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Methanation over transition metal catalysts. III. Co/Al/sub 2/O/sub 3/ in sulfur-poisoning studies

Journal Article · · J. Catal.; (United States)
OSTI ID:6408801
Poisoning of Co/Al/sub 2/O/sub 3/ by H/sub 2/S in CO hydrogenation was studied in an all-quartz recycle reactor; the studies were carried out at atmospheric pressure and at 390/sup 0/C with feed gas containing 1 to 4% CO in H/sub 2/ and 13 to 100 ppB H/sub 2/S. Sulfur-poisoned catalysts were analyzed using Auger electron spectroscopy (AES). Addition of 13 ppB H/sub 2/S reduced the steady-state methanation activity of Co/Al/sub 2/O/sub 3/ by more than 10/sup 3/-fold at 390/sup 0/C; 90 ppB H/sub 2/S reduced the activity 10/sup 4/-fold. AES studies showed that the loss in methanation activity resulted from two-dimensional surface sulfide formation; no sulfur was present in the subsurface regions. In the sulfur poisoning of Co/Al/sub 2/O/sub 3/, carbon plays only a secondary role. Poisoning by sulfur appears to be due primarily to geometric blockage of sites, with one sulfur atom adsorbed per two surface Co atoms. Electronic effects due to sulfur adsorption are also important as evidenced by a 12 kcal/mole reduction in the activation energy for methanation upon poisoning.
Research Organization:
Univ. of Delaware, Newark
OSTI ID:
6408801
Journal Information:
J. Catal.; (United States), Journal Name: J. Catal.; (United States) Vol. 69:2; ISSN JCTLA
Country of Publication:
United States
Language:
English