Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst
Year: 2017
Type: article
Abstract: Catalytic transformation of CO 2 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 CO 2 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 CO 2 can be achieved through a weakly bonded carbamate zwitterion intermediate derived from a simple Lewis base adduct of CO 2 . 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 CO 2 and is likely to have considerable implications in the fields of CO 2 conversion and gold catalytic chemistry.
Source: Nature Communications
Language: English
Subfield: Process Chemistry and Technology
Field: Chemical Engineering
Domain: Physical Sciences
SDG: Climate action
Open Access status: gold
Estimated APC paid: $6,990
Funders: National Natural Science Foundation of China, Chinese Academy of Sciences, Youth Innovation Promotion Association of the Chinese Academy of Sciences, Natural Science Foundation of Liaoning Province, Fundamental Research Funds for the Central Universities, Youth Innovation Promotion Association, Science Fund for Distinguished Young Scholars of Dalian Province
OpenAlex ID: W2768004292