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Identification of single-site gold catalysis in acetylene hydrochlorination

DOI: 10.1126/science.aal3439 DOI Help

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)