弯曲碳表面基团作为合成光气用碳催化剂的活性位。
Bent Carbon Surface Moieties as Active Sites on Carbon Catalysts for Phosgene Synthesis.
机构信息
Technische Universität München, Department of Chemistry and Catalysis Research Center, Lichtenbergstrasse 4, 85748, Garching, Germany.
Laboratory of Inorganic Materials Chemistry, Schuit Institute of Catalysis, Eindhoven University of Technology, PO Box 513, 5600 MB, Eindhoven, The Netherlands.
出版信息
Angew Chem Int Ed Engl. 2016 Jan 26;55(5):1728-32. doi: 10.1002/anie.201508922. Epub 2016 Jan 6.
Active sites in carbon-catalyzed phosgene synthesis from gaseous CO and Cl2 have been identified using C60 fullerene as a model catalyst. The carbon atoms distorted from sp(2) coordination in non-planar carbon units are concluded to generate active Cl2 . Experiments and density functional theory calculations indicate the formation of a surface-bound [C60 ⋅⋅⋅Cl2 ] chlorine species with radical character as key intermediate during phosgene formation. It reacts rapidly with physisorbed CO in a two-step Eley-Rideal-type mechanism.
使用 C60 富勒烯作为模型催化剂，确定了碳催化气相 CO 和 Cl2 合成光气中的活性位。从非平面碳单元中的 sp(2)配位中扭曲的碳原子被认为生成了活性 Cl2。实验和密度泛函理论计算表明，在光气形成过程中，形成了表面结合的 [C60 ⋅⋅⋅Cl2] 氯物种，具有自由基特征，是关键中间体。它在两步 Eley-Rideal 型机理中与物理吸附的 CO 快速反应。
Zotero 插件