US20030162065A1 - Fuel cell power generating device - Google Patents

Fuel cell power generating device Download PDF

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Publication number
US20030162065A1
US20030162065A1 US10/333,849 US33384903A US2003162065A1 US 20030162065 A1 US20030162065 A1 US 20030162065A1 US 33384903 A US33384903 A US 33384903A US 2003162065 A1 US2003162065 A1 US 2003162065A1
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Prior art keywords
fuel
heat
temperature
water
fuel cell
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US10/333,849
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English (en)
Inventor
Shinji Miyauchi
Masataka Ozeki
Koichi Nishimura
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Panasonic Corp
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Individual
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Priority claimed from JP2001176231A external-priority patent/JP4953405B2/ja
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Assigned to MATSUSHITA REFRIGERATION COMPANY, MATSUSHITA ELECTRIC INDUSTRIAL CO., LTD. reassignment MATSUSHITA REFRIGERATION COMPANY ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: MIYAUCHI, SHINJI, NISHIMURA, KOICHI, OZEKI, MASATAKA
Publication of US20030162065A1 publication Critical patent/US20030162065A1/en
Priority to US11/474,766 priority Critical patent/US7691512B2/en
Assigned to PANASONIC CORPORATION reassignment PANASONIC CORPORATION CHANGE OF NAME (SEE DOCUMENT FOR DETAILS). Assignors: MATSUSHITA ELECTRIC INDUSTRIAL CO., LTD.
Assigned to MATSUSHITA ELECTRIC INDUSTRIAL CO., LTD. reassignment MATSUSHITA ELECTRIC INDUSTRIAL CO., LTD. MERGER (SEE DOCUMENT FOR DETAILS). Assignors: MATSUSHITA REFRIGERATION COMPANY
Assigned to PANASONIC CORPORATION reassignment PANASONIC CORPORATION CHANGE OF NAME (SEE DOCUMENT FOR DETAILS). Assignors: MATSUSHITA ELECTRIC INDUSTRIAL CO., LTD.
Priority to US12/400,850 priority patent/US7816048B2/en
Abandoned legal-status Critical Current

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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/04Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313Processes 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
    • H01M8/0432Temperature; Ambient temperature
    • H01M8/04365Temperature; Ambient temperature of other components of a fuel cell or fuel cell stacks
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/04Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/04Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04007Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids related to heat exchange
    • H01M8/04029Heat exchange using liquids
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/04Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04119Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying
    • H01M8/04156Arrangements 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
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/04Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04007Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids related to heat exchange
    • H01M8/04067Heat exchange or temperature measuring elements, thermal insulation, e.g. heat pipes, heat pumps, fins
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/06Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/06Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0668Removal of carbon monoxide or carbon dioxide
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/50Fuel cells

Definitions

  • the present invention relates to a fuel-cell power-generation system of generating power or recovering exhaust heat by using a fuel cell.
  • symbol 1 denotes a fuel cell and a fuel treater 2 water-vapor-reforms a material such as a natural gas, generates a gas mainly containing hydrogen, and supplies the gas to the fuel cell 1 .
  • the fuel treater 2 is provided with a reformer 3 of generating a reformed gas and a carbon-monoxide shifter 4 of making carbon monoxide react with water to produce carbon dioxide and hydrogen.
  • a fuel-side humidifier 5 humidifies a fuel gas to be supplied to the fuel cell 1 .
  • Symbol 6 denotes an air feeder that supplies air serving as an oxidant to the fuel cell 1 .
  • an oxidation-side humidifier 7 humidifies supplied air.
  • the power-generation system is provided with a cooling pipe 8 of supplying water to the fuel cell 1 to cool it and a pump 9 of circulating the water in the cooling pipe 8 .
  • the exhaust heat due to the power generation in the fuel cell 1 recovers in a hot-water storage tank 13 via an exhaust-heat recovery pipe 12 by a heat exchanger 10 and a circulating pump 11 under the connection of the system.
  • the fuel treater 2 When generating power by the above system, the fuel treater 2 requires water in order to water-vapor-reform a material such as a natural gas by the reformer 3 and moreover make the carbon monoxide contained in the reformed gas react with water by means of the carbon-monoxide shifter 4 to produce carbon dioxide and hydrogen, the fuel-side humidifier 5 requires water to humidify a fuel gas to be supplied to the fuel cell 1 , and the oxidation-side humidifier 7 requires water in order to humidify supplied air.
  • the water required for the above power generation has been supplied as city water or ion exchange water from the outside.
  • the above conventional configuration has a problem that a reformation catalyst or shift catalyst stored in the reformer 3 or carbon-monoxide shifter 4 of the fuel treater 2 is deteriorated due to chlorine ions or metallic ions eluted from a pipeline when using general water such as city water in the fuel-gas pipeline or oxidant-gas pipeline of the fuel cell 1 , or a fuel gas or oxidant gas is ionized and electric conductivity is raised to cause a trouble in power generation by the fuel cell.
  • a power-generation system using a conventional fuel cell has the following disadvantages.
  • the system stops supply of a power-generation material to a fuel generator 2 and at the same time, supplies an inert gas such as nitrogen to the fuel generator 2 and circulation channels of a material gas and fuel gas of the fuel cell 1 and exhausts a combustible gas from the fuel-cell power-generation system.
  • an inert gas such as nitrogen
  • the cooling-water pump 9 and city-water pump 11 stop their carrying operations and circulation of cooling water and city water stops.
  • an inert gas such as nitrogen coming out of the fuel generator 2 at approx. 700 ° C. through the circulation channel of a fuel gas passes through the fuel cell 1 and is exhausted to the outside from the fuel cell 1 .
