Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode

Xinchen Kang, Lili Li, Alena Sheveleva, Xue Han, Jiangnan Li, Lifei Liu, Floriana Tuna, Eric J. L. McInnes, Buxing Han (), Sihai Yang () and Martin Schröder ()
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Xinchen Kang: University of Manchester
Lili Li: University of Manchester
Alena Sheveleva: University of Manchester
Xue Han: University of Manchester
Jiangnan Li: University of Manchester
Lifei Liu: Chinese Academy of Science
Floriana Tuna: University of Manchester
Eric J. L. McInnes: University of Manchester
Buxing Han: Chinese Academy of Science
Sihai Yang: University of Manchester
Martin Schröder: University of Manchester

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Electrochemical reduction of carbon dioxide is a clean and highly attractive strategy for the production of organic products. However, this is hindered severely by the high negative potential required to activate carbon dioxide. Here, we report the preparation of a copper-electrode onto which the porous metal–organic framework [Cu2(L)] [H4L = 4,4′,4″,4′′′-(1,4-phenylenebis(pyridine-4,2,6-triyl))tetrabenzoic acid] can be deposited by electro-synthesis templated by an ionic liquid. This decorated electrode shows a remarkable onset potential for reduction of carbon dioxide to formic acid at −1.45 V vs. Ag/Ag+, representing a low value for electro-reduction of carbon dioxide in an organic electrolyte. A current density of 65.8 mA·cm−2 at −1.8 V vs. Ag/Ag+ is observed with a Faradaic efficiency to formic acid of 90.5%. Electron paramagnetic resonance spectroscopy confirms that the templated electro-synthesis affords structural defects in the metal–organic framework film comprising uncoupled Cu(II) centres homogenously distributed throughout. These active sites promote catalytic performance as confirmed by computational modelling.

Date: 2020
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DOI: 10.1038/s41467-020-19236-4

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