High performance fuel processing system for fuel cell power plant

• US 6,932,848 B2
• Filed: 03/28/2003
• Issued: 08/23/2005
• Est. Priority Date: 03/28/2003
• Status: Active Grant

• Current Assignee: Hyaxiom Incorporated
• Original Assignee: UTC Fuel Cells, LLC
• Inventors: Gupta, Nikunj, Vanderspurt, Thomas Henry, Ghosh, Shubhro, She, Ying, Dardas, Zissis
• Primary Examiner(s): Bhat, N.
• Application Number:
  US10/402,506
• Publication Number:
  US 20040187384A1
• Time in Patent Office: 879 Days
• Field of Search: 481/97.R, 481/271, 481/277, 422/177, 422/190, 422/196, 429/19, 423/246
• US Class Current: 48/127.7
• CPC Class Codes: C01B 2203/0233 the reforming step being a steam reforming step
• CPC Class Codes: C01B 2203/0244 the reforming step being an autothermal reforming step, e.g. secondary reforming processes
• CPC Class Codes: C01B 2203/0288 containing two CO-shift steps
• CPC Class Codes: C01B 2203/044 Selective oxidation of carbon monoxide
• CPC Class Codes: C01B 2203/047 the impurity being carbon monoxide
• CPC Class Codes: C01B 2203/066 with fuel cells
• CPC Class Codes: C01B 2203/1041 Composition of the catalyst
• CPC Class Codes: C01B 2203/107 Platinum catalysts
• CPC Class Codes: C01B 2203/127 Catalytic desulfurisation
• CPC Class Codes: C01B 3/16 using catalysts
• CPC Class Codes: C01B 3/583 the reaction being the selective oxidation of carbon monoxide
• CPC Class Codes: H01M 8/0612 from carbon-containing material
• CPC Class Codes: H01M 8/0668 Removal of carbon monoxide or carbon dioxide
• CPC Class Codes: Y02E 60/50 Fuel cells
• CPC Class Codes: Y02P 20/52 using catalysts, e.g. selective catalysts

Abstract

A fuel processing system (FPS) (110) is provided for a fuel cell power plant (115) having a fuel cell stack assembly (CSA) (56). A water gas shift (WGS) reaction section (12, 120) of the FPS (110) reduces the concentration of carbon monoxide (CO) in the supplied hydrocarbon reformate, and a preferred oxidation (PROX) section (40) further reduces the CO concentration to an acceptable level. The WGS section (12, 120) includes a reactor (124) with a high activity catalyst for reducing the reformate Co concentration to a relatively low level, e.g., 2,000 ppmv or less, thereby relatively reducing the structural volume of the FPS (110). The high activity catalyst is active at temperatures as low as 250° C., and may be a noble-metal-on-ceria catalyst of Pt and Re on a nanocrystaline, cerium oxide-based support. Then only a low temperature PROX reactor (46) is required for preferential oxidation in the FPS (110).

Claims

1. In a fuel processing system (FPS) (110) for a fuel cell power plant (115) including a fuel cell stack assembly (CSA) (56), the FPS (110) including at least a water gas shift (WGS) reaction section (12, 120) for receiving hydrocarbon reformate containing CO and reducing the concentration of CO in the reformate via the shift reaction, and at least a preferential oxidation (PROX) section (40) for further reducing the concentration of CO in the reformate to a concentration acceptable for operating the CSA (56), the improvement wherein:

the WGS section (12, 120) includes a low temperature reactor (124) with a high activity catalyst therein for reducing the concentration of CO in the reformate to a relatively low level, thereby relatively reducing the structural volume of the FPS (110), said high activity catalyst comprises a noble-metal-on-ceria based, nanophase-structure catalyst in the low temperature reactor (124) of the WGS section (120) being active at temperatures as low as 250°

C.

2. The fuel processing system of claim 1 wherein the high activity catalyst in the low temperature WGS reactor (124) reduces the concentration of CO in the reformate to about 2,000 ppmv or less.

3. The fuel processing system of claim 2 wherein the PROX section (40) comprises a low temperature PROX reactor (46), the low temperature PROX reactor (46) being the only PROX reactor in the FPS (110).

4. The fuel processing system of claim 3 wherein the concentration of CO in the reformate following the further reduction thereof in the low temperature PROX reactor (46) is less than about 10 ppmv.

5. The fuel processing system of claim 2 wherein said high activity catalyst with said reactor (124) of the WGS section (120) comprises a noble-metal-on-ceria-based, nanophase-structured catalyst.

6. The fuel processing system of claim 5 wherein said noble-metal-on-ceria-based catalyst comprises platinum (Pt) and rhenium (Re) mixed metal on a nanocrystaline, cerium oxide-based support.