  • the fuel cell 1 keeps a temperature of approx. 70° C. for a while. Because the temperature is higher than an environmental temperature and the heat retained by the fuel cell 1 is only exhausted to the outside after circulation of cooling water is stopped. Therefore, it is necessary to use the heat of the fuel cell 1 also after power generation in order to effectively use the heat produced for the power generation.
  • the present invention is achieved to solve the above problems and its object is to provide a fuel-cell power-generation system not causing a trouble of lowering the power-generation efficiency of a fuel cell after power generation is completed.
  • a first aspect of the present invention is a fuel-cell power-generation system comprising:
  • a second aspect of the present invention is the fuel-cell power-generation system according to the first aspect of the present invention, comprising:
  • circulation means of circulating said heat transport medium between said heat exchange means and said heat-using means are provided.
  • a third aspect of the present invention is the fuel-cell power-generation system according to the second aspect of the present invention, wherein
  • said heat transport medium is constituted so as to pass through said condenser and contribute to condensation of the said unused exhaust gas in said condenser, and condensation-capacity detection means of detecting the condensation capacity of said condenser and control means of controlling the output of said circulation means in accordance with a detection signal of said condensation-capacity detection means are comprised.
  • water can be self-supported without using outside water by using the recover water obtained by condensing water by a condenser for the water for water-vapor reformation by the reformer of a fuel treater, the water of making carbon monoxide react with water to produce carbon dioxide and hydrogen, the water of humidifying the fuel gas to be supplied to a fuel cell, and the water for humidifying supplied air by an oxidation-side humidifier.
  • ion removal means such as ion exchange resins for removing chlorine ions from general water such as city water in a fuel-gas supply system and oxidant-gas supply system or preventing the deterioration of an ion-removing capacity according to operation time.
  • ion removal means such as ion exchange resins for removing chlorine ions from general water such as city water in a fuel-gas supply system and oxidant-gas supply system or preventing the deterioration of an ion-removing capacity according to operation time.
  • a fourth aspect of the present invention is the fuel-cell power-generation system according to the third aspect of the present invention, wherein
  • said condensation-capacity detection means is condensed-water-temperature detection means of detecting the temperature of condensed water supplied from said condenser.
  • a fifth aspect of the present invention is the fuel-cell power-generation system according to the fourth aspect of the present invention, further comprising:
  • medium-temperature detection means of detecting a temperature of said heat transport medium recovering exhaust heat in said heat exchange means, and wherein said control means controls the output of said circulation means by also using the temperature of said heat transport medium detected by said medium-temperature detection means.
  • a sixth aspect of the present invention is the fuel-cell power-generation system according to the third aspect of the present invention, wherein
  • said condensation-capacity detection means is medium-temperature detection means of detecting the temperature of said heat transport medium coming into said condenser or medium-temperature detection means of detecting the temperature of said heat transport medium going out of said condenser.
  • the output of circulation means is controlled by control means to store the exhaust heat of a fuel cell in heat-using means by assuming that a condensation capacity is sufficient.
  • the circulation means is stopped to complete exhaust-heat recovery by assuming that the condensation capacity is deteriorated.
  • a seventh aspect of the present invention is the fuel-cell power-generation system according to the third aspect of the invention, wherein
  • said condensation-capacity detection means is heat-using-temperature detection means of detecting the temperature of said heat-using means.
  • a seventh aspect of the present invention when the temperature detected by heat-using temperature detecting means is equal to or lower than a predetermined temperature, the output of the circulation means is continuously controlled by control means and stored in the heat-using means of a fuel cell by assuming that a condensation capacity is sufficient. Moreover, when the temperature detected by the heat-using temperature detecting means is equal to or higher than the predetermined temperature, the circulation means is stopped by the control means to complete exhaust heat recovery by assuming that the condensation capacity is deteriorated.
  • An eighth aspect of the present invention is the fuel-cell power-generation system according to the third aspect of the present invention, wherein
  • said condensation-capacity detection means is medium-temperature detection means of detecting the temperature of said heat transport medium recovering exhaust heat in said heat exchange means.
  • the output value of circulation means is obtained by using the temperature of a heat-transport medium detected by medium-temperature detection means.
  • the output value of the circulation means is continuously controlled by control means and stored in the heat-using means of a fuel cell by assuming that a condensation capacity is sufficient.
  • the circulation means is stopped by the control means to complete exhaust heat recovery
  • a ninth aspect of the present invention is the fuel-cell power-generation system according to the first aspect of the present invention, wherein
  • the unused exhaust gas to be condensed by said condenser is at least either of an oxidant gas and a fuel gas.
  • a tenth aspect of the present invention is the fuel-cell power-generation system according to the first aspect of the present invention, wherein cooling is continued until the temperature of said fuel cell becomes a predetermined threshold value or less even after supply of said fuel and said oxidant to said fuel cell is stopped.
  • An eleventh aspect of the present invention is the fuel-cell power-generation system according to the first aspect of the present invention, further comprising:
  • a cooling-circulation system through which a first heating medium set, so as to pass through said fuel cell and to carry the heat of said fuel cell, circulates;
  • temperature detection means of directly or indirectly detecting the temperature of said fuel cell
  • said heat-medium circulation means operates at least until the temperature detected by said temperature detection means becomes a predetermined threshold value or less after supply of said fuel and said oxidant to said fuel cell is stopped.
  • a twelfth aspect of the present invention is the fuel-cell power-generation system according to the eleventh aspect of the present invention, wherein
  • said heat release means has a heat exchanger of performing heat exchange between said first heating medium and a second heating medium
  • said heat exchanger performs said heat exchange until the temperature detected by said temperature detection means becomes a predetermined threshold value or less after supply of said fuel and said oxidant to said fuel cell is stopped.
  • a thirteenth aspect of the present invention is the fuel-cell power-generation system according to the eleventh or the twelfth aspect of the present invention, wherein
  • the temperature detected by said temperature detection means is the temperature of said first heating medium or said cooling-circulation system.
