Single-Atom Catalysis toward Efficient CO2 Conversion to CO and Formate Products

作者：Xiong Su, Xiaofeng Yang, Yanqiang Huang, Bin Liu, Tao Zhang · 发表于：Accounts of Chemical Research · 年份：2018 · DOI：10.1021/acs.accounts.8b00478 · 被引用次数：501 · 研究领域：CO2 Reduction Techniques and Catalysts、Carbon dioxide utilization in catalysis、Catalytic Processes in Materials Science

Conspectus Simply yet powerfully, single-atom catalysts (SACs) with atomically dispersed metal active centers on supports have received a growing interest in a wide range of catalytic reactions. As a specific example, SACs have exhibited distinctive performances in CO2 chemical conversions. The unique structures of SACs are appealing for adsorptive activation of CO2 molecules, transfer of intermediates from support to active metal sites, and production of desirable products in CO2 conversion. In this Account, we have exemplified our recent endeavors in the development of SACs toward CO2 conversions in thermal catalysis and electrocatalysis. In terms of the support not only stabilizing but also working collaboratively with the single active sites, the proper choice of support is of great importance for its stability, activity, and selectivity in single-atom catalysis. Three distinctive strategies for SAC architectureslattice-matched oxide supported, heteroatom-doped carbon anchored, and mimetic ligand chelatedare intensively discussed from the perspective of support design for SACs in different reaction environments. To achieve a high-temperature thermal reduction of CO2 to CO, TiO2 (rutile), lattice-matched to the IrO2 active site, was chosen as a support to realize the thermal stability of Ir1/TiO2 SAC, and it shows great capability toward CO2 conversion and excellent selectivity to CO due to the effective block of the over-reduction of CO2 to methane over single Ir active...