Details

Autor(en) / Beteiligte

• Zhang, Yangyang
• Chen, Yanxu
• Wang, Xiaowen
• Feng, Yafei
• Zhang, Huaikun
• Zhang, Genqiang

Titel

Self‐Polarization Triggered Multiple Polar Units Toward Electrochemical Reduction of CO2 to Ethanol with High Selectivity

Ist Teil von

• Angewandte Chemie International Edition, 2023-06, Vol.62 (26), p.e202302241-n/a

Auflage

International ed. in English

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2023

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Electrochemical conversion of CO2 to highly valuable ethanol has been considered a intriguring strategy for carbon neutruality. However, the slow kinetics of coupling carbon‐carbon (C−C) bonds, especially the low selectivity ethanol than ethylene in neutral conditions, is a significant challenge. Herein, the asymmetrical refinement structure with enhanced charge polarization is built in the vertically oriented bimetallic organic frameworks (NiCu‐MOF) nanorod array with encapsulated Cu2O (Cu2O@MOF/CF), which can induce an intensive internal electric field to increase the C−C coupling for producing ethanol in neutral electrolyte. Particularly, when directly employed Cu2O@MOF/CF as the self‐supporting electrode, the ethanol faradaic efficiency (FEethanol) could reach maximum 44.3 % with an energy efficiency of 27 % at a low working‐potential of −0.615 V versus the reversible hydrogen electrode (vs. RHE) using CO2‐saturated 0.5 M KHCO3 as the electrolyte. Experimental and theoretical studies suggest that the polarization of atomically localized electric fields derived from the asymmetric electron distribution can tune the moderate adsorption of *CO to assist the C−C coupling and reduce the formation energy of H2CCHO*‐to‐*OCHCH3 for the generation of ethanol. Our research offers a reference for the design of highly active and selective electrocatalysts for reducing CO2 to multicarbon chemicals. The asymmetrical refinement structure with self‐polarizing unit possesses benchmark electrocatalytic activity towards CO2 to ethanol reduction on Cu2O@MOF/CF electrodes. Experimental and theoretical studies suggest that the polarization of atomically localized electric fields derived from the asymmetric electron distribution can tune the moderate adsorption of *CO to assist the C−C coupling and reduce the formation energy of CH3CHO* for the generation of ethanol.