Control of evolution of porous copper-based metal–organic materials for electroreduction of CO2 to multi-carbon products. Issue 8 (5th April 2023)

• Record Type: Journal Article
• Authors: Li, Lili; Shan, Lutong; Sheveleva, Alena M.; He, Meng; Ma, Yujie; Zhou, Yiqi; Nikiel, Marek; Lopez-Odriozola, Laura; Natrajan, Louise S.; McInnes, Eric J. L; Schröder, Martin; Yang, Sihai; Tuna, Floriana
• Is Part Of: Materials advances. Volume 4:Issue 8(2023)
• Page Start: 1941
• Page End: 1948
• Publication Date: 2023-04-05
• Subjects: 620.11
• DOI: 10.1039/d3ma00033h
• Languages: English
• ISSNs: 2633-5409

Abstract

Abstract : Formation of multi-carbon (C2+ ) products by electrochemical reduction of CO2 using two porous Cu(ii )-based materials (HKUST-1 and CuMOP, MOP = metal–organic polyhedra) under electrochemical conditions in the presence of TNCQ. 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.