Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 7, Pages 1944-1948Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201712451
Keywords
CO2 reduction; electrocatalysis; metal single sites; metal-organic frameworks; renewable energy
Categories
Funding
- National Key R&D Program of China [2017YFA (0208300)]
- National Natural Science Foundation of China [21522107, 21671180, 21521091, 21390393, U1463202]
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The design of active, selective, and stable CO2 reduction electrocatalysts is still challenging. A series of atomically dispersed Co catalysts with different nitrogen coordination numbers were prepared and their CO2 electroreduction catalytic performance was explored. The best catalyst, atomically dispersed Co with two-coordinate nitrogen atoms, achieves both high selectivity and superior activity with 94% CO formation Faradaic efficiency and a current density of 18.1 mA cm(-2) at an overpotential of 520 mV. The CO formation turnover frequency reaches a record value of 18200 h(-1), surpassing most reported metal-based catalysts under comparable conditions. Our experimental and theoretical results demonstrate that lower a coordination number facilitates activation of CO2 to the CO2 center dot- intermediate and hence enhances CO2 electroreduction activity.
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