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Identification of single-site gold catalysis in acetylene hydrochlorination
Authors:
Grazia
Malta
(Cardiff Catalysis Institute, Cardiff University)
,
Simon A.
Kondrat
(Cardiff Catalysis Institute, Cardiff University)
,
Simon J.
Freakley
(Cardiff Catalysis Institute, Cardiff University)
,
Catherine J.
Davies
(Cardiff Catalysis Institute, Cardiff University)
,
Li
Lu
(Lehigh University)
,
Simon
Dawson
(Cardiff Catalysis Institute, Cardiff University)
,
Adam
Thetford
(UK Catalysis Hub; University College London)
,
Emma K.
Gibson
(University College London)
,
David J.
Morgan
(Cardiff Catalysis Institute, Cardiff University)
,
Wilm
Jones
(UK Catalysis)
,
Peter
Wells
(UK Catalysis; University College London; University of Southampton; Diamond Light Source)
,
Peter
Johnston
(Johnson Matthey PLC)
,
C. Richard A.
Catlow
(Cardiff Catalysis Institute, Cardiff University; UK Catalysis Hub; University College London)
,
Christopher J.
Kiely
(Lehigh University)
,
Graham J.
Hutchings
(Cardiff Catalysis Institute, Cardiff University)
Co-authored by industrial partner:
Yes
Type:
Journal Paper
Journal:
Science
, VOL 355
, PAGES 1399 - 1403
State:
Published (Approved)
Published:
March 2017
Diamond Proposal Number(s):
10306
,
11398
,
15214
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.
Journal Keywords: catalysis; acetylene hydrochlorination; XAFS; XRD; DFT; STEM - HAADF
Subject Areas:
Chemistry
Instruments:
B18-Core EXAFS
Added On:
03/04/2017 14:03
Discipline Tags:
Physical Chemistry
Catalysis
Chemistry
Technical Tags:
Spectroscopy
X-ray Absorption Spectroscopy (XAS)
Extended X-ray Absorption Fine Structure (EXAFS)