Volume 62, Issue 29 e202302096
Research Article

Tailoring *H Intermediate Coverage on the CuAl2O4/CuO Catalyst for Enhanced Electrocatalytic CO2 Reduction to Ethanol

Tingting Zhang

Tingting Zhang

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

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Bowen Yuan

Bowen Yuan

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

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Wenlong Wang

Wenlong Wang

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

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Prof. Dr. Jing He

Corresponding Author

Prof. Dr. Jing He

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

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Prof. Dr. Xu Xiang

Corresponding Author

Prof. Dr. Xu Xiang

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

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First published: 07 April 2023
Citations: 61

Graphical Abstract

We propose a *H-intermediate-mediating strategy for ethanol electroproduction from CO2RR. The findings reveal that the in situ generated CuAl2O4 in Cu-based catalyst could accelerate water dissociation and tailor *H intermediate coverage, which favors hydrogenation of the *HCCOH to ethanol. This study directs a feasible avenue for mediating *H intermediate coverage and tailoring *H-involved reduction reaction pathways on an efficient and durable Cu-based oxide catalyst.

Abstract

The direct electrochemical conversion of CO2 to multi-carbon products offers a promising pathway for producing value-added chemicals using renewable electricity. However, producing ethanol remains a challenge because of the competitive ethylene formation and hydrogen evolution reactions. Herein, we propose an active hydrogen (*H)-intermediate-mediating strategy for ethanol electroproduction on a layered precursor-derived CuAl2O4/CuO catalyst. The catalyst delivered a Faradaic efficiency of 70 % for multi-carbon products and 41 % for ethanol at current density of 200 mA cm−2 and exhibited a continuous 150 h durability in a flow cell. The intensive spectroscopic studies combined with theoretical calculations revealed that the in situ generated CuAl2O4 could tailor *H intermediate coverage and the elevated *H coverage favors the hydrogenation of the *HCCOH intermediate, accounting for the increased yield of ethanol. This work directs a pathway for enhancing ethanol electroproduction from CO2 reduction by tailoring *H intermediate coverage.

Conflict of interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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