格式化
催化作用
纳米材料基催化剂
化学
路易斯酸
碳酸氢盐
席夫碱
胶体金
组合化学
无机化学
有机化学
高分子化学
材料科学
纳米颗粒
纳米技术
作者
Qinggang Liu,Xiaofeng Yang,Lin Li,Shu Miao,Yong Li,Yanqin Li,Xinkui Wang,Yanqiang Huang,Tao Zhang
标识
DOI:10.1038/s41467-017-01673-3
摘要
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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