WO2022193545A1 - 一种直接利用甲醇重整气的燃料电池系统及其工作方法 - Google Patents

一种直接利用甲醇重整气的燃料电池系统及其工作方法 Download PDF

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WO2022193545A1
WO2022193545A1 PCT/CN2021/113997 CN2021113997W WO2022193545A1 WO 2022193545 A1 WO2022193545 A1 WO 2022193545A1 CN 2021113997 W CN2021113997 W CN 2021113997W WO 2022193545 A1 WO2022193545 A1 WO 2022193545A1
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gas
unit
heat exchange
fuel cell
exchange unit
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PCT/CN2021/113997
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French (fr)
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李�昊
程健
张瑞云
卢成壮
许世森
李卫东
王保民
杨冠军
黄华
白发琪
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华能国际电力股份有限公司
中国华能集团清洁能源技术研究院有限公司
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Publication of WO2022193545A1 publication Critical patent/WO2022193545A1/zh

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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
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H01M8/0618—Reforming processes, e.g. autothermal, partial oxidation or steam reforming
    • 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
    • H01M8/04007—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids related to heat exchange
    • 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
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04119—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying
    • H01M8/04156—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying with product water removal
    • H01M8/04164—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying with product water removal by condensers, gas-liquid separators or filters
    • 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
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0432—Temperature; Ambient temperature
    • H01M8/04328—Temperature; Ambient temperature of anode reactants at the inlet or inside the fuel cell
    • 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
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0438—Pressure; Ambient pressure; Flow
    • H01M8/04388—Pressure; Ambient pressure; Flow of anode reactants at the inlet or inside the fuel cell
    • 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
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0438—Pressure; Ambient pressure; Flow
    • H01M8/04395—Pressure; Ambient pressure; Flow of cathode reactants at the inlet or inside the fuel cell
    • 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
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/0438—Pressure; Ambient pressure; Flow
    • H01M8/04402—Pressure; Ambient pressure; Flow of anode exhausts
    • 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
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04694—Processes for controlling fuel cells or fuel cell systems characterised by variables to be controlled
    • H01M8/04746—Pressure; Flow
    • H01M8/04753—Pressure; Flow of fuel cell reactants
    • 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
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04694—Processes for controlling fuel cells or fuel cell systems characterised by variables to be controlled
    • H01M8/04746—Pressure; Flow
    • H01M8/04761—Pressure; Flow of fuel cell exhausts
    • 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
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • 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
    • 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
    • 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 application belongs to the technical field of fuel cells, and in particular relates to a fuel cell system that directly utilizes methanol reformed gas and a working method thereof.
  • Molten carbonate fuel cell is a high-temperature fuel cell operating at 650°C. It uses hydrogen-rich gas as raw material and can directly convert chemical energy in the raw material into electrical energy. It is a clean, efficient, low-noise and low-pollution power generation. Way.
  • the cost of molten carbonate fuel cell power generation systems using hydrogen, natural gas, and syngas as raw materials is relatively high, while methanol reforming hydrogen production is a low-cost, clean and efficient way to produce hydrogen.
  • the hydrogen produced by methanol reforming is passed into the anode of the fuel cell, and the fuel cell power generation system using methanol as the raw material can be realized, which can reduce the cost of power generation.
  • the traditional methanol reforming hydrogen production device needs to be equipped with a gas separation device to purify the hydrogen in the methanol reformed gas, the process is complicated and lengthy, the cost is high, and the fuel utilization rate of the molten carbonate fuel cell is low.
  • the purpose of the present application is to provide a fuel cell system that directly utilizes methanol reformed gas and its working method, which shortens the process flow of the molten carbonate fuel cell power generation system using methanol as a raw material, and reduces the amount of molten carbon dioxide.
  • the cost of salt fuel cell power generation system and the cost of power generation make full use of the energy in the fuel.
  • the present application discloses a fuel cell system that directly utilizes methanol reformed gas, including a methanol reforming reaction unit, a first heat exchange unit, a first gas-liquid separation unit, a second gas-liquid separation unit, a catalytic combustion unit, a second a heat exchange unit, a third heat exchange unit, a fuel cell unit and a gas mixing device;
  • the inlet of the methanol reforming reaction unit is connected with a methanol feed pipe, the outlet of the methanol reforming reaction unit is connected with the hot side inlet of the first heat exchange unit, and the hot side outlet of the first heat exchange unit is connected with the first gas-liquid separation unit.
  • the inlet is connected, the gas phase outlet of the first gas-liquid separation unit is connected to the cold side inlet of the second heat exchange unit, the cold side outlet of the second heat exchange unit is connected to the anode fuel inlet of the fuel cell unit, and the anode of the fuel cell unit is connected
  • the exhaust gas outlet is connected to the inlet of the catalytic combustion unit, the inlet of the catalytic combustion unit is also connected with an O2 intake pipe, the outlet of the catalytic combustion unit is connected to the hot side inlet of the second heat exchange unit, and the hot side outlet of the second heat exchange unit is connected to The inlet of the second gas-liquid separation unit is connected, and the gas-phase outlet of the second gas-liquid separation unit is connected with the inlet of the gas mixing device.
