Journal
ACS CATALYSIS
Volume 7, Issue 3, Pages 1520-1525Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b03353
Keywords
CO2 reduction; electrocatalysis; iron Fe-N-C materials; structure-selectivity relationship
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Selective electrochemical reduction of CO, into energy-dense organic compounds is a promising strategy for using CO, as a carbon source. Herein, we investigate a series of iron-based catalysts synthesized by pyrolysis of Fe-, N-, and C-containing precursors for the electroreduction of CO, to CO under aqueous conditions and demonstrate that the selectivity of these materials for CO2 reduction over proton reduction is governed by the ratio of isolated FeN4 sites vs Fe-based nanoparticles. This ratio can be synthetically tuned to generate electrocatalysts producing controlled CO/H-2 ratios. It notably allows preparing materials containing only FeN4 sites, which are able to selectively reduce CO, to CO in aqueous solution with Faradaic yields of over 90% and at low overpotential.
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