  • a fourteenth aspect of the present invention is the fuel-cell power-generation system according to the twelfth aspect of the present invention, wherein
  • the temperature detected by said temperature detection means is the temperature of said second heating medium.
  • a fifteenth aspect of the present invention is a fuel-cell power-generation system, comprising:
  • a cooling-circulation system through which a first heating medium set, so as to pass through said fuel cell and to carry the heat of said fuel cell, circulates;
  • At least either of said heating-medium circulation means and said heat release means continuously operates until the temperature detected by said temperature detection means becomes a predetermined threshold value or less even after supply of said fuel and said oxidant to said fuel cell is stopped.
  • FIG. 1 is a block diagram of a fuel-cell power-generation system of embodiment 1 of the present invention.
  • FIG. 2 is a block diagram of a fuel-cell power-generation system of embodiment 2 of the present invention.
  • FIG. 3 is a block diagram of a fuel-cell power-generation system of embodiment 3 of the present invention.
  • FIG. 4 is a block diagram of a fuel-cell power-generation system of embodiment 4 of the present invention.
  • FIG. 5 is a block diagram of a fuel-cell power-generation system of embodiment 5 of the present invention
  • FIG. 6 is a block diagram showing a fuel-cell power-generation system of an embodiment of the present invention
  • FIG. 7 is a flow chart showing an operation mode under and after power generation by a fuel-cell power-generation system of embodiment 6 of the present invention
  • FIG. 8 is a flowchart showing an operation mode under and after power generation by a fuel-cell power-generation system of embodiment 7 of the present invention.
  • FIG. 9 is a block diagram of a conventional fuel-cell power-generation system. Description of symbols 1 Fuel cell 10 Heat exchange means 11 Heat-transport-medium circulation means 13 Heat-using means 14 Condenser 15 Water-using means 18 Condensation-capacity detection means 19 Control means 32 Fuel generator 33 Blower 34 Cooling pipe 35 Cooling-water pump 36 Heat exchanger 37 Hot-water storage tank 38 City-water pipe 39 City-water pump 310 Fuel-cell-temperature detector 311 City-water-temperature detector 100 Cooling system
  • FIG. 1 is a block diagram of a fuel-cell power-generation system of embodiment 1 of the present invention.
  • FIG. 1 components having the same functions as the power generation system using the conventional fuel cell shown in FIG. 9 are provided with the same symbol and descriptions of details of the functions are omitted by assuming that the functions conform to those in FIG. 9.
  • Symbol 14 denotes a condenser of condensing and heat-exchanging the water vapor contained in an unused exhaust gas (oxidant gas) exhausted from a fuel cell 1
  • 15 denotes water-using means of water-vapor-reforming the condensed water discharged from the condenser 14 by the reformer 3 of the fuel treater 2 , making carbon monoxide in a reformed gas react with water by the carbon-monoxide shifter 4 to produce carbon dioxide and hydrogen, and humidifying the fuel gas to be supplied to the fuel cell 1 by the fuel-side humidifier 5 and the supplied air by the oxidation-side humidifier 7 respectively.
  • the water-using means 15 is constituted by a condensed-water tank 16 of storing condensed water, and a condensed-water pump 17 of supplying condensed water to the fuel treater 2 , fuel-side humidifier 5 , and air-side humidifier 7 .
  • Symbol 18 denotes condensation-capacity detection means of detecting the condensation capacity of the condenser 14 , which always monitors the quantity of condensed water for unit time from the condenser 14 .
  • Symbol 19 denotes control means of controlling the output of heat-transport-medium circulation means (hereafter referred to as circulation pump 11 ) and thereby controlling the quantity of circulation water of a heat transport medium (circulation water), making heat-using means (hereafter referred to as hot-water storage tank) 13 recover the exhaust heat of the fuel cell 1 through the exhaust-heat recovery pipe 12 , and receiving a condensation-capacity detection signal of the condensation-capacity detection means 18 .
  • circulation pump 11 heat-transport-medium circulation means
  • hot-water storage tank 13 heat-using means
  • the fuel-cell power-generation system When the fuel-cell power-generation system operates (generates power), it circulates the heat generated by the fuel cell 1 during power generation as cooling water through the pump 9 and makes the heat transport medium (circulation water of city water stored in the hot-water storage tank 13 ) flowing through the exhaust-heat recovery pipe 12 heat-carry the heat by the heat exchange means 10 .
  • an oxidant gas is humidified by the oxidation-side humidifier 7 by the air feeder 6 and supplied to the fuel cell 1 .
  • the unused gas not contributing to the power generation by the fuel cell 1 is heat-exchanged with a heat transport medium (circulation water of city water) flowing through the exhaust-heat recovery pipe 12 by the condenser 14 similarly to the case of the heat exchange means 10 , and the water is condensed and recovered in the condensed-water tank 16 of the water-using means 15 as condensed water.
  • a heat transport medium circulation water of city water
  • the control means 19 receives a condensation-capacity detection signal from the condensation-capacity detection means 18 .
  • the control means 19 controls the output of the circulation pump 11 and recovers the exhaust heat of the fuel cell 1 through the exhaust-heat recovery pipe 12 .
  • the dew point of the unused gas exhausted from the fuel cell 1 is lower and the heat capacity of the unused gas exhausted from the fuel cell 1 is smaller, compared with the temperature of the cooling water in the cooling pipe 8 which is almost equal to the operating temperature of the fuel cell 1 under power generation (approx. 70° to 80° C. for a polymer electrolytic fuel cell) and the heat capacity of the cooling water. Therefore, heat exchange of the circulation water from the hot-water storage tank 13 is performed in order of the condenser 14 first and then heat exchange means 10 .