  • the cold side inlet of the third heat exchange unit is connected, the cold side outlet of the third heat exchange unit is connected with the cathode fuel inlet of the fuel cell unit, and the cathode exhaust gas outlet of the fuel cell unit is connected with the hot side inlet of the third heat exchange unit , the hot-side outlet of the third heat exchange unit is connected with a cathode tail gas discharge pipe; the liquid-phase outlets of the first gas-liquid separation unit and the second gas-liquid separation unit are connected with a condensed water discharge pipe.
  • an anode gas flow detection and control device is provided on the connecting pipeline between the cold side outlet of the second heat exchange unit and the anode fuel inlet of the fuel cell unit, and the cold side outlet of the third heat exchange unit is connected to the fuel cell
  • a cathode gas flow detection and control device is provided on the connecting pipeline between the cathode fuel inlets of the unit, an air flow detection and control device is provided on the air intake pipe, and a CO2 flow detection and control device is provided on the CO2 intake pipe
  • the connecting pipeline between the gas phase outlet of the second gas-liquid separation unit and the inlet of the gas mixing device is provided with an anode tail gas flow detection and control device; an anode gas flow detection and control device, a cathode gas flow detection and control device, and an air flow rate
  • the detection and control device, the CO 2 flow detection and control device and the anode tail gas flow detection and control device are respectively connected with the control unit of the system.
  • a compression unit is provided on the connecting pipeline between the gas phase outlet of the second gas-liquid separation unit and the inlet of the gas mixing device.
  • a defoaming device is provided before the inlet of the compression unit.
  • the first heat exchange unit is a gas-liquid type heat exchanger
  • the second heat exchange unit and the third heat exchange unit are gas-gas type heat exchangers.
  • the condensed water outlets of the first gas-liquid separation unit and the second gas-liquid separation unit are respectively connected to the cold-side inlet of the first heat exchange unit.
  • a temperature detection device is provided on the connecting pipeline between the outlet of the methanol reforming reaction unit and the hot side inlet of the first heat exchange unit, and the condensed water outlet of the first gas-liquid separation unit and the second gas-liquid separation unit
  • the connection pipeline with the cold side inlet of the first heat exchange unit is respectively provided with a flow detection and control device, and the temperature detection device and the flow detection and control device are respectively connected with the control unit of the system.
  • the wall surface in the mixing device is a smooth curved surface, and the mixing device is provided with a turbulent component.
  • a first waste heat heat exchanger is arranged between the second heat exchange unit and the second gas-liquid separation unit, a second waste heat heat exchanger is arranged on the cathode tail gas discharge pipe, the first waste heat heat exchanger and The second waste heat exchangers are all used to heat the external medium.
  • the working method of the fuel cell system that directly utilizes methanol reformate gas disclosed in the present application is characterized in that, it includes:
  • the methanol reforming reaction unit undergoes a methanol reforming reaction, and the generated mixed gas enters the first heat exchange unit after heat exchange and condensation, and then enters the first gas-liquid separation unit to remove moisture to obtain a low-temperature mixed gas containing hydrogen and carbon dioxide; low-temperature mixed gas; After heat exchange in the second heat exchange unit, it enters the anode fuel inlet of the fuel cell unit, and the anode tail gas enters the catalytic combustion unit to remove unreacted H 2 and then enters the second heat exchange unit after heat exchange and condensation.
  • the moisture is removed in the separation unit, the remaining gas enters the gas mixing device, mixes with air and CO 2 , and enters the cathode fuel inlet of the fuel cell unit after the third heat exchange unit heats up and heats up, and the cathode tail gas enters the third heat exchange unit for exchange. After the heat is cooled down, it is discharged from the cathode exhaust exhaust pipe.
  • the present application discloses a fuel cell system that directly utilizes methanol reformed gas, the anode fuel required by the fuel cell unit is hydrogen-rich gas, and the cathode fuel is carbon dioxide and air, which can fully utilize the hydrogen and Carbon dioxide is used as the fuel, and the methanol reforming process for hydrogen production is low in cost; the methanol reformed gas is directly used, only water vapor is removed, and the hydrogen and carbon dioxide in it are not separated and purified, and the process route is simple.
  • the anode tail gas of the fuel cell is subjected to catalytic combustion treatment, which makes full use of the heat of unreacted hydrogen in the anode tail gas and improves the thermal efficiency of the power generation cell system; the anode tail gas after catalytic combustion is subsequently mixed with the cathode intake air to serve as the cathode raw material for reuse.
  • the waste heat of the exhaust gas is comprehensively utilized, the comprehensive thermoelectric efficiency of the fuel cell power generation system is improved, and the energy consumption of the system is reduced.
  • the key operation parameters of the system can be controlled to ensure the efficient and stable operation of the system.
  • a compression unit is provided on the connecting pipeline between the gas phase outlet of the second gas-liquid separation unit and the inlet of the gas mixing device, which can control the speed and flow of the circulating exhaust gas.
