Identification of single-site gold catalysis in acetylene hydrochlorination.

نویسندگان

  • Grazia Malta
  • Simon A Kondrat
  • Simon J Freakley
  • Catherine J Davies
  • Li Lu
  • Simon Dawson
  • Adam Thetford
  • Emma K Gibson
  • David J Morgan
  • Wilm Jones
  • Peter P Wells
  • Peter Johnston
  • C Richard A Catlow
  • Christopher J Kiely
  • Graham J Hutchings
چکیده

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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عنوان ژورنال:
  • Science

دوره 355 6332  شماره 

صفحات  -

تاریخ انتشار 2017