Pt Atomic Single-Layer Catalyst Embedded in Defect-Enriched Ceria for Efficient CO Oxidation

Shaohua Xie; Liping Liu; Yue Lu; Chunying Wang; Sufeng Cao; Weijian Diao; Jiguang Deng; Wei Tan; Lu Ma; Steven N Ehrlich; Yaobin Li; Yan Zhang; Kailong Ye; Hongliang Xin; Maria Flytzani-Stephanopoulos; Fudong Liu

doi:10.1021/jacs.2c08902

Pt Atomic Single-Layer Catalyst Embedded in Defect-Enriched Ceria for Efficient CO Oxidation

J Am Chem Soc. 2022 Nov 23;144(46):21255-21266. doi: 10.1021/jacs.2c08902. Epub 2022 Nov 2.

Authors

Shaohua Xie¹, Liping Liu², Yue Lu³, Chunying Wang⁴, Sufeng Cao⁵, Weijian Diao⁶, Jiguang Deng⁷, Wei Tan^{1

8}, Lu Ma⁹, Steven N Ehrlich⁹, Yaobin Li⁴, Yan Zhang⁴, Kailong Ye¹, Hongliang Xin², Maria Flytzani-Stephanopoulos⁵, Fudong Liu¹

Affiliations

¹ Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States.
² Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, Virginia 24061, United States.
³ Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China.
⁴ Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China.
⁵ Department of Chemical and Biological Engineering, Tufts University, Medford, Massachusetts 02155, United States.
⁶ Department of Chemical and Biological Engineering, Villanova University, Villanova, Pennsylvania 19085, United States.
⁷ College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124, China.
⁸ State Key Laboratory of Pollution Control and Resource Reuse, School of Environment; Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing University, Nanjing 210023, China.
⁹ National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United States.

PMID: 36322840
DOI: 10.1021/jacs.2c08902

Abstract

The local coordination structure of metal sites essentially determines the performance of supported metal catalysts. Using a surface defect enrichment strategy, we successfully fabricated Pt atomic single-layer (Pt_ASL) structures with 100% metal dispersion and precisely controlled local coordination environment (embedded vs adsorbed) derived from Pt single-atoms (Pt₁) on ceria-alumina supports. The local coordination environment of Pt₁ not only governs its catalytic activity but also determines the Pt₁ structure evolution upon reduction activation. For CO oxidation, the highest turnover frequency can be achieved on the embedded Pt_ASL in the CeO₂ lattice, which is 3.5 times of that on the adsorbed Pt_ASL on the CeO₂ surface and 10-70 times of that on Pt₁. The favorable CO adsorption on embedded Pt_ASL and improved activation/reactivity of lattice oxygen within CeO₂ effectively facilitate the CO oxidation. This work provides new insights for the precise control of the local coordination structure of active metal sites for achieving 100% atomic utilization efficiency and optimal intrinsic catalytic activity for targeted reactions simultaneously.