Abstract
Oxidation of CO into CO2 is a major solution to reduce CO emission into the atmosphere and to remove CO in fuel gas cleanup. Furthermore, CO oxidation serves as a prototypical reaction for heterogeneous catalysis. This review provides an overview and an update on how to study catalytic CO oxidation at a strictly molecular level by performing well-controlled gas-phase experiments in combination with quantum chemistry calculations. The advances in the unique catalytic reactivity of single-atom cluster catalysts are emphasized. The catalytically active sites and various mechanistic aspects in the redox couples N2O/CO and O2/CO for the seemingly simple oxidation reaction are described.
摘要
将一氧化碳(CO)氧化成二氧化碳(CO2)是降低大气中CO排 放和相关气体净化的有效方法, CO氧化也是非均相催化领域研究 的重要模型反应. 利用质谱实验结合量子化学理论计算, 研究原子 团簇催化氧化CO能够获得相关催化过程的微观反应机制. 本文综 述了气相原子团簇催化氧化CO的最新研究进展, 重点关注单原子 团簇催化剂独特的催化活性. 围绕CO + N2O → CO2 + N2和2CO + O2→ 2CO2两个催化反应, 本文详细讨论了催化活性位的结构特 点以及不同类型的催化反应机制.
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This work was financially supported by the National Natural Science Foundation of China (21773253).
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He SG proposed the topic and outline of the manuscript. Wang LN collected the related information and drafted the manuscript. Li XN gave some valuable comments.
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Li-Na Wang received her BSc degree in chemistry from Hefei Normal University in 2013, her MSc degree in chemistry from South China University of Technology in 2016, and her PhD degree from the Institute of Chemistry, Chinese Academy of Sciences (ICCAS) in 2019. Her research interests are experimental and theoretical investigations on the reactions of noble-metal-free metal oxide clusters in catalytic CO oxidation.
Xiao-Na Li received her BSc degree in chemistry from Jilin Normal University in 2004, MSc degree in chemistry from Jilin University in 2007, and PhD degree in 2010 from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. She joined the ICCAS in January 2011. Her research interests are experimental and theoretical studies on the reactions of metal oxide clusters in catalytic CO oxidation.
Sheng-Gui He received his BSc degree in physics and PhD degree in chemistry from the University of Science and Technology of China in 1997 and 2002, respectively. After the postdoctoral experience at the University of Kentucky (2002-2005) with Prof. Dennis J. Clouthier and Colorado State University (2005-2007) with Prof. Elliot R. Bernstein, he joined ICCAS in January 2007. His research interests are focused on experimental and theoretical studies on reactive intermediates including free radicals and atomic clusters.
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Wang, LN., Li, XN. & He, SG. Recent research progress in the study of catalytic CO oxidation by gas phase atomic clusters. Sci. China Mater. 63, 892–902 (2020). https://doi.org/10.1007/s40843-019-1206-2
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DOI: https://doi.org/10.1007/s40843-019-1206-2