Patent EP0206608A2 successfully refreshed from Google Patents.
EP0206608A2
Expired / Lapsed
EP
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Fuel cell integrated with steam reformer
Assignee: United States Department of Energy
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Filing: 1986-06-09
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Granted: —
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Expires: 2006-06-09
Abstract
Abstract @ A H 2 -air fuel cell integrated with a steam reformer is disclosed wherein a superheated water/methanol mixture is fed to a catalytic reformer to provide a continuous supply of hydrogen to the fuel cell, the gases exhausted from the anode of the fuel cell providing the thermal energy, via combustion, for superheating the water/methanol mixture.
Inventors
- 👤 Bahjat S. Beshty
- 👤 James A. Whelan
Bibliographic Details
Application Number
—
Jurisdiction
EP
Data Source
google_patents
Last Synchronized
2026-11-02 22:22
CPC Classifications
C; C01; C01B; C01B3/00; C01B3/02; C01B3/32; C01B3/323; B; B01; B01B; B01B1/00; B01B1/005; H; H01; H01M; H01M8/00; H01M8/06; H01M8/0606; H01M8/0612; Y; Y02; Y02E; Y02E60/00; Y02E60/30; Y02E60/50
Claims Analysis
Total Claims: 37
Claim 1
Independent Claim
388 words
A process of providing a continuous supply of hydrogen fuel to a fuel cell system, the system being comprised of a heat exchanger, a burner, a catalytic reactor containing a catalyst bed for catalyzing the production of hydrogen from a gaseous mixture of water and methanol and a fuel cell comprised of a fuel electrode, an oxygen electrode and an electrolyte disposed therebetween, the process comprising the steps of: (a) passing a gaseous mixture consisting essentially of water and methanol to the heat exchanger to heat the mixture to a superheated state, the temperature and composition of the superheated mixture being sufficient to supply at least about 90% of the heat required for reforming the methanol contained in said mixture by condensation, (b) passing the superheated gaseous mixture of water and methanol into the catalytic reactor to form hydrogen by an endothermic reaction of water and methanol over the catalyst bed, the catalytic reactor being in the form of a tube having a length to diameter ratio of from about 2 to about 6, said catalyst bed comprising a low activity, high stability zinc oxide and chromium oxide catalyst comprised of about 30 to 65 percent by weight Zn and about 5 to 35 percent by weight Cr, followed by a high activity zinc oxide and copper oxide catalyst on alumina comprised of about 5 to 20 percent by weight Zn, about 15 to 40 percent by weight Cu, and about 15 to 50 percent by weight alumina, the temperature of said superheated mixture being between about 425° and about 600°C and the water to methanol ratio being between about 2 and about 9. (c) directing hydrogen produced in step (b) to the fuel electrode of the fuel cell, (d) directing air into the oxygen electrode of the fuel cell to effect an electrochemical reaction to produce electricity, (e) exhausting the gaseous effluent from the fuel electrode, a portion of which is a combustible gas, burning the combustible portion of the fuel electrode exhaust in the burner, feeding the burner exhaust to the heat exchanger to supply heat for the superheating of the water and methanol in step (a) whereby the gases exhausted from the fuel electrode supply at least a major portion of the thermal energy, via combustion, to heat the water/methanol mixture to the superheated state.
