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FUEL 254: Activation of molecular hydrogen on palladium separation membrane surfaces in the presence of H2S

Journal Article · · Abstracts of Papers of the American Chemical Society
OSTI ID:1015117
 [1];  [2];  [2];  [2];  [3]
  1. Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Chemical Engineering
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States). Office of Research and Development

Dense palladium-based membranes are of significant interest for separation of hydrogen from mixed gas streams. In this work, flux measurements, materials characterization, and computational modeling combine to provide a framework for understanding the influence of sulfur on molecular hydrogen's dissociative adsorption on Pd and Pd-alloy surfaces and, thus, a foundation for membrane design improvements. Two modes of sulfur-induced deactivation are observed during membrane flux testing. A corrosive decay mechanism is associated with formation of a thick, low diffusivity, Pd4S scale layer on the membrane surface. In this case, both the surface region and top layer of the scale display Pd4S stoichiometry; Pd-terminated Pd4S low-index faces appear to provide the activity required for hydrogen dissociation. A catalytic poisoning mechanism is not associated with formation of a stable sulfide compound; instead, it may result in formation of a thin, sulfur-rich (relative to Pd4S) overlayer that effectively inhibits the dissociation reaction.

Research Organization:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
Sponsoring Organization:
USDOE Assistant Secretary for Fossil Energy (FE)
OSTI ID:
1015117
Report Number(s):
NETL-TPR--2114
Journal Information:
Abstracts of Papers of the American Chemical Society, Journal Name: Abstracts of Papers of the American Chemical Society Vol. 235; ISSN 0065-7727
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

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