  • the control means 19 detects that a condensation-capacity detection signal output from the condensation-capacity detection means 18 becomes a predetermined value or less, confirms that the recovered quantity of condensed water is decreased due to reduction of the condensation capacity of the condenser 14 , and stops the power generation and exhaust-heat recovery by the fuel cell 1 .
  • the condenser 14 condenses the unused exhaust gas exhausted from the fuel cell 1 to recover water
  • the condensation-capacity detection means 18 always monitors the condensation capacity of the condenser
  • the control means 19 controls the output of the circulation pump 11 to store the exhaust heat of the fuel cell 1 when sufficiently having a condensation capacity and stops the circulation pump 11 and completes exhaust-heat recovery when the condensation capacity lowers.
  • water can be self-supported without taking in water from the outside-by using the recovered water obtained by condensing the water for humidifying supplied air by the condenser 14 for the water for reformation and shift to the reformer 3 and carbon-monoxide shifter 4 of the fuel treater 2 , supplied gas at the fuel-side humidifier 5 and oxidation-side humidifier 7 .
  • the condenser 14 is constituted so as to condense only an oxidant gas among unused exhaust gases of the fuel cell 1 .
  • the same advantage can be also obtained by adding a configuration of condensing the unused exhaust gas of a fuel gas. It is also allowed to condense only the fuel gas.
  • FIG. 2 is a block diagram of a fuel-cell power-generation system of embodiment 2 of the present invention.
  • components having functions same as those of the conventional fuel-cell power-generation system shown in FIG. 9 and the fuel-cell power-generation system of the embodiment 1 shown in FIG. 1 are provided with the same symbol and descriptions of details of those functions are omitted by assuming that the functions conform to those described for FIGS. 9 and 1.
  • Symbol 20 denotes exhaust-heat-recovery-temperature detection means of detecting the temperature of a heat transport medium at the exit of an exhaust-heat recovery pipe 12 connected to heat exchange means 10 so as to output the exhaust-heat recovery temperature for a hot-water storage tank 13 to control means 19 .
  • the heat generated by a fuel cell 1 during power generation is circulated as cooling water through a pump 9 and the heat exchange means 10 makes a heat transport medium (circulation water of city water stored in the hot-water storage tank 13 ) flowing through an exhaust-heat recover pipe 12 carry the heat.
  • an oxidant gas is humidified in an oxidation-side humidifier 7 by an air feeder 6 and supplied to a fuel cell 1 .
  • the unused gas not contributing to the power generation by the fuel cell 1 is heat-exchanged with a heat transport medium (circulation water of city water) flowing through the exhaust-heat recovery pipe 12 by a condenser 14 similarly to the case of the heat exchange means 10 , and moisture is condensed and recovered in a condensed-water tank 16 of water-using means 15 as condensed water.
  • a heat transport medium circulation water of city water
  • the control means 19 receives a condensation-capacity detection signal from condensation-capacity detection means 18 and when the condensation capacity of the condenser 14 is equal to or more than a predetermined value, that is, when the quantity of high-temperature water due to exhaust-heat recovery to the hot-water storage tank 13 is small, or when the temperature of circulation water coming into the condenser 14 from the hot-water storage tank 13 is low, controls the output of a circulation pump 11 so that the exhaust-heat recovery temperature by exhaust-heat-recovery-temperature detection means 20 becomes a predetermined value (60° to 80° C. in the case of a polymer electrolytic fuel cell), and recovers the exhaust heat of the fuel cell 1 through the exhaust-heat recovery pipe 12 . That is, hot water is stored in a laminated state at a predetermined stored hot-water temperature (60° to 80° C.) from the upper portion of the hot-water storage tank 13 .
  • a predetermined value that is, when the quantity of high-temperature water due to exhaust
  • the control means 19 receives that a condensation-capacity detection signal output from the condensation-capacity detection means 18 becomes a predetermined value or less, and confirms that hot-water storage due to exhaust heat recovery to the hot-water storage tank 13 is almost completed and a storage volume of condensed water is lowered by the drop of condensation capacity of the condenser 14 , and then stops the output of the circulation pump 11 and the power generation and exhaust heat recovery by the fuel cell 1 .
  • the condenser 14 condenses the unused exhaust gas exhausted from the fuel cell 1 to recover water
  • the condensation-capacity detection means 18 always monitors the condensation capacity of the condenser 14
  • the control means 19 controls the output of the circulation pump 11 and stores the exhaust heat of the fuel cell 1 in the hot-water storage tank 13 when a sufficient condensation capacity is left, and stops the circulation pump 11 to complete exhaust heat recovery when the condensation capacity decreases.
  • water can be self-supported without taking in water from the outside by using the recovered water obtained by condensing the water by the condenser 14 for the water for reformation and shift to be supplied to the reformer 3 and carbon-monoxide shifter 4 of the fuel treater 2 and for the water for humidifying supplied air and supplied gas at the fuel-side humidifier 5 and the oxdation-side humidifier 7 .
  • ion removal means such as ion exchange resin for removing chlorine ions from general water such as city water in a fuel-gas supply system and oxidant-gas supply system or by reducing deterioration of ion removal capacity proportionate to work time.
  • ion removal means such as ion exchange resin for removing chlorine ions from general water such as city water in a fuel-gas supply system and oxidant-gas supply system or by reducing deterioration of ion removal capacity proportionate to work time.
  • the exhaust-heat-recovery-temperature detection means 20 controls an exhaust-heat recovery temperature so that it becomes a predetermined temperature and the control means 19 controls the output of the circulation pump 11 , it is possible to store hot water in the hot-water storage tank 13 in a laminated state from the upper portion.
  • humidified exhaust gas air of 60° to 65° C. is obtained as the temperature of unused exhaust gas after chemical reaction with the fuel cell 1 while the fuel cell is operated and when heat-exchanging the air with water serving as a heat transport medium by the condenser 14 , a temperature rise of 15° to 20° C. is obtained when keeping the flow rate of the heat transport medium at 0.8 to 1.0 L/min.
