Issue 15, 2024

Enhanced electrochemical CO2-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Abstract

Electrocatalytic reduction of carbon dioxide (CO2RR) to C2+ products presents an ideal approach to mitigate the continuous accumulation of CO2 for achieving carbon neutrality. However, the selectivity for C2+ products is constrained by the high energy barrier associated with C–C coupling and the sluggishness of multiple proton-coupled electron transfer (PCET), resulting in reduced efficiency and selectivity. Herein, a single-atom Cu catalyst with second-shell S coordination (Cu–C3N4–S) is prepared, exhibiting higher ethylene (C2H4) faradaic efficiency (60.2% at −0.9 V vs. RHE). The second-shell S doping structure is confirmed using a DFT theoretical model combined with synchrotron X-ray absorption spectroscopy. Simultaneously, the adsorption of *CO2 intermediates is detected by in situ Raman spectroscopy, allowing for the inference of potential reaction pathways. It is confirmed that through the regulation of second-shell S doping, a notable reduction in the energy barrier of C–C coupling ensues, concurrently tackling the electron demand in the PECT reaction via the construction of an electron transfer pathway (S–N–Cu) at a lower overpotential. This study contributes novel insights to the design of atomic-sized copper-based catalysts inspired by the indirect coordination and heteroatom regulation technique.

Graphical abstract: Enhanced electrochemical CO2-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Supplementary files

Article information

Article type
Paper
Submitted
28 Dec 2023
Accepted
03 Mar 2024
First published
05 Mar 2024

J. Mater. Chem. A, 2024,12, 9075-9087

Enhanced electrochemical CO2-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Y. Shen, Y. Pan, H. Xiao, H. Zhang, C. Zhu, Q. Fang, Y. Li, L. Lu, L. Ye and S. Song, J. Mater. Chem. A, 2024, 12, 9075 DOI: 10.1039/D3TA08073K

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