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Identification of single-site gold catalysis in acetylene hydrochlorination

Identification of single-site gold catalysis in acetylene hydrochlorination
Identification of single-site gold catalysis in acetylene hydrochlorination
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.
0036-8075
1399-1403
Malta, Grazia
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Kondrat, Simon A.
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Freakley, Simon J.
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Davies, Catherine J.
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Lu, Li
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Dawson, Simon
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Thetford, Adam
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Gibson, Emma K.
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Morgan, David J.
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Jones, Wilm
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Wells, Peter
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Johnston, Peter
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Catlow, C. Richard A.
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Kiely, Christopher J.
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Hutchings, Graham J.
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Malta, Grazia
f8644878-b7a5-4e78-b099-8ea07b1dd233
Kondrat, Simon A.
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Freakley, Simon J.
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Davies, Catherine J.
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Lu, Li
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Dawson, Simon
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Thetford, Adam
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Gibson, Emma K.
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Morgan, David J.
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Jones, Wilm
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Wells, Peter
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Johnston, Peter
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Catlow, C. Richard A.
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Kiely, Christopher J.
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Hutchings, Graham J.
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Malta, Grazia, Kondrat, Simon A., Freakley, Simon J., Davies, Catherine J., Lu, Li, Dawson, Simon, Thetford, Adam, Gibson, Emma K., Morgan, David J., Jones, Wilm, Wells, Peter, Johnston, Peter, Catlow, C. Richard A., Kiely, Christopher J. and Hutchings, Graham J. (2017) Identification of single-site gold catalysis in acetylene hydrochlorination. Science, 355 (6332), 1399-1403. (doi:10.1126/science.aal3439).

Record type: Article

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.

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Accepted/In Press date: 7 March 2017
e-pub ahead of print date: 30 March 2017
Published date: 31 March 2017
Organisations: FIMS

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Local EPrints ID: 407526
URI: https://eprints.soton.ac.uk/id/eprint/407526
ISSN: 0036-8075
PURE UUID: f60f6299-d66a-429d-b0d6-6279366973ba
ORCID for Peter Wells: ORCID iD orcid.org/0000-0002-0859-9172

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Date deposited: 13 Apr 2017 01:05
Last modified: 17 Sep 2019 00:50

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Contributors

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

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