  • a defoaming device is provided before the inlet of the compression unit to prevent the incompletely removed moisture from affecting the normal operation of the compression unit.
  • the first heat exchange unit adopts a gas-liquid type heat exchanger
  • the second heat exchange unit and the third heat exchange unit adopt gas-gas type heat exchangers, which have higher heat exchange efficiency and improve the utilization rate of waste heat.
  • the mixed gas is cooled by the condensed water of the first gas-liquid separation unit and the second gas-liquid separation unit, which improves the energy utilization rate and reduces the system energy consumption.
  • the wall surface in the mixing device adopts a smooth curved surface to ensure the uniform flow of the internal gas without dead angle, and the turbulent component can improve the mixing degree of the gas at the same time.
  • setting the first waste heat heat exchanger and the second waste heat heat exchanger can make full use of the remaining heat again for external heating, lithium bromide cooling and other uses.
  • the working method of the fuel cell system that directly utilizes methanol reformed gas disclosed in the present application has the advantages of simple process flow, full utilization of reaction products and remaining heat in the system, low cost, low energy consumption, high comprehensive thermoelectric efficiency, and good application prospects.
  • FIG. 1 is a schematic diagram of the overall structure of the system of the application.
  • 1- methanol reforming reaction unit 2- first heat exchange unit; 3- first gas-liquid separation unit; 4- second gas-liquid separation unit; 5- catalytic combustion unit; 6- second heat exchange unit ;7-compression unit;8-third heat exchange unit;9-fuel cell unit;10-gas mixing device;11-methanol storage tank;12-anode gas flow detection and control device;13-cathode gas flow detection and control device; 14-air flow detection and control device; 15-CO 2 flow detection and control device; 16-anode tail gas flow detection and control device.
  • the fuel cell system directly utilizing methanol reformed gas mainly includes a methanol reforming reaction unit 1 , a first heat exchange unit 2 , a first gas-liquid separation unit 3 , and a second gas-liquid separation unit 4 , a catalytic combustion unit 5 , a second heat exchange unit 6 , a third heat exchange unit 8 , a fuel cell unit 9 and a gas mixing device 10 .
  • the inlet of the methanol reforming reaction unit 1 is connected with a methanol feed pipe, the outlet of the methanol reforming reaction unit 1 is connected with the hot side inlet of the first heat exchange unit 2, and the hot side outlet of the first heat exchange unit 2 is connected with the first gas
  • the inlet of the liquid separation unit 3 is connected, the gas phase outlet of the first gas-liquid separation unit 3 is connected to the cold side inlet of the second heat exchange unit 6, and the cold side outlet of the second heat exchange unit 6 is connected to the anode fuel inlet of the fuel cell unit 9.
  • the material port is connected, the anode tail gas outlet of the fuel cell unit 9 is connected with the inlet of the catalytic combustion unit 5, the inlet of the catalytic combustion unit 5 is also connected with an O2 intake pipe, and the outlet of the catalytic combustion unit 5 is connected with the heat of the second heat exchange unit 6.
  • the side inlet is connected, the hot side outlet of the second heat exchange unit 6 is connected to the inlet of the second gas-liquid separation unit 4, the gas phase outlet of the second gas-liquid separation unit 4 is connected to the inlet of the gas mixing device 10, and the The inlet is also connected with an air intake pipe and a CO2 intake pipe, the outlet of the air mixing device 10 is connected with the cold side inlet of the third heat exchange unit 8, and the cold side outlet of the third heat exchange unit 8 is connected with the cathode fuel of the fuel cell unit 9.
  • the feed inlet is connected, the cathode tail gas outlet of the fuel cell unit 9 is connected with the hot side inlet of the third heat exchange unit 8, and the hot side outlet of the third heat exchange unit 8 is connected with a cathode tail gas discharge pipe; the first gas-liquid separation unit 3 A condensed water discharge pipe is connected to the liquid phase outlet of the second gas-liquid separation unit 4 .
  • the connecting pipeline between the cold side outlet of the second heat exchange unit 6 and the anode fuel inlet of the fuel cell unit 9 is provided with an anode gas flow detection and control device 12,
  • a cathode gas flow detection and control device 13 is arranged on the connecting pipeline between the cold side outlet of the third heat exchange unit 8 and the cathode fuel inlet of the fuel cell unit 9, and an air flow detection and control device is arranged on the air intake pipe 14.
  • a CO2 flow detection and control device 15 is provided on the CO2 inlet pipe, and an anode tail gas flow detection and control device is provided on the connecting pipeline between the gas phase outlet of the second gas-liquid separation unit 4 and the inlet of the gas mixing device 10 16;
  • Anode gas flow detection and control device 12, cathode gas flow detection and control device 13, air flow detection and control device 14, CO 2 flow detection and control device 15 and anode tail gas flow detection and control device 16 are respectively connected with the system. Control unit connection.
