Issue 8, 2023

Control of evolution of porous copper-based metal–organic materials for electroreduction of CO2 to multi-carbon products

Abstract

Electrochemcial reduction of CO2 to multi-carbon (C2+) products is an important but challenging task. Here, we report the control of structural evolution of two porous Cu(II)-based materials (HKUST-1 and CuMOP, MOP = metal–organic polyhedra) under electrochemical conditions by adsorption of 7,7,8,8-tetracyanoquinodimethane (TNCQ) as an additional electron acceptor. The formation of Cu(I) and Cu(0) species during the structural evolution has been confirmed and analysed by powder X-ray diffraction, and by EPR, Raman, XPS, IR and UV-vis spectroscopies. An electrode decorated with evolved TCNQ@CuMOP shows a selectivity of 68% for C2+ products with a total current density of 268 mA cm−2 and faradaic efficiency of 37% for electrochemcial reduction of CO2 in 1 M aqueous KOH electrolyte at −2.27 V vs. RHE (reversible hydrogen electrode). In situ electron paramagnetic resonance spectroscopy reveals the presence of carbon-centred radicals as key reaction intermediates. This study demonstrates the positive impact of additional electron acceptors on the structural evolution of Cu(II)-based porous materials to promote the electroreduction of CO2 to C2+ products.

Graphical abstract: Control of evolution of porous copper-based metal–organic materials for electroreduction of CO2 to multi-carbon products

Supplementary files

Article information

Article type
Paper
Submitted
17 jan 2023
Accepted
12 mar 2023
First published
05 apr 2023
This article is Open Access
Creative Commons BY license

Mater. Adv., 2023,4, 1941-1948

Control of evolution of porous copper-based metal–organic materials for electroreduction of CO2 to multi-carbon products

L. Li, L. Shan, A. M. Sheveleva, M. He, Y. Ma, Y. Zhou, M. Nikiel, L. Lopez-Odriozola, L. S. Natrajan, E. J. L. McInnes, M. Schröder, S. Yang and F. Tuna, Mater. Adv., 2023, 4, 1941 DOI: 10.1039/D3MA00033H

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