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Angew Chem Int Ed Engl. 2018 Feb 12;57(7):1944-1948. doi: 10.1002/anie.201712451. Epub 2018 Jan 16.

Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO2.

Author information

1
Department of Chemistry,iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
2
Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
3
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
4
Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.

Abstract

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 18 200 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.- intermediate and hence enhances CO2 electroreduction activity.

KEYWORDS:

CO2 reduction; electrocatalysis; metal single sites; metal-organic frameworks; renewable energy

PMID:
29266615
DOI:
10.1002/anie.201712451

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