  • a compression unit 7 is provided on the connecting pipeline between the gas phase outlet of the second gas-liquid separation unit 4 and the inlet of the gas mixing device 10 .
  • a de-foaming device such as a de-foaming net, a de-foaming grid, etc., is provided before the inlet of the compression unit 7 .
  • the first heat exchange unit 2 is a gas-liquid type heat exchanger
  • the second heat exchange unit 6 and the third heat exchange unit 8 are gas-gas type heat exchangers.
  • the condensed water outlets of the first gas-liquid separation unit 3 and the second gas-liquid separation unit 4 are connected to the cold-side inlet of the first heat exchange unit 2 respectively.
  • a temperature detection device is provided on the connecting pipeline between the outlet of the methanol reforming reaction unit 1 and the hot side inlet of the first heat exchange unit 2, and the first gas-liquid separation unit 3 and the second gas-liquid separation unit 4
  • the connection pipelines between the condensate water outlet and the cold side inlet of the first heat exchange unit 2 are respectively provided with flow detection and control devices, and the temperature detection and flow detection and control devices are respectively connected to the control unit of the system.
  • the wall surface in the mixing device 10 is a smooth curved surface, and the mixing device 10 is provided with flow-disturbing components, such as a flow-disturbing column, a flow-disturbing plate, and the like.
  • a first waste heat heat exchanger is arranged between the second heat exchange unit 6 and the second gas-liquid separation unit 4, and a second waste heat exchanger is arranged on the cathode tail gas discharge pipe Heater, the first waste heat heat exchanger and the second waste heat heat exchanger are all used to heat the external medium, which can be used for heating, lithium bromide refrigeration, etc.
  • the methanol reforming reaction unit 1 undergoes a methanol reforming reaction, and the generated mixed gas enters the first heat exchange unit 2 after heat exchange and condensation, and then enters the first gas-liquid separation unit 3 to remove moisture to obtain a low-temperature mixed gas containing hydrogen and carbon dioxide;
  • the low-temperature mixed gas enters the anode fuel feed port of the fuel cell unit 9 after heat exchange and temperature rise in the second heat exchange unit 6, and the anode tail gas enters the catalytic combustion unit 5 to remove the unreacted H 2 and then enters the second heat exchange unit 6 for heat exchange.
  • the remaining gas After condensation, moisture is removed in the second gas-liquid separation unit 4, the remaining gas enters the gas mixing device 10, mixed with air and CO2 , and enters the cathode fuel feed of the fuel cell unit 9 after heat exchange in the third heat exchange unit 8
  • the cathode exhaust gas enters the third heat exchange unit 8 and is discharged from the cathode exhaust gas discharge pipe after heat exchange and cooling.
  • the system is mainly composed of fuel processing system, fuel cell body, anode tail gas circulation and waste heat recovery and utilization system.
  • the fuel processing system mainly includes a methanol reforming hydrogen production unit and a water vapor condensation and separation unit.
  • the methanol reforming hydrogen production unit mainly undergoes a reforming reaction of methanol and water, which generates a mixed gas (water-containing) of hydrogen and carbon dioxide with a proportion of about 75% and 25%, respectively. As shown in the following reaction equation, the main components are generated. It is a mixed gas of hydrogen and carbon dioxide, and then the moisture in the methanol reformed gas is separated by condensation.
  • the main body of the molten carbonate fuel cell stack works at 650°C, and the anode uses hydrogen-rich gas as the fuel.
  • methanol reformate gas is used as the anode fuel, and the carbon dioxide in the methanol reformate gas does not participate in the reaction; the cathode uses carbon dioxide and oxygen ( from air) as a raw material, and electrochemical reactions take place inside the fuel cell.
  • the tail gas circulation unit mainly means that the anode tail gas first undergoes catalytic combustion to remove unreacted hydrogen, and then separates the water vapor in the anode tail gas through heat exchange condensation. At this time, the main component of the anode tail gas is carbon dioxide. The anode exhaust gas is then mixed with cathode intake air and reused as cathode raw material.
  • the waste heat recovery and utilization unit mainly uses the waste heat of the high temperature anode exhaust gas and the high temperature cathode exhaust gas of the molten carbonate fuel cell. First, the waste heat is applied to the anode and cathode intake air of the molten carbonate fuel cell. After the waste heat is completed, the remaining low-grade fuel cell exhaust gas The heat and the low-grade heat of methanol reformate gas can be exchanged with cold water for heating, lithium bromide refrigeration, etc.

