Iridium Single-Atom Catalyst Performing a Quasi-homogeneous Hydrogenation Transformation of CO2 to Formate

By Xianzhao Shao, Xiaofeng Yang, Jinming Xu, Song Liu, S. Miao, Xiaoyan Liu, X. Su, Hongmin Duan, Yanqiang Huang, Tao Zhang. Chem, 2019

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Summary Heterogeneous single-atom catalysts (SACs) with atomically dispersed active metal centers represent an intermediary between heterogeneous and homogeneous catalysis. In this work, a porous organic polymer with aminopyridine functionalities was designed to fabricate a stable, atomically dispersed Ir catalyst. This Ir-based SAC exhibits excellent catalytic activity during the liquid-phase hydrogenation of CO2 to formate. The associated turnover number is as high as 25,135, representing the best performance yet for a heterogeneous conversion of CO2 to formate. Spectral characterization and density functional theory modeling demonstrate that the chemical structure of the Ir single-atom active site is analogous to that of a homogeneous mononuclear Ir pincer complex catalyst. As a result, a catalytic mechanism similar to that over a homogeneous Ir catalyst occurs during CO2 hydrogenation with this quasi-homogeneous Ir-based SAC. This work suggests a promising basis for the design of efficient SACs for the once-dominant homogeneous catalytic processes.

Subfields: Inorganic Chemistry, Materials Chemistry, Process Chemistry and Technology

View Paper: https://www.semanticscholar.org/paper/42af3a646de536abcb804e2fa3ea2f1cd8588d59