State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry , Chinese Academy of Sciences , Beijing 100190 , China.
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Center of Excellence in Molecular Sciences , Beijing 100190 , China.
J Phys Chem A. 2019 Oct 31;123(43):9257-9267. doi: 10.1021/acs.jpca.9b05185. Epub 2019 Jul 31.
Oxidation of CO into CO is a prototypical reaction in heterogeneous catalysis and is one of the extensively studied reactions in the gas phase to explore the underlying mechanisms of related catalysis. In this Feature Article, we present and discuss our recent advances in the fundamental understanding of catalytic CO oxidation by O mediated with heteronuclear metal oxide clusters (HMOCs) using state-of-the-art mass spectrometry and quantum chemistry calculations. The HMOCs can be considered as ideal models for active sites on mixed or oxide supported catalysts at a strictly molecular level. A concept of electronegativity-ladder effect was proposed to account for the enhanced reactivity of noble metal (NM) doped HMOCs, and then this effect was successfully extended in the design of NM-free HMOCs in catalytic CO oxidation by O. The future directions and the challenges were also discussed.
一氧化碳氧化为二氧化碳是多相催化中的典型反应，也是气相中广泛研究的反应之一，旨在探索相关催化的基础机制。在这篇专题文章中，我们介绍并讨论了使用最先进的质谱和量子化学计算，在含氧原子介导的异核金属氧化物簇（HMOC）催化一氧化碳氧化方面的基本理解的最新进展。HMOC 可以被视为混合或氧化物负载催化剂上活性位点的理想模型，在严格的分子水平上。我们提出了电负性阶梯效应的概念，以解释掺杂贵金属（NM）的 HMOC 的增强反应性，然后成功地将该效应扩展到 NM 自由的 HMOC 在催化 CO 氧化中的应用。还讨论了未来的方向和挑战。