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Abstract

本申请公开的一种直接利用甲醇重整气的燃料电池系统及其工作方法，属于燃料电池技术领域。主要包括甲醇重整反应单元、第一换热单元、第一气液分离单元、第二气液分离单元、催化燃烧单元、第二换热单元、第三换热单元、燃料电池单元和混气装置。本申请直接利用甲醇重整气作为阳极原料，不做氢气提纯分离处理，缩短简化了工艺流程；同时，阳极尾气经过催化燃烧，充分释放阳极尾气中未反应的氢气的热量，提高燃料电池发电系统热效率，并将经过催化燃烧的阳极尾气与阴极进气混合，作为阴极原料循环利用，提高燃料利用率，提高熔融碳酸盐燃料电池发电系统热电综合效率，具有良好的应用前景。

Description

一种直接利用甲醇重整气的燃料电池系统及其工作方法 技术领域
本申请属于燃料电池技术领域，具体涉及一种直接利用甲醇重整气的燃料电池系统及其工作方法。
背景技术
熔融碳酸盐燃料电池是一种工作于650℃的高温燃料电池，采用富氢气体作为原料，可以直接将原料中的化学能转化为电能，是一种清洁高效、低噪音、低污染的发电方式。
目前，以氢气、天然气、合成气为原料的熔融碳酸盐燃料电池发电系统成本相对偏高，而甲醇重整制氢是一种成本较低、清洁高效的制氢方式，将其与熔融碳酸盐燃料电池结合，将甲醇重整制得的氢气通入燃料电池阳极，实现用甲醇为原料的燃料电池发电系统，可降低发电成本。但是，传统甲醇重整制氢装置要配备气体分离装置来提纯甲醇重整气中的氢气，工艺复杂冗长，成本偏高，熔融碳酸盐燃料电池燃料利用率低。
发明内容
为了解决上述问题，本申请的目的在于提供一种直接利用甲醇重整气的燃料电池系统及其工作方法，缩短了以甲醇为原料的熔融碳酸盐燃料电池发电系统工艺流程，降低了熔融碳酸盐燃料电池发电系统成本及发电成本，充分利用了燃料中的能量。
本申请是通过以下技术方案来实现：
本申请公开了一种直接利用甲醇重整气的燃料电池系统，包括甲醇重整反应单元、第一换热单元、第一气液分离单元、第二气液分离单元、催化燃烧单元、第二换热单元、第三换热单元、燃料电池单元和混气装置；
甲醇重整反应单元的进口连接有甲醇进料管，甲醇重整反应单元的出口与 第一换热单元的热侧进口连接，第一换热单元的热侧出口与第一气液分离单元的进口连接，第一气液分离单元的气相出口与第二换热单元的冷侧进口连接，第二换热单元的冷侧出口与燃料电池单元的阳极燃料进料口连接，燃料电池单元的阳极尾气出口与催化燃烧单元的进口连接，催化燃烧单元的进口还连接有O 2进气管，催化燃烧单元的出口与第二换热单元的热侧进口连接，第二换热单元的热侧出口与第二气液分离单元的进口连接，第二气液分离单元的气相出口与混气装置的进口连接，混气装置的进口还连接有空气进气管和CO 2进气管，混气装置的出口与第三换热单元的冷侧进口连接，第三换热单元的冷侧出口与燃料电池单元的阴极燃料进料口连接，燃料电池单元的阴极尾气出口与第三换热单元的热侧进口连接，第三换热单元的热侧出口连接有阴极尾气排出管；第一气液分离单元和第二气液分离单元的液相出口均连接有冷凝水排出管。
优选地，第二换热单元的冷侧出口与燃料电池单元的阳极燃料进料口之间的连接管路上设有阳极气体流量检测及控制装置，第三换热单元的冷侧出口与燃料电池单元的阴极燃料进料口之间的连接管路上设有阴极气体流量检测及控制装置，空气进气管上设有空气流量检测及控制装置，CO 2进气管上设有CO 2流量检测及控制装置，第二气液分离单元的气相出口与混气装置的进口之间的连接管路上设有阳极尾气流量检测及控制装置；阳极气体流量检测及控制装置、阴极气体流量检测及控制装置、空气流量检测及控制装置、CO 2流量检测及控制装置和阳极尾气流量检测及控制装置均分别与系统的控制单元连接。
优选地，第二气液分离单元的气相出口与混气装置的进口之间的连接管路上设有压缩单元。
进一步优选地，压缩单元进口前设有除沫装置。
优选地，第一换热单元为气-液型换热器，第二换热单元和第三换热单元为气-气型换热器。
优选地，第一气液分离单元和第二气液分离单元的冷凝水出口均分别与第 一换热单元的冷侧入口连接。
进一步优选地，甲醇重整反应单元的出口与第一换热单元的热侧进口之间的连接管路上设有温度检测装置，第一气液分离单元和第二气液分离单元的冷凝水出口与第一换热单元的冷侧入口之间的连接管路上均分别设有流量检测及控制装置，温度检测装置和流量检测及控制装置均分别与系统的控制单元连接。
优选地，混合装置内的壁面为圆滑曲面，混合装置内设有扰流部件。
