Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst

Qinggang Liu, Xiaofeng Yang (), Lin Li, Shu Miao, Yong Li, Yanqin Li, Xinkui Wang (), Yanqiang Huang () and Tao Zhang
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Qinggang Liu: Dalian University of Technology
Xiaofeng Yang: Chinese Academy of Sciences
Lin Li: Chinese Academy of Sciences
Shu Miao: Chinese Academy of Sciences
Yong Li: University of Bremen
Yanqin Li: Dalian University of Technology
Xinkui Wang: Dalian University of Technology
Yanqiang Huang: Chinese Academy of Sciences
Tao Zhang: Chinese Academy of Sciences

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: 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.

Date: 2017
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DOI: 10.1038/s41467-017-01673-3

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