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

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

doi:10.1021/jacs.2c08902

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

Journal Article · Wed Nov 02 00:00:00 EDT 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c08902· OSTI ID:1973505

^[1]; ^[2]; ^[3]; Wang, Chunying ^[4]; Cao, Sufeng ^[5]; Diao, Weijian ^[6]; ^[3]; ^[7]; Ma, Lu ^[8]; Ehrlich, Steven N. ^[8]; Li, Yaobin ^[4]; ^[4]; Ye, Kailong ^[1]; ^[2]; Flytzani-Stephanopoulos, Maria ^[5]; ^[1]

Univ. of Central Florida, Orlando, FL (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Beijing University of Technology (China)
Chinese Academy of Sciences (China)
Tufts Univ., Medford, MA (United States)
Villanova Univ., PA (United States)
Univ. of Central Florida, Orlando, FL (United States); Nanjing Univ. (China)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

The local coordination structure of metal sites essentially determines the performance of supported metal catalysts. Here, 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1973505

Report Number(s):: BNL-224379-2023-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 46 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
adsoprtion
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chemical structure
oxidation
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Pt Atomic Single-Layer Catalyst Embedded in Defect-Enriched Ceria for Efficient CO Oxidation

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