优选地，第二换热单元与第二气液分离单元之间设有第一余热换热器，阴极尾气排出管上设有第二余热换热器，第一余热换热器和第二余热换热器均用于加热外部介质。
本申请公开的上述直接利用甲醇重整气的燃料电池系统的工作方法，其特征在于，包括：
甲醇重整反应单元发生甲醇重整反应，生成的混合气体进入第一换热单元换热冷凝后，进入第一气液分离单元中除去水分，得到含有氢气和二氧化碳的低温混合气体；低温混合气体在第二换热单元中换热升温后进入燃料电池单元的阳极燃料进料口，阳极尾气进入催化燃烧单元除去未反应的H 2后进入第二换热单元换热冷凝后在第二气液分离单元中除去水分，剩余气体进入混气装置，与空气和CO 2混合，在第三换热单元换热升温后进入燃料电池单元的阴极燃料进料口，阴极尾气进入第三换热单元换热降温后由阴极尾气排出管排出。
与现有技术相比，本申请具有以下有益的技术效果：
本申请公开的一种直接利用甲醇重整气的燃料电池系统，燃料电池单元所需的阳极燃料为富氢气体，阴极燃料为二氧化碳和空气，可以充分利用甲醇重整制氢工艺产生的氢气和二氧化碳作为燃料，甲醇重整制氢工艺成本低；直接使用甲醇重整气，只去除水蒸汽，不对其中的氢气和二氧化碳做分离提纯处理，工艺路线简单。燃料电池阳极尾气做催化燃烧处理，充分利用了阳极尾气中未反应的氢气的热量，提高发电电池系统热效率；后续将经过催化燃烧的阳极尾 气与阴极进气混合，作为阴极原料，重复利用。综合利用了尾气的余热，提高了燃料电池发电系统综合热电效率，减少了系统能耗。
进一步地，通过在系统的关键部位设置流量检测及控制装置，能够控制系统的关键运行参数，保证系统高效、稳定地运行。
进一步地，第二气液分离单元的气相出口与混气装置的进口之间的连接管路上设有压缩单元，能够控制循环尾气的速度及流量。
更进一步地，压缩单元进口前设有除沫装置，防止未完全去除的水分影响压缩单元的正常运行。
进一步地，第一换热单元采用气-液型换热器，第二换热单元和第三换热单元采用气-气型换热器，具有较高的换热效率，提高余热利用率。
进一步地，利用第一气液分离单元和第二气液分离单元的冷凝水对混合气进行降温，提高了能源利用率，减少了系统能耗。
进一步地，混合装置内的壁面采用圆滑曲面，保证内部气体的均匀流动无死角，同时扰流部件能够提高气体的混合程度。
进一步地，设置第一余热换热器和第二余热换热器能够再次将剩余热量充分利用，对外做供暖、溴化锂制冷等使用。
本申请公开的上述直接利用甲醇重整气的燃料电池系统的工作方法，工艺流程简单，充分利用了系统中反应产物及其余热，系统的成本低、能耗低、综合热电效率高，具有良好的应用前景。
附图说明
图1为本申请的系统整体结构示意图。
图中：1-甲醇重整反应单元；2-第一换热单元；3-第一气液分离单元；4-第二气液分离单元；5-催化燃烧单元；6-第二换热单元；7-压缩单元；8-第三换热单元；9-燃料电池单元；10-混气装置；11-甲醇储罐；12-阳极气体流量检测及控制装置；13-阴极气体流量检测及控制装置；14-空气流量检测及控制装置；15-CO 2 流量检测及控制装置；16-阳极尾气流量检测及控制装置。
具体实施方式
下面结合附图对本申请做进一步详细描述，其内容是对本申请的解释而不是限定：
如图1，为本申请的直接利用甲醇重整气的燃料电池系统，主要包括甲醇重整反应单元1、第一换热单元2、第一气液分离单元3、第二气液分离单元4、催化燃烧单元5、第二换热单元6、第三换热单元8、燃料电池单元9和混气装置10。
甲醇重整反应单元1的进口连接有甲醇进料管，甲醇重整反应单元1的出口与第一换热单元2的热侧进口连接，第一换热单元2的热侧出口与第一气液分离单元3的进口连接，第一气液分离单元3的气相出口与第二换热单元6的冷侧进口连接，第二换热单元6的冷侧出口与燃料电池单元9的阳极燃料进料口连接，燃料电池单元9的阳极尾气出口与催化燃烧单元5的进口连接，催化燃烧单元5的进口还连接有O 2进气管，催化燃烧单元5的出口与第二换热单元6的热侧进口连接，第二换热单元6的热侧出口与第二气液分离单元4的进口连接，第二气液分离单元4的气相出口与混气装置10的进口连接，混气装置10的进口还连接有空气进气管和CO 2进气管，混气装置10的出口与第三换热单元8的冷侧进口连接，第三换热单元8的冷侧出口与燃料电池单元9的阴极燃料进料口连接，燃料电池单元9的阴极尾气出口与第三换热单元8的热侧进口连接，第三换热单元8的热侧出口连接有阴极尾气排出管；第一气液分离单元3和第二气液分离单元4的液相出口均连接有冷凝水排出管。