  • After performing heat exchange by the condenser 14 by further performing heat exchange by the heat exchange means 10 , it is possible to raise the temperature up to the vicinity of a cooling-water circulation temperature (70° to 80° C.) Therefore, the exhaust-heat recovery efficiency of the fuel cell 1 is further improved.
  • the condenser 14 is constituted so as to condense only the oxidant gas among unused exhaust gases of the fuel cell 1 .
  • the same advantage can be obtained by additionally using a configuration of condensing the unused exhaust gas of a fuel gas. Moreover, it is allowed to condense only a fuel gas.
  • FIG. 3 is a block diagram of a fuel-cell power-generation system of embodiment 3 of the present invention.
  • FIG. 3 components having the same functions as those of the conventional fuel-cell power-generation system shown in FIG. 9 and the fuel-cell power-generation system of the embodiment 1 shown in FIG. 1 are provided with the same symbol. Descriptions of details of those functions are omitted by assuming that the functions conform to those shown in FIGS. 9 and 1.
  • Symbol 21 denotes condensation-capacity detection means of detecting the condensation capacity of a condenser 14 , which is a thermistor serving as condenser-temperature detection means of detecting the entrance temperature of a heat transport medium to the condenser 14 .
  • the heat due to power generation by a fuel cell 1 is circulated as cooling water through a pump 9 and heat-exchange means 10 makes a heat transport medium (circulation water of city water stored in a hot-water storage tank 13 ) flowing through an exhaust-heat recovery pipe 12 carry heat.
  • an oxidant gas is humidified by an oxidation-side humidifier 7 and supplied to the fuel cell 1 by an air feeder 6 .
  • the unused gas not contributing to the power generation by the fuel cell 1 is heat-exchanged with a heat transport medium (circulation water of city water) flowing through the exhaust-heat recovery pipe 12 by means of the condenser 14 similar to the case of the heat exchange means 10 , and moisture is condensed and recovered by a condensed-water storage tank 16 of water-using means 15 as condensed water.
  • the control means 19 receives a condensation-capacity detection signal (condenser entrance temperature of heat transport medium) from condenser-temperature detection means 21 and when the entrance temperature is sufficiently lower than the exhaust-gas temperature (60° to 65° C.), that is, when the quantity of high-temperature water due to exhaust heat recovery to the hot-water storage tank 13 is small, determines that the condensation capacity of the condenser 14 is equal to or more than a predetermined value, controls the output of a circulation pump 11 , and recovers the exhaust heat of the fuel cell 1 through the exhaust-heat recovery pipe 12 .
  • a condensation-capacity detection signal condenser entrance temperature of heat transport medium
  • the exhaust-gas temperature 60° to 65° C.
  • the condensation capacity of the condenser 14 is equal to or less than a predetermined value, that is, when the quantity of high-temperature water due to exhaust-heat recovery to the hot-water storage tank 13 increases, the condensation-capacity detection signal (condenser entrance temperature of heat transport medium) of the condenser-temperature detection means 21 becomes a predetermined value or more and the control means 19 confirms that the quantity of recovered condensed water is decreased due to deterioration of the condensation capacity of the condenser 14 , stops the output of the circulation pump 11 , and stops the power generation and exhaust heat recovery by the fuel cell 1 .
  • the condenser 14 condenses the unused exhaust gas exhausted from the fuel cell 1 to recover water, and simultaneously the condenser-temperature detection means 21 always monitors the condensation capacity of the condenser 14 , the control means 19 controls the output of the circulation pump 11 to store the exhaust heat of the fuel cell 1 in the hot-water storage tank 13 when a sufficient condensation capacity is left, and stops the circulation pump 11 to complete the exhaust-heat recovery when the condensation capacity is decreased.
  • the condenser-temperature detection means can be realized by a simple configuration such as adding a thermistor to the entrance of the condenser 14 , it is possible to downsize and rationalize the fuel-cell power-generation system.
  • the condenser-temperature detection means of detecting the condensation capacity of the condenser 14 is constituted so as to detect the entrance temperature of the heat transport medium to the condenser 14 .
  • the same advantage is obtained by using a configuration of detecting the exit temperature of the heat transport medium of the condenser 14 .
  • FIG. 4 is a block diagram of a fuel-cell power-generation system of embodiment 4 of the present invention.
  • FIG. 4 components having the same functions as those of the conventional fuel-cell power-generation system shown in FIG. 9 and the fuel-cell power-generation system of the embodiment 1 shown in FIG. 1 are provided with the same symbol and descriptions of details of those functions are omitted by assuming that the functions conform to those in FIGS. 9 and 1.
  • Symbols 22 , 23 , and 24 denote condensation-capacity detection means of respectively detecting the condensation capacity of a condenser 14 and are thermistors serving as a plurality of heat-using-temperature detection means provided to confirm a stored-heat-temperature distribution due to exhaust heat recovery by a hot-water storage tank 13 .
  • the fuel-cell power-generation system When the fuel-cell power-generation system operates (generates power), it circulates the heat generated by a fuel cell 1 during power generation as cooling water through a pump 9 and heat exchange means 10 makes a heat transport medium (circulation water of city water stored in a hot-water storage tank 13 ) flowing through an exhaust-heat recovery pipe 12 carry heat.
  • a heat transport medium circulation water of city water stored in a hot-water storage tank 13
  • an oxidant gas is humidified by an oxidation-side humidifier 7 and supplied to the fuel cell 1 .
  • the unused gas not contributing to the power generation by the fuel cell 1 is heat-exchanged with a heat transport medium (circulation water of city water) flowing through an exhaust-heat recovery pipe 12 by a condenser 14 as is the case of the heat exchange means 10 , and moisture is condensed and recovered as condensed water by a condensed-water tank 16 of water-using means 15 .
