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论文类型：期刊论文

发表时间：2017-11-10

发表刊物：NATURE COMMUNICATIONS

收录刊物：Scopus、SCIE、PubMed

卷号：8

期号：1

页面范围：1407

ISSN号：2041-1723

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 degrees 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.