IP Library › Granted Patent US 8,926,942
Granted Patent B2
US 8,926,942 · App. 12/679,506 · Granted Jan 6, 2015

Methods and systems for generating hydrogen and separating carbon dioxide

Inventors: Marco J. Castaldi (Yonkers, NY); Robert J. Farrauto (Princeton, NJ); Tuncel M. Yegulalp (Teaneck, NJ)
Assignee: The Trustees of Columbia University in the City of New York
B01D53/02C01B3/38C01B3/48C01B3/56B01D2253/112B01D2256/16B01D2259/504C01B2203/0233C01B2203/0283C01B2203/0425C01B2203/0475C01B2203/06C01B2203/066C01B2203/1064C01B2203/1235C01B2203/82Y02C10/08
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Quick Facts
Patent No.
US 8,926,942
App. No.
12/679,506
Granted
Jan 6, 2015
Kind
B2
Abstract

Methods and systems for generating hydrogen and separating carbon dioxide from a feed stream including hydro-carbons and water are disclosed. In some embodiments, the method includes the following: providing a catalytic chamber including a monolithic structure having surfaces coated with carbon dioxide adsorbing materials and one or more washcoated layers of combined steam reforming, water gas shift, and combustion catalysts; directing the feed stream into said catalytic chamber; controlling the feed stream so that it has a temperature range that allows the reactive generation of carbon dioxide and hydrogen gas but does not cause substantial development of coke between hydrocarbons in the feed stream and said surfaces of said monolithic structure; and adsorbing said carbon dioxide generated by heating the feed stream, wherein said carbon dioxide is adsorbed onto carbon dioxide adsorbing materials on said surfaces of said monolithic structure.

Claims (36)

1. A method of generating hydrogen and separating carbon dioxide from a feed stream including hydrocarbons and water, the method comprising:

providing a first catalytic chamber including surfaces coated with carbon dioxide adsorbing materials and one or more washcoated layers of combined steam reforming and water gas shift catalysts;

providing a second catalytic chamber including surfaces coated with carbon dioxide adsorbing materials and one or more washcoated layers of combined steam reforming and water gas shift catalysts;

controlling the feed stream to be alternatingly fed to at least one of said first and second catalytic chamber so that it has a temperature range that allows the reactive generation of carbon dioxide and hydrogen gas but does not cause substantial development of coke between hydrocarbons in the feed stream and said surfaces of said catalytic chamber; and

adsorbing and desorbing said carbon dioxide generated by heating the feed stream, wherein said carbon dioxide is alternatingly adsorbed onto and desorbed from said surfaces of said first and second catalytic chambers coated with carbon dioxide adsorbing materials.

2. The method according to claim 1 , wherein said carbon dioxide adsorbing materials wherein at least one of said carbon dioxide adsorbing materials is an alkaline metal oxide including one of CaO, MgO, SrO, BaO, and a combination thereof.

3. The method according to claim 1 , wherein an upper end of said temperature range is less than about 500 degrees Celsius.

4. The method according to claim 1 , wherein at least one of said first and second catalytic chambers includes surfaces having steam reforming, water gas shift, and combustion catalysts.

5. The method according to claim 4 , wherein said steam reforming, water gas shift, and combustion catalysts include one or more platinum group metal components.

6. The method according to claim 1 , said method further comprising:

desorbing said carbon dioxide adsorbed onto carbon dioxide adsorbing materials.

7. The method according to claim 6 , wherein said carbon dioxide is desorbed by at least one of reducing the pressure in at least one of said first and second catalytic chambers and heating said carbon dioxide adsorbing materials.

8. A system for generating hydrogen and separating carbon dioxide from a feed stream including hydrocarbons and water, the system comprising:

a first catalytic chamber having an inlet and an outlet and means for opening and closing said inlet and said outlet;

a second catalytic chamber having an inlet and an outlet and means for opening and closing said inlet and said outlet;

a first monolithic structure positioned within said first chamber, said monolithic structure having surfaces coated with carbon dioxide adsorbing materials and one or more washcoated layers of combined steam reforming and water gas shift catalysts;

a second monolithic structure positioned within said second chamber, said monolithic structure having surfaces coated with carbon dioxide adsorbing materials and one or more washcoated layers of combined steam reforming and water gas shift catalysts;

a heat source for heating the feed stream to a temperature range that allows the reactive generation of carbon dioxide and hydrogen gas but does not cause substantial development of coke between hydrocarbons in the feed stream and said surfaces of said monolithic structure; and

means for heating said carbon dioxide adsorbing materials;

wherein said carbon dioxide adsorbing materials are configured to adsorb carbon dioxide generated by heating the feed stream with said heat source and said outlet is configured to allow hydrogen gas to exit said chamber; wherein

said feed stream is configured to be alternatingly delivered to said first chamber and said second chamber.

9. The system according to claim 8 , wherein at least one of the surfaces of said first and second chambers and said surfaces of said first and second monolithic structures include steam reforming, water gas shift, and combustion catalysts positioned thereon.

10. The system according to claim 8 , wherein at least one of said carbon dioxide adsorbing materials is an alkaline metal oxide including one of CaO, MgO, SrO, BaO, and a combination thereof

11. The system according to claim 8 , wherein said system is configured for desorbing said carbon dioxide adsorbed by said carbon dioxide adsorbing materials by at least one of reducing the pressure in at least one of said first and second catalytic chambers and heating said carbon dioxide adsorbing materials.

12. The system according to claim 8 , wherein at least one of said first and second monolithic structure is a heat exchanger.

13. A high surface area structure for generating hydrogen and separating carbon dioxide from a feed stream including hydrocarbons and water, the structure comprising:

a first monolithic structure having a washcoated high surface area stabilized carrier;

a second monolithic structure having a washcoated high surface area stabilized carrier;

carbon dioxide adsorbing materials deposited on surfaces on said high surface area stabilized carrier; and

one or more washcoated layers of combined steam reforming and water gas shifting catalysts on said monolithic structure;

wherein said washcoated layers of said stabilized carriers, said carbon dioxide adsorbing materials, and said one or more washcoated layers of combined steam reforming and water gas shifting catalysts are configured so as to resist the formation of coke between hydrocarbons in the feed stream and said surfaces of said monolithic structure when said temperature of the feed stream is less than about 500 degrees Celsius; wherein

the feed stream is configured to be alternatingly delivered to said first monolithic structure and said second monolithic structure.

14. The high surface are structure according to claim 13 , wherein said high surface area stabilized carrier includes one or more washcoated layers of one of activated Al2O3, CeO2, CeO2-ZrO2, Al stabilized CeO2, SiO2, TiO2, zeolites, and a combination thereof.

15. The high surface are structure according to claim 13 , wherein at least one of said carbon dioxide adsorbing materials is an alkaline metal oxide including one of CaO, MgO, SrO, BaO, and a combination thereof deposited on a high surface area carrier.

16. The high surface are structure according to claim 13 , wherein at least one of said first and second monolithic structures includes surfaces having at least one or more washcoated layers of alkaline material and combined steam reforming, water gas shift, and combustion catalysts.

17. The high surface are structure according to claim 16 , wherein said steam reforming, water gas shift, and combustion catalysts include one or more platinum group metal components.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 24, 2010
From: CASTALDI, MARCO J.; FARRAUTO, ROBERT J.; YEGULALP, TUNCEL M.
To: THE TRUSTEES OF COLUMBIA UNIVERSITY IN THE CITY OF NEW YORK
Reel/Frame 025035/0900 →
Continuity (2)
Provisional Application 60975930 · Sep 28, 2007
Related Publication 20100284904A1 · Nov 11, 2010