期刊
SCIENCE
卷 364, 期 6445, 页码 1091-+出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aaw7515
关键词
-
资金
- European Research Council [681292]
- Ministry of Science and Technology, Taiwan [MOST 107-2628-M-002-015-RSP]
Currently, the most active electrocatalysts for the conversion of CO2 to CO are gold-based nanomaterials, whereas non-precious metal catalysts have shown low to modest activity. Here, we report a catalyst of dispersed single-atom iron sites that produces CO at an overpotential as low as 80 millivolts. Partial current density reaches 94 milliamperes per square centimeter at an overpotential of 340 millivolts. Operando x-ray absorption spectroscopy revealed the active sites to be discrete Fe3+ ions, coordinated to pyrrolic nitrogen (N) atoms of the N-doped carbon support, that maintain their +3 oxidation state during electrocatalysis, probably through electronic coupling to the conductive carbon support. Electrochemical data suggest that the Fe3+ sites derive their superior activity from faster CO2 adsorption and weaker CO absorption than that of conventional Fe2+ sites.
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