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

Nat Commun. 2019 Aug 23;10(1):3808. doi: 10.1038/s41467-019-11856-9.

Authors

Hui Wang¹, Jin-Xun Liu^{2

3}, Lawrence F Allard⁴, Sungsik Lee⁵, Jilei Liu⁶, Hang Li¹, Jianqiang Wang¹, Jun Wang¹, Se H Oh⁷, Wei Li⁷, Maria Flytzani-Stephanopoulos⁶, Meiqing Shen^{8

9

10}, Bryan R Goldsmith^{11

12}, Ming Yang¹³

Affiliations

¹ School of Chemical Engineering and Technology, Tianjin University, Tianjin, China.
² Department of Chemical Engineering, University of Michigan, Ann Arbor, MI, USA.
³ Catalysis Science and Technology Institute, University of Michigan, Ann Arbor, MI, USA.
⁴ Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA.
⁵ Argonne National Laboratory, X-ray Science Division, Lemont, IL, USA.
⁶ School of Chemical and Biological Engineering, Tufts University, Medford, MA, USA.
⁷ Chemical and Materials Systems Laboratory, General Motors Global Research and Development, Warren, MI, USA.
⁸ School of Chemical Engineering and Technology, Tianjin University, Tianjin, China. mqshen@tju.edu.cn.
⁹ State Key Laboratory of Engines, Tianjin University, Tianjin, China. mqshen@tju.edu.cn.
¹⁰ Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, China. mqshen@tju.edu.cn.
¹¹ Department of Chemical Engineering, University of Michigan, Ann Arbor, MI, USA. bgoldsm@umich.edu.
¹² Catalysis Science and Technology Institute, University of Michigan, Ann Arbor, MI, USA. bgoldsm@umich.edu.
¹³ Chemical and Materials Systems Laboratory, General Motors Global Research and Development, Warren, MI, USA. ming.yang@gm.com.

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.