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Surface and reaction studies of the sulfur poisoning of transition metal methanation catalysts

Thesis/Dissertation ·
OSTI ID:6320345
Surface and reaction studies of the sulfur poisoning of transition metal methanation catalysts (cobalt, iron, and ruthenium or alumina) at 200/sup 0/-400/sup 0/C, 1 atm, 0-16% carbon monoxide in hydrogen, and 0-100 ppb hydrogen sulfide showed that the catalysts underwent more than 1000-fold reduction in methanation activity in the presence of 13 ppb hydrogen sulfide. The sulfur-poisoning was due primarily to geometric blockage of the surface sites. Cobalt and iron underwent more than 100-fold deactivation due to bulk carburization of the metal and formation of multilayer graphitic deposits on the surface. The activation energy for methanation on ruthenium was independent of sulfur and carbon deactivation, indicating the absence of electronic effects which are induced by bulk carburization of cobalt and iron and by formation of a surface sulfide layer. Carbon and sulfur appeared to cause similar electronic changes in the metal surfaces as indicated by the kinetic behavior in methanation.
OSTI ID:
6320345
Country of Publication:
United States
Language:
English