Surpassing the single-atom catalytic activity limit through paired Pt-O-Pt ensemble built from isolated Pt1 atoms

Hui Wang, Jin-Xun Liu, Lawrence F. Allard, Sungsik Lee, Jilei Liu, Hang Li, Jianqiang Wang, Jun Wang, Se H. Oh, Wei Li, Maria Flytzani-Stephanopoulos, Meiqing Shen (), Bryan R. Goldsmith () and Ming Yang ()
Additional contact information
Hui Wang: Tianjin University
Jin-Xun Liu: University of Michigan
Lawrence F. Allard: Oak Ridge National Laboratory
Sungsik Lee: X-ray Science Division
Jilei Liu: Tufts University
Hang Li: Tianjin University
Jianqiang Wang: Tianjin University
Jun Wang: Tianjin University
Se H. Oh: General Motors Global Research and Development
Wei Li: General Motors Global Research and Development
Maria Flytzani-Stephanopoulos: Tufts University
Meiqing Shen: Tianjin University
Bryan R. Goldsmith: University of Michigan
Ming Yang: General Motors Global Research and Development

Nature Communications, 2019, vol. 10, issue 1, 1-12

Abstract: Abstract Despite the maximized metal dispersion offered by single-atom catalysts, further improvement of intrinsic activity can be hindered by the lack of neighboring metal atoms in these systems. Here we report the use of isolated Pt1 atoms on ceria as “seeds” to develop a Pt-O-Pt ensemble, which is well-represented by a Pt8O14 model cluster that retains 100% metal dispersion. The Pt atom in the ensemble is 100–1000 times more active than their single-atom Pt1/CeO2 parent in catalyzing the low-temperature CO oxidation under oxygen-rich conditions. Rather than the Pt-O-Ce interfacial catalysis, the stable catalytic unit is the Pt-O-Pt site itself without participation of oxygen from the 10–30 nm-size ceria support. Similar Pt-O-Pt sites can be built on various ceria and even alumina, distinguishable by facile activation of oxygen through the paired Pt-O-Pt atoms. Extending this design to other reaction systems is a likely outcome of the findings reported here.

Date: 2019
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DOI: 10.1038/s41467-019-11856-9

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