Identification of single-site gold catalysis in acetylene hydrochlorination

Grazia Malta, Simon A Kondrat, Simon J Freakley, Catherine J Davies, Li Lu, Simon Dawson, Adam Thetford, Emma K Gibson, David J Morgan, Wilm Jones, Peter Wells, Peter Johnston, C. Richard A. Catlow, Christopher J. Kiely, Graham J. Hutchings

Research output: Contribution to journalArticlepeer-review

180 Citations (Scopus)

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.
Original languageEnglish
Pages (from-to)1399-1403
Number of pages5
JournalScience
Volume355
Issue number6332
Early online date31 Mar 2017
DOIs
Publication statusPublished - 31 Mar 2017

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