The Crystal Plane is not the Key Factor for CO2‐to‐Methane Electrosynthesis on Reconstructed Cu2O Microparticles. (27th December 2021)

• Record Type: Journal Article
• Authors: Deng, Bangwei; Huang, Ming; Li, Kanglu; Zhao, Xiaoli; Geng, Qin; Chen, Si; Xie, Hongtao; Dong, Xing'an; Wang, Hong; Dong, Fan
• Is Part Of: Angewandte Chemie. Volume 134:Number 7(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-12-27
• Subjects: Adsorption Configuration -- CO2 Reduction Reaction -- Cuprous Oxide -- Interface -- Reconstruction; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202114080
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Cu2 O microparticles with controllable crystal planes and relatively high stability have been recognized as a good platform to understand the mechanism of the electrocatalytic CO2 reduction reaction (CO2 RR). Herein, we demonstrate that the in situ generated Cu2 O/Cu interface plays a key role in determining the selectivity of methane formation, rather than the initial crystal plane of the reconstructed Cu2 O microparticles. Experimental results indicate that the methane evolution is dominated on all three different crystal planes with similar Tafel slopes and long‐term stabilities. Density functional theory (DFT) calculations further reveal that *CO is protonated via a similar bridge configuration at the Cu2 O/Cu interface, regardless of the initial crystal planes of Cu2 O. The Gibbs free energy changes (Δ G ) of *CHO on different reconstructed Cu2 O planes are close and more negative than that of *OCCOH, indicating the methane formation is more favorable than ethylene on all Cu2 O crystal planes. Abstract : The in‐depth mechanism of electrocatalytic CO2 reduction on in situ reconstructed Cu2 O microparticles is still ambiguous. Now strong evidence shows that the Cu2 O/Cu interface plays a key role in determining the selectivity of methane production rather than the initial crystal planes of the Cu2 O microparticles.