Claim 2
Dependent Claim
388 words
A process of providing a continuous supply of hydrogen fuel to a fuel cell system, the system being comprised of a heat exchanger, a burner, a catalytic reactor containing a catalyst bed for catalyzing the production of hydrogen from a gaseous mixture of water and methanol and a fuel cell comprised of a fuel electrode, an oxygen electrode and an electrolyte disposed therebetween, the process comprising the steps of: (a) passing a gaseous mixture consisting essentially of water and methanol to the heat exchanger to heat the mixture to a superheated state, the temperature and composition of the superheated mixture being sufficient to supply at least about 90% of the heat required for reforming the methanol contained in said mixture by condensation, (b) passing the superheated gaseous mixture of water and methanol into the catalytic reactor to form hydrogen by an endothermic reaction of water and methanol over the catalyst bed, the catalytic reactor being in the form of a tube having a length to diameter ratio of from about 2 to about 6, said catalyst bed comprising a low activity, high stability zinc oxide and chromium oxide catalyst comprised of about 30 to 65 percent by weight Zn and about 5 to 35 percent by weight Cr, followed by a high activity zinc oxide and copper oxide catalyst on alumina comprised of about 5 to 20 percent by weight Zn, about 15 to 40 percent by weight Cu, and about 15 to 50 percent by weight alumina, the temperature of said superheated mixture being between about 425° and about 600°C and the water to methanol ratio being between about 2 and about 9. (c) directing hydrogen produced in step (b) to the fuel electrode of the fuel cell, (d) directing air into the oxygen electrode of the fuel cell to effect an electrochemical reaction to produce electricity, (e) exhausting the gaseous effluent from the fuel electrode, a portion of which is a combustible gas, burning the combustible portion of the fuel electrode exhaust in the burner, feeding the burner exhaust to the heat exchanger to supply heat for the superheating of the water and methanol in step (a) whereby the gases exhausted from the fuel electrode supply at least a major portion of the thermal energy, via combustion, to heat the water/methanol mixture to the superheated state.
Claim 3
Dependent Claim
282 words
A process of providing a continuous supply of hydrogen fuel to a fuel cell system, the system being comprised of a heat exchanger, a burner, a catalytic reactor containing a catalyst bed for catalyzing the production of hydrogen from a gaseous mixture consisting essentially of water and methanol and a fuel cell comprised of a fuel electrode, an oxygen electrode and an electrolyte disposed therebetween, the process comprising the steps of: (a) passing a gaseous mixture of water and methanol to the heat exchanger to heat the mixture to a superheated state, the temperature and composition of the superheated mixture being sufficient to supply at least about 75% of heat required for reforming the methanol contained in said mixture by condensation, (b) passing the superheated gaseous mixture of water and methanol into the catalytic reactor to form hydrogen by an endothermic reaction of water and methanol over the catalyst bed, the catalytic reactor being in the form of a simple tube having a length to diameter ratio of less than about 10 to 1, (c) directing hydrogen produced in step (b) to the fuel electrode of the fuel cell, (d) directing air into the oxygen electrode of the fuel cell to effect an electrochemical reaction to produce electricity, (e) exhausting the gaseous effluent from the fuel electrode, a portion of which is a combustible gas, burning the combustible portion of the fuel electrode exhaust in the burner, feeding the burner exhaust to the heat exchanger to supply heat for the superheating of the water and methanol in step (a) whereby the gases exhausted from the fuel electrode supply the thermal energy, via combustion, to heat the water/methanol mixture to the superheated state.
Claim 4
Dependent Claim
282 words
A process of providing a continuous supply of hydrogen fuel to a fuel cell system, the system being comprised of a heat exchanger, a burner, a catalytic reactor containing a catalyst bed for catalyzing the production of hydrogen from a gaseous mixture consisting essentially of water and methanol and a fuel cell comprised of a fuel electrode, an oxygen electrode and an electrolyte disposed therebetween, the process comprising the steps of: (a) passing a gaseous mixture of water and methanol to the heat exchanger to heat the mixture to a superheated state, the temperature and composition of the superheated mixture being sufficient to supply at least about 75% of heat required for reforming the methanol contained in said mixture by condensation, (b) passing the superheated gaseous mixture of water and methanol into the catalytic reactor to form hydrogen by an endothermic reaction of water and methanol over the catalyst bed, the catalytic reactor being in the form of a simple tube having a length to diameter ratio of less than about 10 to 1, (c) directing hydrogen produced in step (b) to the fuel electrode of the fuel cell, (d) directing air into the oxygen electrode of the fuel cell to effect an electrochemical reaction to produce electricity, (e) exhausting the gaseous effluent from the fuel electrode, a portion of which is a combustible gas, burning the combustible portion of the fuel electrode exhaust in the burner, feeding the burner exhaust to the heat exchanger to supply heat for the superheating of the water and methanol in step (a) whereby the gases exhausted from the fuel electrode supply the thermal energy, via combustion, to heat the water/methanol mixture to the superheated state.