在本申请的一个较优的实施例中，第二换热单元6的冷侧出口与燃料电池单元9的阳极燃料进料口之间的连接管路上设有阳极气体流量检测及控制装置12，第三换热单元8的冷侧出口与燃料电池单元9的阴极燃料进料口之间的连接管路上设有阴极气体流量检测及控制装置13，空气进气管上设有空气流量检 测及控制装置14，CO 2进气管上设有CO 2流量检测及控制装置15，第二气液分离单元4的气相出口与混气装置10的进口之间的连接管路上设有阳极尾气流量检测及控制装置16；阳极气体流量检测及控制装置12、阴极气体流量检测及控制装置13、空气流量检测及控制装置14、CO 2流量检测及控制装置15和阳极尾气流量检测及控制装置16均分别与系统的控制单元连接。
在本申请的一个较优的实施例中，第二气液分离单元4的气相出口与混气装置10的进口之间的连接管路上设有压缩单元7。优选地，压缩单元7进口前设有除沫装置，如除沫网、除沫栅板等。
在本申请的一个较优的实施例中，第一换热单元2为气-液型换热器，第二换热单元6和第三换热单元8为气-气型换热器。
在本申请的一个较优的实施例中，第一气液分离单元3和第二气液分离单元4的冷凝水出口均分别与第一换热单元2的冷侧入口连接。优选地，甲醇重整反应单元1的出口与第一换热单元2的热侧进口之间的连接管路上设有温度检测装置，第一气液分离单元3和第二气液分离单元4的冷凝水出口与第一换热单元2的冷侧入口之间的连接管路上均分别设有流量检测及控制装置，温度检测装置和流量检测及控制装置均分别与系统的控制单元连接。
在本申请的一个较优的实施例中，混合装置10内的壁面为圆滑曲面，混合装置10内设有扰流部件，如扰流柱、扰流板等。
在本申请的一个较优的实施例中，第二换热单元6与第二气液分离单元4之间设有第一余热换热器，阴极尾气排出管上设有第二余热换热器，第一余热换热器和第二余热换热器均用于加热外部介质，可用于供暖、溴化锂制冷等。
上述系统的工作方法如下：
甲醇重整反应单元1发生甲醇重整反应，生成的混合气体进入第一换热单元2换热冷凝后，进入第一气液分离单元3中除去水分，得到含有氢气和二氧化碳的低温混合气体；低温混合气体在第二换热单元6中换热升温后进入燃料 电池单元9的阳极燃料进料口，阳极尾气进入催化燃烧单元5除去未反应的H 2后进入第二换热单元6换热冷凝后在第二气液分离单元4中除去水分，剩余气体进入混气装置10，与空气和CO 2混合，在第三换热单元8换热升温后进入燃料电池单元9的阴极燃料进料口，阴极尾气进入第三换热单元8换热降温后由阴极尾气排出管排出。
本申请的工作原理如下：
该系统主要由燃料处理系统、燃料电池本体和阳极尾气循环及余热回收利用系统组成。
燃料处理系统主要包括甲醇重整制氢单元和水蒸气冷凝分离单元。甲醇重整制氢单元主要通过甲醇和水发生重整反应，该反应生成占比分别约为75％和25％的氢气和二氧化碳的混合气体(含水)，如下面反应方程式所示，生成主要成分为氢气和二氧化碳的混合气体，再通过冷凝分离出去甲醇重整气中的水分。
CH 3OH→CO+2H 2
H 2O+CO→CO 2+H 2
CH 3OH+H 2O→CO 2+3H 2
熔融碳酸盐燃料电池堆本体工作于650℃，阳极采用富氢气体为燃料，本专利则采用甲醇重整气作为阳极燃料，甲醇重整气中的二氧化碳不参与反应；阴极采用二氧化碳和氧气(来自空气)为原料，并在燃料电池内部发生电化学反应。
尾气循环单元主要是指阳极尾气首先经过催化燃烧出去未反应的氢气，再经过换热冷凝分离出去阳极尾气中的水蒸气，此时阳极尾气中的主要成分为二氧化碳。再将此阳极尾气与阴极进气混合，作为阴极原料被再次利用。
余热回收利用单元主要利用熔融碳酸盐燃料电池高温阳极尾气和高温阴极尾气余热，首先对熔融碳酸盐燃料电池阳极进气和阴极进气进行余热，完成余热后燃料电池尾气中剩余的低品位热量和甲醇重整气的低品位热量可以与冷水 进行换热，用于供暖、溴化锂制冷等。
以上所述，仅为本申请实施方式中的部分，本申请中虽然使用了部分术语，但并不排除使用其它术语的可能性。使用这些术语仅仅是为了方便的描述和解释本申请的本质，把它们解释成任何一种附加的限制都是与本申请精神相违背的。以上所述仅以实施例来进一步说明本申请的内容，以便于更容易理解，但不代表本申请的实施方式仅限于此，任何依本申请所做的技术延伸或再创造，均受本申请的保护。

Claims (10)

  1. 一种直接利用甲醇重整气的燃料电池系统，其特征在于，包括甲醇重整反应单元(1)、第一换热单元(2)、第一气液分离单元(3)、第二气液分离单元(4)、催化燃烧单元(5)、第二换热单元(6)、第三换热单元(8)、燃料电池单元(9)和混气装置(10)；
