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Stabilization of Cu+ by tuning CuO-CeO2 interface for selective electrochemical CO2 reduction to ethylene

Abstract

Electrochemical conversion of carbon dioxide (CO2) to multi-carbon fuels and chemical feedstocks is important but remains challenging. Here we report the stabilization of Cu+ within a CuO-CeO2 interface for efficient and selective electrocatalytic CO2 reduction toward ethylene under ambient conditions. Tuning the CuO/CeO2 interfacial interaction permits dramatic suppression of proton reduction and enhancement of CO2 reduction, with an ethylene faradaic efficiency (FE) as high as 50.0% at −1.1 V (versus the reversible hydrogen electrode) in 0.1 M KHCO3, in stark contrast to 22.6% over pure CuO immobilized on carbon black (CB). The composite catalyst presents a 2.6-fold improvement in ethylene current compared to CuO/CB at similar overpotentials, which also exceeds many recently reported Cu-based materials. The FE for C2H4 maintained over 48.0% even after 9 h of continuous polarization. The Cu+ species are believed to be the adsorption as well as active sites for activation of CO2 molecules, which remains almost unchanged after 1 h of electrolysis. Further density functional theory calculations demonstrate preferred formation of Cu+ at the CuO-CeO2 interface. This work provides a simple avenue to converting CO2 into high-value hydrocarbons by rational stabilization of Cu+ species.

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Supplementary files

Article information


Submitted
05 Jul 2020
Accepted
01 Sep 2020
First published
01 Sep 2020

Green Chem., 2020, Accepted Manuscript
Article type
Paper

Stabilization of Cu+ by tuning CuO-CeO2 interface for selective electrochemical CO2 reduction to ethylene

S. Chu, X. Yan, C. Choi, S. Hong, A. Robertson, J. Masa, B. Han, Y. Jung and Z. Sun, Green Chem., 2020, Accepted Manuscript , DOI: 10.1039/D0GC02279A

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