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

Wang, Hui; Liu, Jin -Xun; Allard, Lawrence F.; Lee, Sungsik; Liu, Jilei; Li, Hang; Wang, Jianqiang; Wang, Jun; Oh, Se H.; Li, Wei; Flytzani-Stephanopoulos, Maria; Shen, Meiqing; Goldsmith, Bryan R.; Yang, Ming

doi:10.1038/s41467-019-11856-9

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

Journal Article · Fri Aug 23 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-11856-9· OSTI ID:1558401

Wang, Hui ^[1]; Liu, Jin -Xun ^[2];

^[3];

^[4]; Liu, Jilei ^[5]; Li, Hang ^[1]; Wang, Jianqiang ^[1]; Wang, Jun ^[1]; Oh, Se H. ^[6]; Li, Wei ^[6]; Flytzani-Stephanopoulos, Maria ^[5]; Shen, Meiqing ^[7];

^[2];

^[6]

Tianjin Univ., Tianjin (China)
Univ. of Michigan, Ann Arbor, MI (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Tufts Univ., Medford, MA (United States)
General Motors Global Research and Development, Warren, MI (United States)
Tianjin Univ., Tianjin (China); Collaborative Innovation Center of Chemical Science and Engineering, Tianjin (China)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NSFC); General Motors Research and Development

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1558401

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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

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