In:
Angewandte Chemie, Wiley, Vol. 135, No. 26 ( 2023-06-26)
Abstract:
Electrochemical conversion of CO 2 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 Cu 2 O (Cu 2 O@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 Cu 2 O@MOF/CF as the self‐supporting electrode, the ethanol faradaic efficiency (FE ethanol ) 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 CO 2 ‐saturated 0.5 M KHCO 3 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 H 2 CCHO*‐to‐*OCHCH 3 for the generation of ethanol. Our research offers a reference for the design of highly active and selective electrocatalysts for reducing CO 2 to multicarbon chemicals.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v135.26
DOI:
10.1002/ange.202302241
Language:
English
Publisher:
Wiley
Publication Date:
2023
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