Memory-dictated dynamics of single-atom Pt on CeO2 for CO oxidation

Zihao Zhang; Jinshu Tian; Yubing Lu; Shize Yang; Dong Jiang; Weixin Huang; Yixiao Li; Jiyun Hong; Adam S Hoffman; Simon R Bare; Mark H Engelhard; Abhaya K Datye; Yong Wang

doi:10.1038/s41467-023-37776-3

Memory-dictated dynamics of single-atom Pt on CeO₂ for CO oxidation

Nat Commun. 2023 May 9;14(1):2664. doi: 10.1038/s41467-023-37776-3.

Authors

Zihao Zhang^#^{1

2}, Jinshu Tian^#¹, Yubing Lu¹, Shize Yang³, Dong Jiang², Weixin Huang², Yixiao Li², Jiyun Hong⁴, Adam S Hoffman⁴, Simon R Bare⁴, Mark H Engelhard¹, Abhaya K Datye⁵, Yong Wang^{6

7}

Affiliations

¹ Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
² The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA.
³ Eyring Materials Center, Arizona State University, Tempe, AZ, 85257, USA.
⁴ Stanford Synchrotron Radiation Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁵ Department of Chemical and Biological Engineering and Center for Micro-Engineered Materials, University of New Mexico, Albuquerque, NM, 87131, USA.
⁶ Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA. yong.wang@pnnl.gov.
⁷ The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA. yong.wang@pnnl.gov.

^# Contributed equally.

Abstract

Single atoms of platinum group metals on CeO₂ represent a potential approach to lower precious metal requirements for automobile exhaust treatment catalysts. Here we show the dynamic evolution of two types of single-atom Pt (Pt₁) on CeO₂, i.e., adsorbed Pt₁ in Pt/CeO₂ and square planar Pt₁ in Pt_ATCeO₂, fabricated at 500 °C and by atom-trapping method at 800 °C, respectively. Adsorbed Pt₁ in Pt/CeO₂ is mobile with the in situ formation of few-atom Pt clusters during CO oxidation, contributing to high reactivity with near-zero reaction order in CO. In contrast, square planar Pt₁ in Pt_ATCeO₂ is strongly anchored to the support during CO oxidation leading to relatively low reactivity with a positive reaction order in CO. Reduction of both Pt/CeO₂ and Pt_ATCeO₂ in CO transforms Pt₁ to Pt nanoparticles. However, both catalysts retain the memory of their initial Pt₁ state after reoxidative treatments, which illustrates the importance of the initial single-atom structure in practical applications.

Abstract

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