Single-atom gold oxo-clusters prepared in alkaline solutions catalyse the heterogeneous methanol self-coupling reactions

Sufeng Cao, Ming Yang, Ahmed O. Elnabawy, Antonios Trimpalis, Sha Li, Chongyang Wang, Florian Göltl, Zhihengyu Chen, Jilei Liu, Junjun Shan, Mengwei Li, Terry Haas, Karena W. Chapman, Sungsik Lee, Lawrence F. Allard, Manos Mavrikakis, Maria Flytzani-Stephanopoulos

Research output: Contribution to journalArticlepeer-review

43 Scopus citations

Abstract

In an effort to obtain the maximum atom efficiency, research on heterogeneous single-atom catalysts has intensified recently. Anchoring organometallic homogeneous catalysts to surfaces creates issues with retaining mononuclearity and activity, while the several techniques developed to prepare atomically dispersed precious metals on oxide supports are usually complex. Here we report a facile one-pot synthesis of inorganometallic mononuclear gold complexes formed in alkaline solutions as robust and versatile single-atom gold catalysts. The complexes remain intact on impregnation onto supports or after drying in air to give a crystalline powder. They can be used to interrogate the nuclearity of the catalytically active gold site for reactions known to be catalysed by oxidized gold species. We show that the [Au1–Ox]– cluster directs the heterogeneous coupling of two methanol molecules to methyl formate and hydrogen with a 100% selectivity below 180 °C. The reaction is industrially important as well as the key step in methanol steam reforming on gold catalysts.

Original languageEnglish (US)
Pages (from-to)1098-1105
Number of pages8
JournalNature Chemistry
Volume11
Issue number12
DOIs
StatePublished - Dec 1 2019
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Fingerprint

Dive into the research topics of 'Single-atom gold oxo-clusters prepared in alkaline solutions catalyse the heterogeneous methanol self-coupling reactions'. Together they form a unique fingerprint.

Cite this