Dynamic Oxygen-Vacancy Redistribution Regulates the Structural Evolution and Stability of Supported Au Nanoparticles
5 affiliations
- 1Institute of Molecular Plus
- 2Tianjin University
- 3School of Chemical Engineering and Technology
- 4Tiangong University
- 5Tianjin Key Laboratory of Low-Dimensional Electronic Materials and Advanced Instrumentation
Abstract
Supported metal nanoparticles (NPs) on reducible oxides are widely employed as heterogeneous catalysts, where the metal-support interaction plays a pivotal role in determining catalytic activity, stability, and resistance to sintering. Oxygen vacancies (Ovs) in cerium oxide (CeO2-x) are known to modify the electronic and structural properties of the support; however, how their redistribution regulates the structural evolution and stability of supported metal nanoparticles at the atomic scale remains poorly understood. Here, by combining molecular dynamics simulations, density functional theory calculations, and experimental observations, we show that Ovs are preferentially distributed in the second oxygen layer rather than the outermost surface and undergo temperature-dependent redistribution. Increasing Ov concentration induces a pronounced size-dependent structural reconstruction of supported Au NPs, with smaller NPs exhibiting greater flattening associated with enhanced interfacial electron transfer. Meanwhile, vacancy-enhanced metal-support interactions restrict NP mobility and improve resistance to sintering. Under H2O-containing conditions, water dissociation further stabilizes the NPs through surface H species while triggering extensive oxygen redistribution within the CeO2-x lattice. The second oxygen layer accommodates substantial changes in oxygen population while preserving a relatively stable electronic environment, highlighting its role as a dynamic oxygen reservoir. These results establish a unified picture in which oxygen-vacancy dynamics couple support restructuring with the morphology and mobility of supported Au NPs, offering an atomic-scale basis for designing sintering-resistant metal/oxide catalysts.
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BibTeX
@misc{yang2026dynamic,
title = {{Dynamic Oxygen-Vacancy Redistribution Regulates the Structural Evolution and Stability of Supported Au Nanoparticles}},
author = {Siyuan Yang and Zhongliang Cao and Weiwei Zhang and Langli Luo and Xing Chen},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15008960/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008960/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Dynamic Oxygen-Vacancy Redistribution Regulates the Structural Evolution and Stability of Supported Au Nanoparticles
AU - Siyuan Yang
AU - Zhongliang Cao
AU - Weiwei Zhang
AU - Langli Luo
AU - Xing Chen
PY - 2026
DA - 2026/09/16
PB - ChemRxiv
DO - 10.26434/chemrxiv.15008960/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008960/v1
AB - Supported metal nanoparticles (NPs) on reducible oxides are widely employed as heterogeneous catalysts, where the metal-support interaction plays a pivotal role in determining catalytic activity, stability, and resistance to sintering. Oxygen vacancies (Ovs) in cerium oxide (CeO2-x) are known to modify the electronic and structural properties of the support; however, how their redistribution regulates the structural evolution and stability of supported metal nanoparticles at the atomic scale remains poorly understood. Here, by combining molecular dynamics simulations, density functional theory calculations, and experimental observations, we show that Ovs are preferentially distributed in the second oxygen layer rather than the outermost surface and undergo temperature-dependent redistribution. Increasing Ov concentration induces a pronounced size-dependent structural reconstruction of supported Au NPs, with smaller NPs exhibiting greater flattening associated with enhanced interfacial electron transfer. Meanwhile, vacancy-enhanced metal-support interactions restrict NP mobility and improve resistance to sintering. Under H2O-containing conditions, water dissociation further stabilizes the NPs through surface H species while triggering extensive oxygen redistribution within the CeO2-x lattice. The second oxygen layer accommodates substantial changes in oxygen population while preserving a relatively stable electronic environment, highlighting its role as a dynamic oxygen reservoir. These results establish a unified picture in which oxygen-vacancy dynamics couple support restructuring with the morphology and mobility of supported Au NPs, offering an atomic-scale basis for designing sintering-resistant metal/oxide catalysts.
ER -