Two Distinct Oxidation Dispersion Mechanisms in Pd-CeO2 Mediated by Thermodynamic and Kinetic Behaviors of Highly Dispersed Pd Species - Details

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Using　environmental　scanning　transmission　electron　microscopy　and　a　global　optimization　algorithm,　we　unraveled　the　preoxidation　dispersion　and　direct　dispersion　mechanisms　in　Pd-CeO2(100)　systems,　mediated　by　the　behaviors　of　highly　dispersed　Pd　species.　At　lower　temperatures,　Pd　nanoparticles　first　undergo　oxidation,　followed　by　the　dispersion　of　PdO　nanoparticles.　In　contrast,　at　higher　temperatures,　Pd　nanoparticles　directly　convert　into　highly　distributed　cationic　Pd　species.　These　distinct　dispersion　mechanisms　are　driven　by　the　thermodynamic　and　kinetic　differences　of　environment-dependent　Pd1-2O　and　Pd1-4O　species,　providing　a　fundamental　basis　for　precisely　controlling　catalyst　dispersion　states.　　©　2025　American　Physical　Society.

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[ 1 ] [Zou C.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 2 ] [Liu W.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 3 ] [Chen S.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 4 ] [Xu Y.]Institute of Molecular Engineering Plus, Institute of Molecule Catalysis and in Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
[ 5 ] [Tang Y.]Institute of Molecular Engineering Plus, Institute of Molecule Catalysis and in Situ/Operando Studies, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
[ 6 ] [Li S.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 7 ] [Yang F.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 8 ] [Yu L.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 9 ] [Zeng C.]Hitachi High-Tech Scientific Solutions (Beijing) Co. Ltd., Beijing, 100015, China
[ 10 ] [Zhang Y.-Y.]Wenzhou Institute, University of Chinese Academy of Sciences, Wenzhou, 325001, China
[ 11 ] [Hu X.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 12 ] [Wang L.]Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, China
[ 13 ] [Han Z.-K.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 14 ] [Jiang Y.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 15 ] [Yuan W.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 16 ] [Yang H.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China
[ 17 ] [Wang Y.]Center of Electron Microscopy, State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China

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Physical Review Letters

ISSN： 0031-9007

Year： 2025

Issue： 21

Volume： 134

8 . 1 0 0

JCR@2023

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ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 1

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