Claim 5
Dependent Claim
30 words
The process of Claim 2 wherein a portion of the catalytic reactor exhaust is comprised of water which is condensed and recycled for use in the catalytic steam reforming reaction.
Claim 6
Dependent Claim
21 words
The process of Claim 2 wherein the water/ methanol mixture is superheated to a temperature between about 800° and about 1100°F.
Claim 7
Dependent Claim
21 words
The process of Claim 2 wherein the water/ methanol mixture is superheated to a temperature of about 850 to about 1000°F.
Claim 8
Dependent Claim
23 words
The process of Claim 2 wherein the water/ methanol molar ratio in the superheated gaseous mixture is between about 2 to about 9.
Claim 9
Dependent Claim
13 words
The process of Claim 2 wherein the fuel cell electrolyte is phosphoric acid.
Claim 10
Dependent Claim
22 words
The process of Claim 2 wherein the catalyst in the catalyst bed is a combination of zinc and chromium oxides on alumina.
Claim 11
Dependent Claim
80 words
The process of Claim 2 wherein the catalyst bed comprises a low activity, high stability zinc oxide and chromium oxide catalyst comprised of about 40 to 65 percent by weight Zn and about 10 to 30 percent by weight Cr, followed by a high activity zinc oxide and copper oxide catalyst on alumina comprised of about 5 to 20 percent by weight Zn, about 20 to 35 percent by weight Cu, and about 20 to 40 percent by weight alumina.
Claim 12
Dependent Claim
229 words
A process of providing a continuous supply of hydrogen fuel to a fuel cell system, the system being comprised of a heat exchanger, a burner, a catalytic reactor containing a catalyst bed for catalyzing the production of hydrogen from a gaseous mixture consisting essentially of water and methanol and a fuel cell comprised of a fuel electrode, an oxygen electrode and an electrolyte disposed therebetween, the process comprising the steps of: (a) passing a gaseous mixture of water and methanol to the heat exchanger to heat the mixture to a superheated state, (b) passing the superheated gaseous mixture of water and methanol into the catalytic reactor to form hydrogen by an endothermic reaction of water and methanol over the catalyst bed, (c) directing hydrogen produced in step (b) to the fuel electrode of the fuel cell, (d) directing air into the oxygen electrode of the fuel cell to effect an electrochemical reaction to produce electricity, (e) exhausting the gaseous effluent from the fuel electrode, a portion of which is a combustible gas, burning the combustible portion of the fuel electrode exhaust in the burner, feeding the burner exhaust to the heat exchanger to supply heat for the superheating of the water and methanol in step (a) whereby the gases exhausted from the fuel electrode supply the thermal energy, via combustion, to heat the water/methanol mixture to the superheated state.
Claim 13
Dependent Claim
229 words
A process of providing a continuous supply of hydrogen fuel to a fuel cell system, the system being comprised of a heat exchanger, a burner, a catalytic reactor containing a catalyst bed for catalyzing the production of hydrogen from a gaseous mixture consisting essentially of water and methanol and a fuel cell comprised of a fuel electrode, an oxygen electrode and an electrolyte disposed therebetween, the process comprising the steps of: (a) passing a gaseous mixture of water and methanol to the heat exchanger to heat the mixture to a superheated state, (b) passing the superheated gaseous mixture of water and methanol into the catalytic reactor to form hydrogen by an endothermic reaction of water and methanol over the catalyst bed, (c) directing hydrogen produced in step (b) to the fuel electrode of the fuel cell, (d) directing air into the oxygen electrode of the fuel cell to effect an electrochemical reaction to produce electricity, (e) exhausting the gaseous effluent from the fuel electrode, a portion of which is a combustible gas, burning the combustible portion of the fuel electrode exhaust in the burner, feeding the burner exhaust to the heat exchanger to supply heat for the superheating of the water and methanol in step (a) whereby the gases exhausted from the fuel electrode supply the thermal energy, via combustion, to heat the water/methanol mixture to the superheated state.
Claim 14
Dependent Claim
30 words
The process of Claim 10 wherein a portion of the catalytic reactor exhaust is comprised of water which is condensed and recycled for use in the catalytic steam reforming reaction.
