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Identification of single-site gold catalysis in acetylene hydrochlorination

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Science  31 Mar 2017:
Vol. 355, Issue 6332, pp. 1399-1403
DOI: 10.1126/science.aal3439

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Supported gold ions

The mercuric chloride catalyst for acetylene hydrochlorination creates vinyl chloride, an important polymer feedstock. However, a more environmentally friendly catalyst of gold supported on carbon can now replace mercuric chloride. Malta et al. used x-ray spectroscopic studies of the working catalysts and computational modeling to show that the active species are coexisting single-site Au+ and Au3+ cations. These species are analogs of soluble catalysts with single metal atoms that react via a similar redox couple.

Science, this issue p. 1399

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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