Dynamic and reversible transformations of subnanometre-sized palladium on ceria for efficient methane removal

Jiang, Dong; Wan, Gang; Stenlid, Joakim Halldin; García-Vargas, Carlos E.; Zhang, Jianghao; Sun, Chengjun; Li, Junrui; Abild-Pedersen, Frank; Tassone, Christopher J.; Wang, Yong

doi:10.1038/s41929-023-00983-8

Title: Dynamic and reversible transformations of subnanometre-sized palladium on ceria for efficient methane removal

Journal Article · Thu Jul 20 00:00:00 EDT 2023 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-023-00983-8· OSTI ID:2000051

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

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^[1]; Zhang, Jianghao ^[1]; Sun, Chengjun ^[3];

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Washington State University, Pullman, WA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford University, CA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Washington State University, Pullman, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Reversibly adjusting the active structures of supported metal catalysts in response to dynamic working conditions has long been pursued. Here we report the reaction-environment-modulated transformations of subnanometre-sized Pd on CeO₂ for efficient methane removal, leveraging the reaction environments at different stages of automotive exhaust aftertreatment. During the cold start of vehicles, inactive Pd₁ single atoms are readily transformed into PdO_$$x$$ subnanometre clusters by CO even at room temperature with excess O₂, resulting in boosted low-temperature CH₄ oxidation. At elevated temperatures, dispersion of PdO_$$x$$ cluster into Pd₁ against metal sintering renders outstanding hydrothermal stability to the catalyst, to be activated during the next vehicle start. Combined experimental and computational studies elucidate the dynamically evolved Pd speciation on CeO₂ at an atomic level. In conclusion, modulating the reversible nature of supported metals helps overcome the long-existing trade-off between low-temperature activity and high-temperature stability, also providing a new paradigm for designing intelligent catalysts that brings single-atom/cluster catalysts closer to real applications.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); Knut and Alice Wallenberg Foundation

Grant/Contract Number:: AC02-76SF00515; FG02-05ER15712; AC02-06CH11357; AC02-05CH11231; 2019.0586

OSTI ID:: 2000051

Journal Information:: Nature Catalysis, Vol. 6, Issue 7; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Dynamic and reversible transformations of subnanometre-sized palladium on ceria for efficient methane removal

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