  • Control means 19 receives a stored-heat-temperature-distribution detection signal from heat-using-temperature detection means 22 , 23 , or 24 and when the condensation capacity of the condenser 14 is equal to or more than a predetermined value, that is, when the quantity of high-temperature water due to exhaust heat recovery to a hot-water storage tank 13 is small (when the detection temperature of the heat-using-temperature detection means 24 closest to the circulation-water suction port of the exhaust-heat recovery pipe 12 among the heat-using-temperature detection means 22 , 23 , and 24 is equal to or lower than a predetermined value), controls the output of a circulation pump 11 and recovers exhaust heat of the fuel cell 1 through the exhaust-heat recovery pipe 12 .
  • the control means 19 estimates deterioration of the condensation capacity of the condenser 14 (decrease in the quantity of recovered condensed water) due to a rise of the circulation-water temperature of the exhaust-heat recovery pipe 12 , stops the output of the circulation pump 11 , and stops the power generation and exhaust heat recovery by the fuel cell 1 .
  • the condenser 14 condenses the unused exhaust gas exhausted from the fuel cell 1 and recovers water
  • the heat-using-temperature detection means 22 , 23 , and 24 always monitor the condensation capacity of the condenser 14
  • the control means 19 controls the output of the circulation pump 11 and stores the exhaust heat of the fuel cell 1 in he hot-water storage tank 13 when a sufficient condensation capacity is left and stops the circulation pump 11 to complete the exhaust heat recovery when the condensation capacity is deteriorated.
  • the condenser-temperature detection means can be also used as a thermistor serving as the heat-using-temperature detection means of confirming the stored-heat temperature distribution of the heat-using means (hot-water storage tank), it is possible to downsize and rationalize the fuel-cell power-generation system.
  • FIG. 5 is a block diagram of a fuel-cell power-generation system of embodiment 5 of the present invention.
  • FIG. 5 components having the same functions as those of the conventional fuel-cell power-generation system shown in FIG. 9 and the fuel-cell power-generation system of the embodiment 2 shown in FIG. 2 are provided with the same symbol and descriptions of details of those functions are omitted by assuming that the functions conform to those in FIGS. 9 and 2.
  • control means 19 receives an exhaust-heat recovery temperature from exhaust-heat-recovery-temperature detection means 20 of detecting the temperature of a heat transport medium at the exit side of an exhaust-heat recovery pipe 12 connected to heat exchange means 10 and controls the output of a circulation pump 11 so that an exhaust-heat temperature becomes a predetermined value (60° to 80° C.) condensation-capacity detection means is constituted so as to detect a condensation capacity by using the fact that a value output to the circulation pump 11 correlates with a circulation-water temperature at the suction side of the circulation pump 11 of the exhaust-heat recovery pipe 12 .
  • the circulation pump 11 slowly rotates.
  • the circulation pump 11 quickly rotates in order to keep the above exhaust-heat recover temperature at the predetermined value (60° to 80° C.)
  • the fuel-cell power-generation system When the fuel-cell power-generation system operates (generates power), it circulates the heat generated by a fuel cell 1 during power generation as cooling water through a pump 9 and the heat exchange means 10 makes a heat transport medium (circulation water of city water stored in a hot-water storage tank 13 ) carry heat.
  • a heat transport medium circulation water of city water stored in a hot-water storage tank 13
  • an oxidant gas is humidified by an oxidation-side humidifier 7 and supplied to the fuel cell 1 by an air feeder 6 .
  • the unused gas not contributing to the power generation by the fuel cell 1 is heat-exchanged with a heat transport medium (circulation water of city water) flowing through the exhaust-heat recovery pipe 12 by the condenser 14 as is the case of the heat exchange means 10 , and moisture is condensed and recovered by the condensed-water tank 16 of water-using means 15 as condensed water.
  • a heat transport medium circulation water of city water
  • the control means 19 receives an exhaust-heat recovery temperature from the exhaust-heat-recovery-temperature detection means 20 of detecting the temperature of a heat transport medium at the exit side of the exhaust-heat recovery pipe 12 and when the condensation capacity of the condenser 14 is equal to or more than a predetermined value, that is, when the quantity of high-temperature water due to exhaust heat recovery to the hot-water storage tank 13 is small, or the output value of the circulation pump 11 to be output so that an exhaust-heat recovery temperature is always kept at a predetermined temperature (60° to 80° C.) is equal to or less than a predetermined value, controls the output of the circulation pump 11 , and recovers exhaust heat of the fuel cell 1 through the exhaust-heat recovery pipe 12 .
  • a predetermined value 60° to 80° C.
  • the control means 19 estimates deterioration of the condensation capacity of the condenser 14 due to a rise of the circulation-water temperature (decrease of quantity of recovered condensed water) of the exhaust-heat recovery pipe 12 , stops the output of the circulation pump 11 , and stops the power generation and exhaust heat recovery by the fuel cell 1 .
  • the condenser 14 condenses the unused exhaust gas exhausted from the fuel cell 1 to recover water and receives an exhaust-heat recovery temperature from the exhaust-heat-recovery-temperature detection means 20 , the control means 19 of controlling the output of the circulation pump 11 always monitors the condensation capacity of the condenser 14 , and the control means 19 controls the output of the circulation pump 11 and stores the exhaust heat of the fuel cell 1 in the hot-water storage tank 13 when a sufficient condensation capacity is left and stops the circulation pump 11 to complete exhaust heat recovery when the condensation capacity lowers.