7. The fuel processing system of claim 1 wherein said noble-metal-on-ceria-based catalyst comprises platinum (Pt) and rhenium (Re) mixed metal on a nanocrystaline, cerium oxide-based support.

8. The fuel processing system of claim 7 wherein said high activity catalyst has a catalyst activity of at least 0.18 moles of CO per moles of Pt per sec. (moles CO/moles Pt-sec.) at 250°

C. for a gas composition of 1.5%-2.5% CO, 25%-35% H₂O, 30-50% H₂, 10-14% CO₂, balance N₂, a CO reaction order in the range of 0.0 to 0.10 and an activation energy of up to about 20 Kcal/mole CO.

9. In a fuel processing system (FPS) (110) for a fuel cell power plant (115) including a fuel cell stack assembly (CSA) (56), the FPS (110) including at least a water gas shift (WGS) reaction section (12, 120) for receiving hydrocarbon reformate containing CO and reducing the concentration of CO in the reformate via the shift reaction, and at least a preferential oxidation (PROX) section (40) for further reducing the concentration of CO in the reformate to a concentration acceptable for operating the CSA (56), the improvement wherein:

the WGS section (12, 120) includes a low temperature reactor (124) with a high activity catalyst for reducing the concentration of CO in the reformate to a relatively low level, thereby relatively reducing the structural volume of the FPS (110), said high activity catalyst in the low temperature reactor (124) of the WGS section (120) comprising a noble-metal-on-ceria-based, nanophase-structured catalyst comprising platinum (Pt) and rhenium (Re) mixed metal on a nanocrystaline, cerium oxide-based support.

10. The fuel processing system (110) of claim 9 wherein the WGS section reactor (124) is a low temperature, WGS reactor (124), and the high activity catalyst is included therein and is active at temperatures as low as 250°

C.

11. The fuel processing system of claim 9 wherein the PROX section (40) comprises a low temperature PROX reactor (46), the low temperature PROX reactor (46) being the only PROX reactor in the FPS (110).

12. The fuel processing system of claim 11 wherein the concentration of CO in the reformate following the further reduction thereof in the low temperature PROX reactor (46) is less than about 50 ppmv.

13. In a fuel processing system (FPS) (110) for a fuel cell power plant (115) including a fuel cell stack assembly (GSA) (56), the FPS (110) including at least a water gas shift (WGS) reaction section (12, 120) for receiving hydrocarbon reformate containing CO and reducing the concentration of CO in the reformate via the shift reaction, and at least a preferential oxidation (PROX) section (40) for further reducing the concentration of CO in the reformate to a concentration acceptable for operating the CSA (56), the improvement wherein:

the WGS section (12, 120) includes a low temperature reactor (124) with a high activity catalyst for reducing the concentration of CO in the reformate to a relatively low level, thereby relatively reducing the structural volume of the FPS (110), said high activity catalyst in the low temperature reactor (124) of the WGS section (120) including at least platinum and having a catalyst activity of at least 0.18 moles of CO per moles of Pt per sec. (moles CO/moles Pt-sec.) at 250°

C. for a gas composition of 1.5%-2.5% CO, 25%-35% H₂O, 30-50% H₂, 10-14% CO₂, balance N₂, a CO reaction order in the range of 0.0 to 0.10 and an activation energy of up to about 20 Kcal/mole CO.

14. The fuel processing system of claim 13 wherein said high activity catalyst with said reactor (124) of the WGS section (120) comprises a noble-metal-on-ceria-based, nanophase-structured catalyst comprising platinum (Pt) and rhenium (Re) mixed metal on a nanocrystaline, cerium oxide-based support.

15. The fuel processing system of claim 14 wherein the high activity catalyst in the low temperature WGS reactor (124) reduces the concentration of CO in the reformate to about 2,000 ppmv or less.

16. The fuel processing system of claim 15 wherein the PROX section (40) comprises a low temperature PROX reactor (46), the low temperature PROX reactor (46) being the only PROX reactor in the FPS (110).

17. The fuel processing system of claim 13 wherein said high activity catalyst with said reactor (124) of the WGS section (120) comprises at least platinum on a nanocrystaline, cerium-based mixed metal oxide support, the mixed metals of said support, in addition to cerium, further including at least a second metal, or mixture thereof, selected from the group consisting of Zr arid Hf, and a third metal, or mixture thereof, selected from the group consisting of Nb, Ta, Mo and W.

18. The fuel processing system of claim 17 wherein the cerium-based mixed-metal oxide support of said high activity catalyst has a surface area on a weight basis of at least about 150 m²/g, an average crystallite size of about 2 to 4 nm and agglomerated to form a skeletal structure with pores, average pore diameters being between about 4 and 9 nm and normally being greater than the average crystallite size, and wherein the surface area of the skeletal structure per volume of the material of the structure is greater than about 350 m²/cm³.