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Cluster catalysis. Propane hydrogenolysis catalyzed by MgO-supported tetrairidium

Journal Article · · Journal of Physical Chemistry; (United States)
DOI:https://doi.org/10.1021/j100100a028· OSTI ID:6879405
; ;  [1]
  1. Univ. of Delaware, Newark, DE (United States) Univ. of California, Davis, CA (United States)

A metal carbonyl cluster with a tetrahedral metal frame, [HIr[sub 4](CO)[sub 11]][sup [minus]], was prepared on the surface of partially hydroxylated MgO powder by adsorption of [Ir[sub 4](CO)[sub 12]]. A supported catalyst was prepared by decarbonylation of the supported [HIr[sub 4](CO)[sub 11]][sup [minus]] by treatment in He followed by H[sub 2] at 300[degree]C. The surface structures were characterized by infrared and X-ray absorption spectroscopies. The decarbonylated cluster had an average Ir-Ir coordination number of 3.4, consistent with the hypothesis that the tetrahedral metal frame was largely retained after decarbonylation. The sample incorporating the decarbonylated clusters was catalytically active for propane hydrogenolysis at 1 atm and 200[degree]C. The catalyst that had been used for 1 day in a flow reactor was characterized by an Ir-Ir coordination number of 3.3. The lack of any significant change in the average cluster size indicates the stability of the supported catalyst, which is modeled as tetrahedral Ir[sub 4] clusters. The rate of the propane hydrogenolysis at 200[degree]C and atmospheric pressure with a H[sub 2]/propane molar ratio of 2.5 was 0.02 molecule of CH[sub 4] produced/(Ir[sub 4] cluster s). 70 refs., 9 figs., 3 tabs.

OSTI ID:
6879405
Journal Information:
Journal of Physical Chemistry; (United States), Journal Name: Journal of Physical Chemistry; (United States) Vol. 98:49; ISSN JPCHAX; ISSN 0022-3654
Country of Publication:
United States
Language:
English