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Kinetics of the methanation reaction over Ru, Ru-Ni, Ru-Cu, and Ni clusters in zeolite Y

Journal Article · · ACS Symp. Ser.; (United States)
OSTI ID:5797706
Kinetics of the methanation reaction over Ru, Ru-Ni, Ru-Cu, and Ni Clusters in zeolite Y were studied in a closed recirculating reactor and a differential flow reactor at 250/sup 0/-230/sup 0/C and 250-500 mm Hg hydrogen. The catalytic activity of RuY was similar to that of Ru on alumina, whereas the activity of NiY was much lower than that of alumina-supported nickel. The activity of RuY decreased about 18 times with the addition of Cu to 1:1 Cu-Ru atomic ratio, but only by approx. 20% with the addition of Ni. The dependence of catalyst activity on hydrogen partial pressure increased from 0.66 to 1.58 in the order NiY < RuNi < RuY < RuCuY. The activation energies were 23.0 and 26.8 kcal/mole for NiY and RuY, respectively, had intermediate values for RuNiY catalysts, but increased up to 36.4 kcal/mole for RuCuY. Deactivation rapidity at 280/sup 0/C decreased in the order Ru/Al/sub 2/O/sub 3/ > RuY > RuCuY > NiY approx. Ni/Al/sub 2/O/sub 3/ > RuNiY. Catalyst treatment with water, carbon monoxide, methane, and ethane showed that only carbon monoxide caused significant deactivation. This effect was attributed to deposition of excess carbon via the Boudart reaction or by dissociation of carbon monoxide; nickel in the bimetallic clusters is believed to hinder these reactions.
Research Organization:
Texas A and M Univ., College Station
OSTI ID:
5797706
Journal Information:
ACS Symp. Ser.; (United States), Journal Name: ACS Symp. Ser.; (United States) Vol. 23:2; ISSN ACSMC
Country of Publication:
United States
Language:
English