    甲醇重整反应单元(1)的进口连接有甲醇进料管，甲醇重整反应单元(1)的出口与第一换热单元(2)的热侧进口连接，第一换热单元(2)的热侧出口与第一气液分离单元(3)的进口连接，第一气液分离单元(3)的气相出口与第二换热单元(6)的冷侧进口连接，第二换热单元(6)的冷侧出口与燃料电池单元(9)的阳极燃料进料口连接，燃料电池单元(9)的阳极尾气出口与催化燃烧单元(5)的进口连接，催化燃烧单元(5)的进口还连接有O 2进气管，催化燃烧单元(5)的出口与第二换热单元(6)的热侧进口连接，第二换热单元(6)的热侧出口与第二气液分离单元(4)的进口连接，第二气液分离单元(4)的气相出口与混气装置(10)的进口连接，混气装置(10)的进口还连接有空气进气管和CO 2进气管，混气装置(10)的出口与第三换热单元(8)的冷侧进口连接，第三换热单元(8)的冷侧出口与燃料电池单元(9)的阴极燃料进料口连接，燃料电池单元(9)的阴极尾气出口与第三换热单元(8)的热侧进口连接，第三换热单元(8)的热侧出口连接有阴极尾气排出管；第一气液分离单元(3)和第二气液分离单元(4)的液相出口均连接有冷凝水排出管。
  2. 根据权利要求1所述的直接利用甲醇重整气的燃料电池系统，其特征在于，第二换热单元(6)的冷侧出口与燃料电池单元(9)的阳极燃料进料口之间的连接管路上设有阳极气体流量检测及控制装置(12)，第三换热单元(8)的冷侧出口与燃料电池单元(9)的阴极燃料进料口之间的连接管路上设有阴极气体流量检测及控制装置(13)，空气进气管上设有空气流量检测及控制装置(14)，CO 2进气管上设有CO 2流量检测及控制装置(15)，第二气液分离单元(4)的气相出口与混气装置(10)的进口之间的连接管路上设有阳极尾气流量 检测及控制装置(16)；阳极气体流量检测及控制装置(12)、阴极气体流量检测及控制装置(13)、空气流量检测及控制装置(14)、CO 2流量检测及控制装置(15)和阳极尾气流量检测及控制装置(16)均分别与系统的控制单元连接。
  3. 根据权利要求1所述的直接利用甲醇重整气的燃料电池系统，其特征在于，第二气液分离单元(4)的气相出口与混气装置(10)的进口之间的连接管路上设有压缩单元(7)。
  4. 根据权利要求3所述的直接利用甲醇重整气的燃料电池系统，其特征在于，压缩单元(7)进口前设有除沫装置。
  5. 根据权利要求1所述的直接利用甲醇重整气的燃料电池系统，其特征在于，第一换热单元(2)为气-液型换热器，第二换热单元(6)和第三换热单元(8)为气-气型换热器。
  6. 根据权利要求1所述的直接利用甲醇重整气的燃料电池系统，其特征在于，第一气液分离单元(3)和第二气液分离单元(4)的冷凝水出口均分别与第一换热单元(2)的冷侧入口连接。
  7. 根据权利要求6所述的直接利用甲醇重整气的燃料电池系统，其特征在于，甲醇重整反应单元(1)的出口与第一换热单元(2)的热侧进口之间的连接管路上设有温度检测装置，第一气液分离单元(3)和第二气液分离单元(4)的冷凝水出口与第一换热单元(2)的冷侧入口之间的连接管路上均分别设有流量检测及控制装置，温度检测装置和流量检测及控制装置均分别与系统的控制单元连接。
  8. 根据权利要求1所述的直接利用甲醇重整气的燃料电池系统，其特征在于，混合装置(10)内的壁面为圆滑曲面，混合装置(10)内设有扰流部件。
  9. 根据权利要求1所述的直接利用甲醇重整气的燃料电池系统，其特征在于，第二换热单元(6)与第二气液分离单元(4)之间设有第一余热换热器，阴极尾气排出管上设有第二余热换热器，第一余热换热器和第二余热换热器均 用于加热外部介质。
  10. 根据权利要求1～9任意一项所述的直接利用甲醇重整气的燃料电池系统的工作方法，其特征在于，包括：
    甲醇重整反应单元(1)发生甲醇重整反应，生成的混合气体进入第一换热单元(2)换热冷凝后，进入第一气液分离单元(3)中除去水分，得到含有氢气和二氧化碳的低温混合气体；低温混合气体在第二换热单元(6)中换热升温后进入燃料电池单元(9)的阳极燃料进料口，阳极尾气进入催化燃烧单元(5)除去未反应的H 2后进入第二换热单元(6)换热冷凝后在第二气液分离单元(4)中除去水分，剩余气体进入混气装置(10)，与空气和CO 2混合，在第三换热单元(8)换热升温后进入燃料电池单元(9)的阴极燃料进料口，阴极尾气进入第三换热单元(8)换热降温后由阴极尾气排出管排出。
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