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; Ming Yang

doi:10.1038/s41467-019-11856-9

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, Ming Yang

Nuclear Energy Materials Microanalysis

Research output: Contribution to journal › Article › peer-review

288 Scopus citations

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.

Original language	English
Article number	3808
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-11856-9
State	Published - Dec 1 2019

Funding

The work from Tianjin University was supported by the National Key R&D Program (2017YFC0211303), the Natural Science Foundation of China (Grant No. 21576207), and the academic collaboration with GM Global R&D. The computational work was supported by start-up funds provided by the University of Michigan. Microscopy work at ORNL was supported by a Strategic Partnership Project funded by GM Global R&D, and, in part, by the US Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office, Propulsion Materials Program. This research used resources of the Advanced Photon Source, a DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02–06CH11357. J.-X.L. thanks Emiel J.M. Hensen for training in the development of the GCMC code.

Funders	Funder number
DOE Office of Science
GM Global R&D
National Key R&D Program	2017YFC0211303
US Department of Energy
U.S. Department of Energy
Office of Science
Office of Energy Efficiency and Renewable Energy
Argonne National Laboratory
University of Michigan
National Natural Science Foundation of China	21576207
Tianjin University

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Wang, H., Liu, J. X., Allard, L. F., Lee, S., Liu, J., Li, H., Wang, J., Wang, J., Oh, S. H., Li, W., Flytzani-Stephanopoulos, M., Shen, M., Goldsmith, B. R., & Yang, M. (2019). Surpassing the single-atom catalytic activity limit through paired Pt-O-Pt ensemble built from isolated Pt₁ atoms. Nature Communications, 10(1), Article 3808. https://doi.org/10.1038/s41467-019-11856-9

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

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.",

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

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

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