TY - JOUR
T1 - An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation
AU - Therrien, Andrew J.
AU - Hensley, Alyssa J.R.
AU - Marcinkowski, Matthew D.
AU - Zhang, Renqin
AU - Lucci, Felicia R.
AU - Coughlin, Benjamin
AU - Schilling, Alex C.
AU - McEwen, Jean Sabin
AU - Sykes, E. Charles H.
N1 - Publisher Copyright:
© 2018 The Author(s) 2018, under exclusive licence to Macmillan Publishers Ltd, part of Springer Nature.
PY - 2018/3/1
Y1 - 2018/3/1
N2 - 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.
AB - 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.
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U2 - 10.1038/s41929-018-0028-2
DO - 10.1038/s41929-018-0028-2
M3 - Article
AN - SCOPUS:85048011817
VL - 1
SP - 192
EP - 198
JO - Nature Catalysis
JF - Nature Catalysis
IS - 3
ER -