  • the exhaust-heat-temperature detection means 20 makes it possible to also use the control means 19 as condenser-temperature detection means because a value output to the circulation pump correlates with a circulation temperature of the circulation pump at the suction side of the exhaust-heat recovery pipe by using the fact that the control means 19 receives an exhaust-heat recovery temperature from the exhaust-heat-recovery-temperature detection means of detecting the temperature of a heat transport medium at the exit side of the exhaust-heat recovery pipe 12 and controls the output of the circulation pump 11 so that the exhaust-heat recovery temperature becomes a predetermined temperature (60° to 80 ° C.). Therefore, it is possible to further downsize and rationalize the fuel-cell power-generation system.
  • FIG. 6 is an illustration showing a configuration of a fuel-cell power-generation system of sixth embodiment of the present invention.
  • the fuel-cell power-generation system of this embodiment is provided with a fuel cell 1 of generating power by using a fuel gas and an oxidant, a fuel generator 32 of generating a hydrogen-rich fuel gas by adding water to a power-generation material such as a natural gas and reforming the material, a blower 33 of supplying air to the fuel cell 1 as an oxidant, a cooling pipe 34 of supplying cooling water serving as a first heating medium of taking out the heat generated by the fuel cell 1 to the outside to the fuel cell 1 , a cooling-water pump 35 located at the cooling pipe 34 to carry cooling water, a heat exchanger 36 of transferring the heat of the cooling water serving as the first heating medium to city water serving as a second heating medium, a hot-water storage tank 37 of storing city water, a city-water pipe 38 of connecting the heat exchanger 36 with the hot-water storage tank 37 , and a city-water pump 39 of carrying city water.
  • a fuel cell 1 of generating power by using a fuel gas and an oxidant
  • FIG. 7 is a flowchart showing operation modes of the cooling-water pump 35 and city-water pump 39 while the fuel-cell power-generation system of the embodiment 6 of the present invention generates power and after power generation is stopped.
  • the fuel cell 1 generates power and heat using the hydrogen-rich fuel gas generated by the fuel generator 32 and the air supplied by the blower 33 .
  • the fuel generator 32 Because the fuel generator 32 generates a hydrogen-rich fuel gas by adding water to a power-generation material such as a natural gas, it is kept at a high temperature (approx. 700° C.) by a burner (not illustrated).
  • the heat generated by the fuel cell 1 is carried to the outside by the cooling water flowing through the cooling pipe 34 .
  • the flow rate of the cooling water adjusts the carrying capacity of the cooling pump 35 for the temperature Tf of the cooling water detected by a fuel-cell-temperature detector 10 set to a position where the cooling water flows out of the fuel cell 1 to coincide with a target temperature Tr1 (approx. 70° C.).
  • Tr1 approximately equal to the temperature of the cooling water flowing out of the fuel cell 1
  • the heat obtained by the cooling water is transferred to the city water flowing through the city-water pipe 38 through the heat exchanger 36 .
  • the flow rate of the city water adjusts the carrying capacity of the city-water pump 39 so that the temperature Tw of city water detected by a city-water-temperature detector 311 set to a position where the city water flows out of the heat exchanger 36 coincides with a target temperature Tr2 (approx.
  • a fuel-cell-temperature detector 310 detects the temperature Tf of the cooling water flowing out of the fuel cell 1 corresponding to the temperature of the fuel cell 1 under power generation ( 001 ).
  • the city-water detector 311 detects the temperature Tw of the city water flowing out of the heat exchanger 36 ( 003 ).
  • the city-water carrying capacity of the city-water pump 39 is increased but when the detected temperature Tw is lower than the target temperature Tr2, the city-water carrying capacity of the city-water pump 39 is decreased ( 004 ).
  • it is allowed to operate the city-water pump 39 by using a generally-used PID controller and thereby computing the city-water carrying power of the city-water pump 39 so that the temperature Tw of the city water may be consistent with the target temperature Tr2.
  • a system controller determines whether power generation by the fuel-cell power-generation system is stopped ( 005 ). When power generation is in operation, step 002 is restarted to repeat operations according to the above flow.
  • the fuel-cell-temperature detector 310 compares the temperature Tf of cooling water with a predetermined threshold temperature Te1 (approx. 60° C.) ( 006 ) and when the temperature Tf of the cooling water is higher than the threshold temperature Te1 (approx. 60° C.), and returns to step 002 to repeat operations according to the above flow.
  • the cooling-water pump 35 and city-water pump 39 for carrying the heat generated by the fuel cell 1 to the outside continues operations even if the power generation by the fuel cell 1 is stopped. Therefore, even if an inert gas such as nitrogen is supplied to the fuel cell 1 through circulation paths of the material gas and fuel gas of the fuel generator 32 and fuel cell 1 , the heat held by the inert gas and the high-temperature remaining fuel gas to be carried by the inert gas is exhausted to the outside through cooling water. Therefore, the fuel cell 1 does not even locally become high in temperature. Therefore, even if the solid polymer type is used for the fuel cell 1 , a solid polymer film is not dried or the power-generation efficiency of the fuel cell 1 is not extremely deteriorated.
  • an inert gas such as nitrogen
  • FIG. 6 is used for the description of this embodiment and the fuel-cell power-generation system of the embodiment 6 of the present invention applies to the detailed description of this embodiment.
  • FIG. 8 is a flowchart showing operation modes of a cooling-water pump 35 and city-water pump 39 while the fuel-cell power-generation system of the embodiment 7 of the present invention generates power and after the power generation is stopped.
  • a fuel-cell-temperature detector 310 detects the temperature Tf of the cooling water flowing out of a fuel cell 1 corresponding to the temperature of the fuel cell 1 ( 001 ).
  • a city-water-temperature detector 311 detects the temperature Tw of the city water flowing out of a heat exchanger 36 ( 003 ).
  • the city-water carrying capacity of the city-water pump 39 is increased but when the detected temperature Tw is lower than the target temperature Tr2, the city-water carrying capacity of the city-water pump 39 is decreased ( 004 ).
