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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 P.; Johnston, Peter; Catlow, C. Richard A.; Kiely, Christopher J.; Hutchings, Graham J.
Science, 03/2017, Volume: 355, Issue: 6332Journal Article
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.
