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[323h] - Hydrogen from Methane in Millisecond Reactors: Partial Oxidation and Water-Gas Shift

Presented at: [323] - Fuel Cells and Hydrogen Fuels # 1
For schedule information click here

 Author Information:

Emil J Klein (speaker)
University of Minnesota
421 Washington Ave. S.E.
Minneapolis, MN 55455
Phone: (612) 625-6083
Fax:
Email: emil@cems.umn.edu
Lanny Schmidt
University of Minnesota
Department of Chemical Engineering and Materials Science, 151 Amundson Hall, 421 Washington Ave. SE
Minneapolis, MN 55455-0132
Phone: 612-625-9391
Fax: 612-626-7246
Email: schmi001@tc.umn.edu

Abstract:

Fuel cell fuel preparation, particularly hydrogen production, has received increased interest in recent years due to the increasing demand for more efficient power sources. The high purity hydrogen, low concentration carbon monoxide fuel streams required for PEM fuel cells have necessitated the design of a reactor system that can convert available natural resources (such as natural gas or gasoline) into high purity hydrogen streams. One attractive design for hydrogen production couples partial oxidation of hydrocarbons on rhodium, with high temperature water-gas shift of the produced synthesis gas on various traditional and non-traditional shift catalysts. This two-stage, millisecond-contact-time system enables the combination of two necessary hydrogen production stages into a single, potentially adiabatic, reactor.

This presentation covers experiments conducted in an effort to determine the extent that partial oxidation and water-gas shift can be carried out in series on metal-coated monoliths at millisecond contact times. Since the temperatures associated with partial oxidation products are typically in excess of 800C, initial water-gas shift reactions are conducted at higher temperatures and on different catalyst (rhodium, nickel, copper, etc.) than the industrial status quo. Maximum H2/CO ratios (>10) and methane conversions (>90%) for given metal catalysts under these millisecond-contact-time conditions were determined by varying both the second-stage (WGS) temperature with an external furnace and the amount of excess steam added to the POx system. Kinetic rate expressions for water-gas shift reactions on rhodium and other non-traditional shift catalyst were determined via variable shift temperature experiments in single stage WGS experiments. Further, heat integration was used via a coaxial reactor with a vacuum jacket to determine the current levels of methane conversion and the H2/CO ratios that could be achieved under completely autothermal conditions.




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