Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-017-01673-3
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Funding
- National Natural Science Foundation of China [21476226, 21676045, 21776269, 21176037]
- China Ministry of Science and Technology [2016YFB0600902]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA09030101, XDB17020400]
- Dalian Science Foundation for Distinguished Young Scholars [2016RJ04]
- Youth Innovation Promotion Association CAS
- Natural Science Foundation of Liaoning Province [201602169]
- Fundamental Research Funds for the Central Universities [DUT15LK29]
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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.
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