Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation

Jiang, Dong; Wan, Gang; García-Vargas, Carlos E.; Li, Linze; Pereira-Hernández, Xavier Isidro; Wang, Chongmin; Wang, Yong

doi:10.1021/acscatal.0c02480

Title: Elucidation of the Active Sites in Single-Atom Pd₁/CeO₂ Catalysts for Low-Temperature CO Oxidation

Journal Article · Thu Aug 20 00:00:00 EDT 2020 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.0c02480· OSTI ID:1726231

^[1]; Wan, Gang ^[2];

^[1];

^[3];

^[1]; Wang, Chongmin ^[3];

^[4]

Washington State Univ., Pullman, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Supported precious metals with atomic dispersion are of great interest in catalysis due to their potentials in achieving maximum atom efficiency and unique reactivities. Herein, the active sites for low-temperature CO oxidation are elucidated over single-atom Pd₁/CeO₂ catalysts prepared via high-temperature atom trapping (AT). The increased oxygen vacancies on CeO₂ surface induced by 800 °C air calcination result in decreased Pd–CeO₂ coordinations, i.e., the coordination-unsaturated Pd²⁺ on CeO₂. Light-off and light-out measurements coupled with CO-DRIFTS and X-ray absorption characterization confirm that these coordination-unsaturated Pd²⁺ on CeO₂ are much more reactive than the fully coordinated counterpart, evidenced by a decrease of T₉₀ (temperature to achieve 90% conversion) by ~100 °C in CO oxidation at a gas hourly space velocity of 300 L g^–1 h^–1.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

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

Grant/Contract Number:: AC05-76RL01830; FG02-05ER15712; AC02-06CH11357; AC02-76SF00515

OSTI ID:: 1726231

Report Number(s):: PNNL-SA-155490

Journal Information:: ACS Catalysis, Vol. 10, Issue 19; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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active site
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atom trapping

Title: Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation

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