Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases p. 1887 - 1898 (1982)
Update date:2022-08-17
Topics:
Oenal, Isik
Butt, John B.
The hydrogenolysis of methylcyclopropane (MCP) has been used as a probe reaction to investigate the stucture sensitivity of the interactions of a series of well-characterized platinum on silica catalysts with oxygen and carbon monooxide.A differential flow reactor combined with a pulse doser has been used to obtain turnover frequencies for the product n- and isobutane at 273 K and feed composition ca. 0.05 mol fraction MCP.Turnover frequencies for the series of Pt/SiO2, ranging in percentage of exposed metal from 7.1 to 81, are substantially increased as a result of a standardized oxygen pulse pre-treatment as a final step before MCP reaction, and the effect is stucture sensitive.Activity is most enhanced on those catalysts of highest percentage of exposed metal and is also a function of oxygen adsorption temperature, being most pronounced above 473 K.However, selectivity, defined as (i-C4/n-C4), is decreased by oxygen pretreatment.The same series of Pt/SiO2, though, is poisoned by carbon monoxide for the MCP hydrogenolysis under the same conditions.Again the effect is stucture sensitive, with intermediate range percentage exposures preferentially retaining activity for carbon monoxide coverages > 40percent.Selectivity is not affected.Carbon monoxide pulse chemisorption experiments indicated a 1:1 adsorption stoichiometry for CO:Pt in this series at 296 K.
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