An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation

Andrew J. Therrien, Alyssa J.R. Hensley, Matthew D. Marcinkowski, Renqin Zhang, Felicia R. Lucci, Benjamin Coughlin, Alex C. Schilling, Jean Sabin McEwen, E. Charles H. Sykes

Research output: Contribution to journalArticlepeer-review

296 Scopus citations

Abstract

Single-atom catalysts have attracted great attention in recent years due to their high efficiencies and cost savings. However, there is debate concerning the nature of the active site, interaction with the support, and mechanism by which single-atom catalysts operate. Here, using a combined surface science and theory approach, we designed a model system in which we unambiguously show that individual Pt atoms on a well-defined Cu2O film are able to perform CO oxidation at low temperatures. Isotopic labelling studies reveal that oxygen is supplied by the support. Density functional theory rationalizes the reaction mechanism and confirms X-ray photoelectron spectroscopy measurements of the neutral charge state of Pt. Scanning tunnelling microscopy enables visualization of the active site as the reaction progresses, and infrared measurements of the CO stretch frequency are consistent with atomically dispersed Pt atoms. These results serve as a benchmark for characterizing, understanding and designing other single-atom catalysts.

Original languageEnglish
Pages (from-to)192-198
Number of pages7
JournalNature Catalysis
Volume1
Issue number3
DOIs
StatePublished - 1 Mar 2018

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