期刊
SCIENCE
卷 349, 期 6253, 页码 1208-1213出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aac8343
关键词
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资金
- U.S. Department of Energy (DOE)/Lawrence Berkeley National Laboratory (LBNL) [101528-002]
- BASF SE (Ludwigshafen, Germany)
- DOE, Office of Science, Office of Basic Energy Sciences, Energy Frontier Research Center [DESC0001015]
- Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, DOE [DE-AC02-05CH11231]
- NSF Graduate Research Fellowships Program
- Amgen Scholar Program
- DOE [DE-AC02-05CH11231]
Conversion of carbon dioxide (CO2) to carbon monoxide (CO) and other value-added carbon products is an important challenge for clean energy research. Here we report modular optimization of covalent organic frameworks (COFs), in which the building units are cobalt porphyrin catalysts linked by organic struts through imine bonds, to prepare a catalytic material for aqueous electrochemical reduction of CO2 to CO. The catalysts exhibit high Faradaic efficiency (90%) and turnover numbers (up to 290,000, with initial turnover frequency of 9400 hour(-1)) at pH 7 with an overpotential of -0.55 volts, equivalent to a 26-fold improvement in activity compared with the molecular cobalt complex, with no degradation over 24 hours. X-ray absorption data reveal the influence of the COF environment on the electronic structure of the catalytic cobalt centers.
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