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Identification of single-site gold catalysis in acetylene hydrochlorination

Malta, Grazia, Kondrat, Simon A., Freakley, Simon J., Davies, Catherine, Lu, Li, Dawson, Simon, Thetford, Adam, Gibson, Emma K., Morgan, David John, Jones, Wilm, Wells, Peter Bernard, Johnston, Peter, Catlow, Charles Richard A., Kiely, Christopher John and Hutchings, Graham John 2017. Identification of single-site gold catalysis in acetylene hydrochlorination. Science 355 (6332) , pp. 1399-1403. 10.1126/science.aal3439

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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.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Advanced Research Computing @ Cardiff (ARCCA)
Cardiff Catalysis Institute (CCI)
Subjects: Q Science > QD Chemistry
Publisher: American Association for the Advancement of Science
ISSN: 0036-8075
Date of First Compliant Deposit: 31 March 2017
Date of Acceptance: 7 March 2017
Last Modified: 19 Oct 2019 22:50
URI: http://orca-mwe.cf.ac.uk/id/eprint/99573

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