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Identification of single-site gold catalysis in acetylene hydrochlorination.

Research paper by Grazia G Malta, Simon A SA Kondrat, Simon J SJ Freakley, Catherine J CJ Davies, Li L Lu, Simon S Dawson, Adam A Thetford, Emma K EK Gibson, David J DJ Morgan, Wilm W Jones, Peter P PP Wells, Peter P Johnston, C Richard A CR Catlow, Christopher J CJ Kiely, Graham J GJ Hutchings

Indexed on: 01 Apr '17Published on: 01 Apr '17Published in: Science



Abstract

There remains considerable debate over the active form of gold under operating conditions of a recently validated gold catalyst for acetylene hydrochlorination. We have performed an in situ x-ray absorption fine structure study of gold/carbon (Au/C) catalysts under acetylene hydrochlorination reaction conditions and show that highly active catalysts comprise single-site cationic Au entities whose activity correlates with the ratio of Au(I):Au(III) present. We demonstrate that these Au/C catalysts are supported analogs of single-site homogeneous Au catalysts and propose a mechanism, supported by computational modeling, based on a redox couple of Au(I)-Au(III) species.