Abstract
The potential of the stopped-flow gas chromatographic reactor (SFGCR) for catalytic investigations was examined through application to methanation studies over alumina-supported nickel and ruthenium catalysts at 375–500 K. It was found that for the SFGCR, the significance of transport resistances could be evaluated more readily than is generally possible with steady state differential flow reactors. Methods for determining the effects of stopped-flow intervals and reversible desorption of reactant on observed rates were also developed. It was demonstrated that for these systems the SFGCR could be operated such that only surface reaction phenomena contributed measurably to observed reaction rates. Rate behavior could be explained by surface heterogeneity, which was substantiated by results from temperature-programmed reaction studies and stopped-flow experiments at varying metal dispersions. The SFGCR was demonstrated to be useful for rapid screening for catalytic activity and structure sensitivity as well as measurement of small rates of reaction.
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