An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation
Autor: | Matthew D. Marcinkowski, Benjamin P. Coughlin, Andrew J. Therrien, Felicia R. Lucci, Jean-Sabin McEwen, Renqin Zhang, E. Charles H. Sykes, Alex C. Schilling, Alyssa J. R. Hensley |
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Rok vydání: | 2018 |
Předmět: |
Reaction mechanism
Materials science biology Process Chemistry and Technology Active site Bioengineering 02 engineering and technology Electronic structure 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Biochemistry Atomic units Catalysis 0104 chemical sciences X-ray photoelectron spectroscopy Chemical physics biology.protein Reactivity (chemistry) Density functional theory 0210 nano-technology |
Zdroj: | Nature Catalysis. 1:192-198 |
ISSN: | 2520-1158 |
Popis: | 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. Single-atom catalysts are of growing importance, but the nature of their structure and reactivity remains under debate. Here, Sykes and co-workers show that single Pt atoms on a well-defined Cu2O surface are capable of performing low-temperature CO oxidation, and provide data on the binding site and electronic structure of the Pt atoms. |
Databáze: | OpenAIRE |
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