  • it is allowed to operate the city-water pump 39 by using a generally-used PID controller and thereby, computing the city-water carrying power of the city-water pump 39 so that the temperature Tw of city water coincides with the target temperature Tr2.
  • a not-illustrated system controller determines whether the power generation by the fuel-cell power-generation system is stopped ( 005 ). When the power generation is continued, step 002 is restarted to repeat operations according to the above flow.
  • step 002 is restarted to repeat operations according to the above flow.
  • the fuel cell 1 does not even locally become a high temperature because the heat held by an inert gas and high-temperature remaining gases carried by the inert gas is exhausted to the outside through cooling water even if the inert gas such as nitrogen is supplied to the fuel cell 1 through circulation paths of the material gas and fuel gas of the fuel generator 32 and fuel cell 1 when power generation is stopped the same as the case of the embodiment 6. Therefore, even if using the solid macromolecular type for the fuel cell 1 , a solid macromolecular film is not locally dried or a trouble of extremely deteriorating the power-generation efficiency of the fuel cell 1 does not occur.
  • the target temperature Tr1 of the fuel cell 1 is set to 70° C. and the target temperature Tr2 of city water is set to 60° C. in the case of the embodiments 6 and 7 of the present invention, the target temperature Tr1 should be set to a temperature at which the power generation by the fuel cell 1 is efficiently performed and therefore, it is not restricted to 70° C. Moreover, the target temperature Tr2 should be set to a temperature requested to store city water in the hot-water storage tank 7 and it is not restricted to 60° C.
  • the threshold temperature Te1 for stopping operations of the cooling-water pump 35 and city-water pump 39 is set to 60° C. in the case of the embodiment 6 of the present invention, the temperature Te1 should be set to a temperature several degrees higher than the temperature requested to store city water in the hot-water storage tank 7 by considering a loss in the heat exchanger 36 and it is not restricted to 60° C.
  • the threshold temperature Te2 for stopping operations of the cooling-water pump 35 and city-water pump 39 is set to 55° C. in the case of the embodiment 7 of the present invention, it should be set to a temperature requested to store city water in the hot-water storage tank 7 and it is not restricted to 55° C.
  • the fuel cell 1 serves one thing of a fuel cell of the present invention and the cooling pipe 34 serves one thing of a cooling-circulation system of the present invention.
  • the cooling-water pump 35 serves as one thing of heating-medium circulation means of the present invention
  • the heat exchanger 36 and city-water pump 39 respectively serve as one thing of heat release means or a heat exchanger of the present invention
  • the fuel-cell-temperature detector 310 and city-water-temperature detector 311 respectively serve as one thing of temperature detection means of the present invention.
  • the cooling water flowing through the cooling pipe 34 serves as one thing of a first heating medium of the present invention and the city water to be carried through the city-water pipe 38 serves as one thing of a second heating medium of the present invention.
  • the present invention is not restricted to the configuration of the above embodiment 6 or 7. It is allowed that temperature detection means of the present invention obtains the temperature of the fuel cell 1 by directly measuring it. Moreover, it is allowed to measure the temperature of the heat exchanger 36 or the temperature of the city-water pipe 38 . In short, temperature detection means of the present invention can directly or indirectly detect the temperature of a fuel cell. Moreover, it is enough that the temperature of the second heating medium of the present invention can be detected but is not restricted by a temperature-measuring portion of the medium.
  • heat release means of the present invention has a configuration in which the heat exchanger 36 releases heat into air without using the hot-water storage tank 7 and city-water pipe 38 .
  • the pump 35 corresponding to heating-medium circulation means operates up to a predetermined threshold value.
  • heat release means has a configuration of performing the operation for heat release such as the circulation of the heating medium or only heating-medium circulation means operates even after supply of a fuel and oxidant to a fuel cell is stopped.
  • the cooling system (refer to symbol 100 in FIG. 6) in a fuel-cell cooling method of the present invention is constituted by at least a cooling-circulation system, heating-medium circulation means, and heat release means in a fuel-cell power-generation system of the present invention.
  • the present invention makes it possible to efficiently recover the heat generated by the fuel cell 1 under power generation by continuing operations of the cooling-water pump 35 and city-water pump 39 until the temperature Tr of cooling water becomes lower than the threshold temperature Te1 (approx. 60° C.) or the temperature Tw of city water becomes lower than the threshold temperature Te2 (approx. 55° C.). Because the cooling-water pump 35 and city-water pump 39 are stopped when the temperature of cooling water or city water becomes lower than the threshold temperature, it is possible to continuously store hot city water at a very-useful temperature without excessively lowering the temperature of stored hot city water.
  • the present invention makes it possible to provide a fuel-cell power-generation system not causing a trouble in power generation by a fuel cell without using ion removal means.
  • water can be self-supported without receiving water from the outside by using the recovered water obtained by condensing the water for reforming and shifting a fuel treater to a reformer or carbon-monoxide shifter and the water for humidifying supply gas and supply air by a fuel-side humidifier and oxidation-side humidifier by a condenser.
  • the present invention makes it possible to provide a fuel-cell power-generation system not deteriorating the power generation efficiency of a fuel cell after power generation is completed.
  • the present invention makes it possible to provide a fuel-cell power-generation system of efficiently taking out the heat generated in a fuel cell to the outside and using the heat in an effective mode.

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US7691512B2 (en) 2010-04-06
CN1238921C (zh) 2006-01-25
EP1396897B1 (fr) 2011-08-31
EP2178149A2 (fr) 2010-04-21
US20090176138A1 (en) 2009-07-09
CN1463474A (zh) 2003-12-24
EP1396897A4 (fr) 2009-06-03
US20060246325A1 (en) 2006-11-02
US7816048B2 (en) 2010-10-19
EP1396897A1 (fr) 2004-03-10
WO2002095854A1 (fr) 2002-11-28

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