Introducing transition-metal components to ceria (CeO₂) is important to tailor the surface redox properties for a broad scope of applications. The emergence of high-entropy oxides (HEOs) has brought transformative opportunities for oxygen defect engineering in ceria yet has been hindered by the difficulty in controllably introducing transition metals to the bulk lattice of ceria. Here, we report the fabrication of ceria-based nanocrystals with surface-confined atomic HEO layers for enhanced catalysis. The increased covalency of the transition-metal–oxygen bonds at the HEO–CeO₂ interface promotes the formation of surface oxygen vacancies, enabling efficient oxygen activation and replenishment for enhanced CO oxidation capabilities. Understanding the structural heterogeneity involving bulk and surface oxygen defects in nanostructured HEOs provides useful insights into rational design of atomically precise metal oxides, whose increased compositional and structural complexities give rise to expanded functionalities.

中文翻译：

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通过高熵氧化物策略增强催化作用的二氧化铈纳米晶体缺陷工程

将过渡金属成分引入二氧化铈 (CeO ₂ ) 对于调整表面氧化还原性能以适应广泛的应用非常重要。高熵氧化物 (HEO) 的出现为二氧化铈中的氧缺陷工程带来了变革性的机会，但由于难以将过渡金属可控地引入二氧化铈的体晶格而受到阻碍。在这里，我们报告了具有表面限制的原子 HEO 层的二氧化铈纳米晶体的制造，以增强催化作用。HEO-CeO _{2处过渡金属-氧键的共价键增加}界面促进表面氧空位的形成，实现有效的氧活化和补充以增强CO氧化能力。了解纳米结构 HEO 中涉及体积和表面氧缺陷的结构异质性为合理设计原子级精确金属氧化物提供了有用的见解，其增加的组成和结构复杂性导致扩展功能。