Claim 15
Dependent Claim
20 words
The process of Claim 10 wherein the water/methanol mixture is superheated to a temperature between about 800° and about 1100°F.
Claim 16
Dependent Claim
20 words
The process of Claim 10 wherein the water/methanol mixture is superheated to a temperature of about 850 to about 1000°F.
Claim 17
Dependent Claim
22 words
The process of Claim 10 wherein the water/methanol molar ratio in the superheated gaseous mixture is between about 2 to about 9.
Claim 18
Dependent Claim
13 words
The process of Claim 10 wherein the fuel cell electrolyte is phosphoric acid.
Claim 19
Dependent Claim
22 words
The process of Claim 10 wherein the catalyst in the catalyst bed is a combination of zinc and chromium oxides on alumina.
Claim 20
Dependent Claim
80 words
The process of Claim 10 wherein the catalyst bed comprises a low activity, high stability zinc oxide and chromium oxide catalyst comprised of about 40 to 65 percent by weight Zn and about 10 to 30 percent by weight Cr, followed by a high activity zinc oxide and copper oxide catalyst on alumina comprised of about 5 to 20 percent by weight Zn, about 20 to 35 percent by weight Cu, and about 20 to 40 percent by weight alumina.
Claim 21
Dependent Claim
85 words
In a process for the production of hydrogen, said process comprising passing a gaseous feed mixture consisting essentially of methanol and water into a reactor over a catalyst bed, the improvement comprising superheating the gaseous mixture to a temperature between about 700° to about 1,100°F., and then feeding the superheated gaseous mixture to the reactor in contact with the catalyst bed contained therein, to produce hydrogen, at least a major portion of the heat for the catalytic reaction being extracted from the superheated gaseous mixture.
Claim 22
Dependent Claim
85 words
In a process for the production of hydrogen, said process comprising passing a gaseous feed mixture consisting essentially of methanol and water into a reactor over a catalyst bed, the improvement comprising superheating the gaseous mixture to a temperature between about 700° to about 1,100°F., and then feeding the superheated gaseous mixture to the reactor in contact with the catalyst bed contained therein, to produce hydrogen, at least a major portion of the heat for the catalytic reaction being extracted from the superheated gaseous mixture.
Claim 23
Dependent Claim
66 words
The process of Claim 18 wherein the catalyst bed is divided into a first section extending from the inlet of the reactor bed and a second section extending from the end of the first section to the outlet of the reactor bed, the first section containing a low activity, high temperature resistant steam reforming catalyst and the second section containing a high activity steam reforming catalyst.
Claim 24
Dependent Claim
23 words
The process of Claim 18 wherein the catalyst in the catalyst bed is a combination of zinc oxide and chromium oxide on alumina.
Claim 25
Dependent Claim
76 words
The process of Claim 19 wherein the low activity catalyst is a combination of oxides of zinc and chromium comprised of about 40% to 60% by weight Zn and about 10% to 30% by weight Cr and the high activity catalyst is a combination of oxides of zinc and copper on alumina comprised of about 5% to 20% by weight Zn, about 20% to 35% by weight Cu and about 20% to 40% by weight alumina.
Claim 26
Dependent Claim
21 words
The process of Claim 18 wherein the water/methanol molar ratio in the gaseous mixture is between about 1.0 to about 10.0.
Claim 27
Dependent Claim
20 words
The process of Claim 18 wherein the gaseous mixture is superheated to a temperature of about 850° to about 1,000°F.
Claim 28
Dependent Claim
128 words
An integrated methanol steam reformer, combustor chamber, and methanol superheater unit comprising: means defining a combustion chamber having an inlet and an exhaust, said exhaust being connected to means defining a duct, superheater means for heating a mixture consisting essentially of methanol and water disposed within said combustion chamber, the outlet of said superheater means being operably connected to the inlet of a methanol heater/supply tube passing through said duct, a shell encompassing said duct adjacent said means defining a combustion chamber, said duct opening into the interior of said shell and a plurality of tubes operably connected to said methanol heater/supply tube disposed within said shell exterior to said duct, said tubes having a catayst for steam reforming of methanol into a hydrogen rich gas disposed therein.
