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<p>The distribution and interaction of oxygen vacancies (V<sub>O</sub>s) critically influence the properties of metal oxides, especially ceria, which is widely used in high-temperature industrial applications. However, V<sub>O</sub> behavior at elevated temperatures remains poorly understood due to the complexity of their interactions and the lack of predictive models. Here, we uncover a periodic one-dimensional subsurface channel on CeO<sub>2</sub> (110), formed by ordered V<sub>O</sub> distributions at high temperatures. This discovery is enabled by in-situ scanning transmission electron microscopy (STEM), first-principles calculations, and a compressed sensing-assisted cluster expansion model. Strong repulsive interactions between neighboring V<sub>O</sub>s drive their ordering, which relieves local stress from V<sub>O</sub>s and polarons and promotes channel formation. A large band gap between the occupied O 2<i>p</i> and unoccupied Ce 4 <i>f</i> band centers helps stabilize this structure. The resulting subsurface channel features sub-nanometer pores and polaron accumulation, enabling directional proton transfer and provides insights into the high catalytic activity of ceria in hydrogenation reactions. These findings not only offer a deeper understanding of V<sub>O</sub> interactions and their underlying mechanisms but also suggest strategies for tailoring V<sub>O</sub> behavior in metal oxides for advanced catalytic and energy applications.</p>

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Periodic one-dimensional subsurface channels induced by ordered oxygen vacancies on CeO2 (110)

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月1日

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  • Guanxing Li,
  • Xiaojuan Hu,
  • Chen Zou,
  • Songda Li,
  • Zhong-Kang Han,
  • Wentao Yuan,
  • Ze Zhang,
  • Yong Wang

摘要

The distribution and interaction of oxygen vacancies (VOs) critically influence the properties of metal oxides, especially ceria, which is widely used in high-temperature industrial applications. However, VO behavior at elevated temperatures remains poorly understood due to the complexity of their interactions and the lack of predictive models. Here, we uncover a periodic one-dimensional subsurface channel on CeO2 (110), formed by ordered VO distributions at high temperatures. This discovery is enabled by in-situ scanning transmission electron microscopy (STEM), first-principles calculations, and a compressed sensing-assisted cluster expansion model. Strong repulsive interactions between neighboring VOs drive their ordering, which relieves local stress from VOs and polarons and promotes channel formation. A large band gap between the occupied O 2p and unoccupied Ce 4 f band centers helps stabilize this structure. The resulting subsurface channel features sub-nanometer pores and polaron accumulation, enabling directional proton transfer and provides insights into the high catalytic activity of ceria in hydrogenation reactions. These findings not only offer a deeper understanding of VO interactions and their underlying mechanisms but also suggest strategies for tailoring VO behavior in metal oxides for advanced catalytic and energy applications.