%0 Journal Article
%T Crossing the great divide between single-crystal reactivity and actual catalyst selectivity with pressure transients
%J -
%D 2018
%R https://doi.org/10.1038/s41929-018-0167-5
%X The quantitative prediction of catalyst selectivity is essential to the design of efficient catalytic processes and requires a detailed knowledge of the reaction mechanism and rate constants. Here we present a study that accurately predicts, using the kinetics and a mechanism derived from fundamental studies on single-crystal gold, the product distribution resulting from the complex reaction network that governs the oxidative coupling of methanol, catalysed by nanoporous gold between 360 and 425£¿K and for a vast range of pressures. Analysis of the transient product responses to micropulses of methanol over nanoporous gold yields a precise understanding of the marked dependence of selectivity on pressure, surface oxygen coverage and temperature. The key to a high selectivity for methyl formate is the surface lifetime and abundance of the methoxy. This successful microkinetic modelling of catalytic reactions across a wide set of reaction conditions is broadly applicable to predicting catalytic selectivity and provides a pathway to designing more efficient catalytic processes
%U https://www.nature.com/articles/s41929-018-0167-5