Claim 29
Dependent Claim
128 words
An integrated methanol steam reformer, combustor chamber, and methanol superheater unit comprising: means defining a combustion chamber having an inlet and an exhaust, said exhaust being connected to means defining a duct, superheater means for heating a mixture consisting essentially of methanol and water disposed within said combustion chamber, the outlet of said superheater means being operably connected to the inlet of a methanol heater/supply tube passing through said duct, a shell encompassing said duct adjacent said means defining a combustion chamber, said duct opening into the interior of said shell and a plurality of tubes operably connected to said methanol heater/supply tube disposed within said shell exterior to said duct, said tubes having a catayst for steam reforming of methanol into a hydrogen rich gas disposed therein.
Claim 30
Dependent Claim
96 words
The apparatus of Claim 24 further including: a fuel cell comprising means defining an anode chamber and means defining a cathode chamber; means for supplying hydrogen rich gas from said reformer to the anode chamber of said fuel cell; means for recovering hydrogen from said anode chamber and employing said hydrogen to heat said mixture of methanol and water prior to its entry into said tubes disposed exterior to said duct; and means for recovering and condensing water from the anode chamber of said fuel cell and employing said water for cooling of said fuel cell.
Claim 31
Dependent Claim
135 words
An integrated apparatus for the production of hydrogen and production of electricity therefrom comprising a reforming chamber having reforming catalyst disposed therein and means for supplying a superheated gaseous mixture consisting essentially of methanol and water to said reforming chamber at such a temperature that at least a major portion of the heat required for reforming said mixture is supplied by the heat contained within said gaseous superheated mixture, said temperature being between about 700° and 1100°F, a fuel cell comprising means defining an anode chamber and means defining a cathode chamber; means for supplying hydrogen rich gas from said reforming chamber to said anode chamber, and means for recovering hydrogen from said anode chamber and employing said hydrogen to heat said mixture of methanol and water prior to its entry into said reforming chamber.
Claim 32
Dependent Claim
135 words
An integrated apparatus for the production of hydrogen and production of electricity therefrom comprising a reforming chamber having reforming catalyst disposed therein and means for supplying a superheated gaseous mixture consisting essentially of methanol and water to said reforming chamber at such a temperature that at least a major portion of the heat required for reforming said mixture is supplied by the heat contained within said gaseous superheated mixture, said temperature being between about 700° and 1100°F, a fuel cell comprising means defining an anode chamber and means defining a cathode chamber; means for supplying hydrogen rich gas from said reforming chamber to said anode chamber, and means for recovering hydrogen from said anode chamber and employing said hydrogen to heat said mixture of methanol and water prior to its entry into said reforming chamber.
Claim 33
Dependent Claim
64 words
The apparatus of Claim 26 wherein the reforming chamber is divided into a first section extending from the inlet of the chamber and a second section extending from the end of the first section to the outlet of the chamber, the first section containing a low activity, high temperature resistant steam reforming catalyst and the second section containing a high activity steam reforming catalyst.
Claim 34
Dependent Claim
23 words
The apparatus of Claim 26 wherein the catalyst in the catalyst bed is a combination of zinc oxide and chromium oxide on alumina.
Claim 35
Dependent Claim
76 words
The apparatus of Claim 28 wherein the low activity catalyst is a combination of oxides of zinc and chromium comprised of about 40% to 60% by weight Zn and about 10% to 30% by weight Cr and the high activity catalyst is a combination of oxides of zinc and copper on alumina comprised of about 5% to 20% by weight Zn, about 20% to 35% by weight Cu and about 20% to 40% by weight alumina.
Claim 36
Dependent Claim
24 words
The process of Claim 26 further comprising means for maintaining the water/methanol molar ratio in the gaseous mixture between about 1.0 to about 10.0.
Claim 37
Dependent Claim
30 words
The apparatus of Claim 26 wherein the temperature at which the gaseous superheated mixture of methanol and water is supplied to said reforming chamber is between about 850° and 1100°F.
References Cited (Backward Citations)
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