Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion

Yang, Weiwei; Polo‐Garzon, Felipe; Zhou, Hua; Huang, Zhennan; Chi, Miaofang; Meyer, III, Harry; Yu, Xinbin; Li, Yuanyuan; Wu, Zili

doi:10.1002/anie.202217323

Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion

Journal Article · Tue Dec 06 23:00:00 EST 2022 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202217323· OSTI ID:1994715

^[1]; ^[1]; Zhou, Hua ^[2]; Huang, Zhennan ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Supported Pd single atom catalysts (SACs) have triggered great research interest in methane combustion yet with contradicting views on their activity and stability. Here, in this paper, we show that the Pd SAs can take different electronic structure and atomic geometry on ceria support, resulting in different catalytic properties. By a simple thermal pretreatment to ceria prior to Pd deposition, a unique anchoring site is created. The Pd SA, taking this site, can be activated to Pd^δ+ (0<δ<2) that has greatly enhanced activity for methane oxidation: T₅₀ lowered by up to 130 °C and almost 10 times higher turnover frequency compared to the untreated catalyst. The enhanced activity of Pd^δ+ site is related to its oxygen-deficient local structure and elongated interacting distance with ceria, leading to enhanced capability in delivering reactive oxygen species and decomposing reaction intermediates. This work provides insights into designing highly efficient Pd SACs for oxidation reactions.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 1994715

Alternate ID(s):: OSTI ID: 2427977
OSTI ID: 1914323

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 5 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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single atoms
thermal pretreatment

Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion

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