |
CN110911717A (zh) | 2020-03-24 |
CN110911717B (zh) | 2021-03-23 |
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