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Abstract
Catalytic transformation of CO2 to formate is generally realized through bicarbonate hydrogenation in an alkaline environment, while it suffers from a thermodynamic sink due to the considerable thermodynamic stability of the bicarbonate intermediate. Here, we devise a route for the direct catalytic conversion of CO2 over a Schiff-base-modified gold nanocatalyst that is comparable to the fastest known nanocatalysts, with a turnover number (TON) of up to 14,470 over 12 h at 90 °C. Theoretical calculations and spectral analysis results demonstrate that the activation of CO2 can be achieved through a weakly bonded carbamate zwitterion intermediate derived from a simple Lewis base adduct of CO2. However, this can only occur with a hydrogen lacking Lewis base center in a polar solvent. This finding offers a promising avenue for the direct activation of CO2 and is likely to have considerable implications in the fields of CO2 conversion and gold catalytic chemistry.
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Details
1 State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, Dalian, China; Dalian Institute of Chemical Physics, Collaborative Innovation Center of Chemistry for Energy Materials, Chinese Academy of Sciences, Dalian, China
2 Dalian Institute of Chemical Physics, Collaborative Innovation Center of Chemistry for Energy Materials, Chinese Academy of Sciences, Dalian, China
3 Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology, University of Bremen, Bremen, Germany
4 State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, Dalian, China