Stabilization of Cu+ by tuning a CuO–CeO2 interface for selective electrochemical CO2 reduction to ethylene. Issue 19 (23rd September 2020)

• Record Type: Journal Article
• Authors: Chu, Senlin; Yan, Xupeng; Choi, Changhyeok; Hong, Song; Robertson, Alex W.; Masa, Justus; Han, Buxing; Jung, Yousung; Sun, Zhenyu
• Is Part Of: Green chemistry. Volume 22:Issue 19(2020)
• Page Start: 6540
• Page End: 6546
• Publication Date: 2020-09-23
• Subjects: Environmental chemistry -- Industrial applications -- Periodicals; Environmental management -- Periodicals; 660
• DOI: 10.1039/d0gc02279a
• Languages: English
• ISSNs: 1463-9262

Abstract

Abstract : By utilizing the synergistic interaction between CuO and CeO2, the stabilization of Cu + species at a metal–oxide interface is realized. H2 production is considerably suppressed, resulting in enhanced ethylene production with a high FE of 50.0%. Abstract : Electrochemical conversion of carbon dioxide (CO2 ) into 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 to 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 ( vs. 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 that of CuO/CB at similar overpotentials, which also exceeds many recently reported Cu-based materials. The FE of C2 H4 remained at 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 the activation of CO2 molecules, which remain almost unchanged after 1 h of electrolysis. Further density functional theory calculations demonstrate the preferred formation of Cu + at the CuO–CeO2 interface. This work provides a simple avenue to convert CO2 into high-value hydrocarbons by rational stabilization of Cu + species.