Chen Shiyuan, Zhang Kai, Chen Yuhui, Shao Bo, Zeng Chaobin, Yuan Wentao, Yang Hangsheng, Han Zhong-Kang, Jiang Ying, Zhang Ze, Wang Yong
Center of Electron Microscopy and State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, China.
Hitachi High-Technologies (Shanghai) Co., Ltd., Shanghai, China.
Nat Commun. 2025 May 24;16(1):4834. doi: 10.1038/s41467-025-60151-3.
Understanding the oxidation of metal nanoparticles is crucial for various applications, particularly in heterogeneous catalysis, such as catalytic oxidation reactions, where metal nanoparticles are typically dispersed on supports. However, the dynamics of interaction between nanoparticles and oxygen, especially under the influence of supporting materials, remain poorly understood, significantly hindering the precise comprehension and regulation of nanoparticle oxidation dynamics. Here, we elucidate two distinct oxidation dynamics in supported nanoparticles using aberration-corrected environmental (scanning) transmission electron microscopy (E(S)TEM), i.e., preferential self-adaptive oxidation initiating at the nanoparticle-support interface, where the support facilitates oxidation, and surface oxidation, where the support inhibits oxidation. Our systematic calculations, corroborated by experimental validations, demonstrate that the interfacial epitaxial match plays a dominant role in determining the oxidation dynamics in oxygen. It serves as a key indicator for developing a straightforward interface engineering strategy to regulate both self-adaptive and surface oxidation processes. This work highlights the diversity of interface-determined oxidation behaviors and offers a strategy for regulating the oxidation dynamics of supported nanoparticles under identical conditions.
了解金属纳米颗粒的氧化对于各种应用至关重要,特别是在多相催化中,例如催化氧化反应,其中金属纳米颗粒通常分散在载体上。然而,纳米颗粒与氧气之间相互作用的动力学,尤其是在载体材料的影响下,仍然知之甚少,这严重阻碍了对纳米颗粒氧化动力学的精确理解和调控。在这里,我们使用像差校正环境(扫描)透射电子显微镜(E(S)TEM)阐明了负载型纳米颗粒中的两种不同氧化动力学,即优先在纳米颗粒 - 载体界面处引发的自适应氧化,其中载体促进氧化,以及表面氧化,其中载体抑制氧化。我们的系统计算得到了实验验证的支持,表明界面外延匹配在决定氧气中的氧化动力学方面起主导作用。它是开发一种直接的界面工程策略以调控自适应和表面氧化过程的关键指标。这项工作突出了界面决定的氧化行为的多样性,并提供了一种在相同条件下调控负载型纳米颗粒氧化动力学的策略。