Zou Xiu-Ping, Wang Li-Na, Li Xiao-Na, Liu Qing-Yu, Zhao Yan-Xia, Ma Tong-Mei, He Sheng-Gui
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemistry and Chemical Engineering, South China University of Technology, 381 Wushan Road, Tianhe District, Guangzhou, 510641, China.
Angew Chem Int Ed Engl. 2018 Aug 20;57(34):10989-10993. doi: 10.1002/anie.201807056. Epub 2018 Jul 23.
The single copper atom doped clusters CuAl O can catalyze CO oxidation by O . The CuAl O clusters are the first group of experimentally identified noble-metal free single atom catalysts for such a prototypical reaction. The reactions were characterized by mass spectrometry and density functional theory calculations. The CuAl O CO is much more reactive than CuAl O in the reaction with CO to generate CO . One adsorbed CO is crucial to stabilize Cu of CuAl O around +I oxidation state and promote the oxidation of another CO. The widely emphasized correlation between the catalytic reactivity of CO oxidation and Cu oxidation state can be understood at the strictly molecular level. The remarkable difference between Cu catalysis and noble-metal catalysis was discussed.
单铜原子掺杂的团簇CuAlO可催化O对CO的氧化反应。CuAlO团簇是第一组通过实验确定的用于此类典型反应的无贵金属单原子催化剂。这些反应通过质谱和密度泛函理论计算进行了表征。在与CO反应生成CO的过程中，CuAlO CO比CuAlO更具反应活性。一个吸附的CO对于稳定CuAlO中处于+I氧化态附近的Cu并促进另一个CO的氧化至关重要。CO氧化催化活性与Cu氧化态之间广泛强调的相关性可以在严格的分子水平上得到理解。讨论了Cu催化与贵金属催化之间的显著差异。
