Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
Publication date: 18th July 2023
Electrochemical conversion of CO2 (CO2RR) provides a promising approach for the mitigation of CO2 emissions and the synthesis of industry-value fuels and chemicals [1], [2]. Among multicarbon products (C2), ethylene (C2H4) and ethanol (C2H5OH) display particular industrial relevance to be utilized as chemical feedstocks due to their elevated energy densities [2]. Thus, the development of new catalysts for CO2RR to enable C2+ product formation with high conversion efficiency, selectivity and stability at high industrial current densities is crucial [3]. Another alternative is to decouple the process into two-steps, then enable first the CO2-to-CO followed by CO-to-C2+ products synthesis [2], [4]. In this context, tandem electrodes are an emerging strategy to efficiently promote CO2RR towards C2+, by combining two different catalyst sites with specific selectivity in order to promote the reactions for C2+ products [2], [5]. In this study, we demonstrate the combination of a CO-selective catalyst (NiOx/Ni-N-C) with a C2+-selective catalyst (CuOx/Cu/C) in different configurations as tandem electrodes for CO2RR. The tandem electrode composed of a layered structure of NiOx/Ni-N-C over CuOx/Cu/C on a H23C8 carbon paper (Freudenberg, from Quintech) efficiently produces C2+ in a flow-cell electrolyzer (1 M KOH), achieving a Faradaic Efficiency (FE) for C2H4 up to 39% (jC2H4 of -291 mA cm-2), and for ethanol up to 17% (jC2H5OH of -124 mA cm-2) at a remarkably high current density of -750 mA cm-2. These astonishing results reveal great potential for optimization once this electrode could also reach even higher current densities until ‑1 A cm-2. The tandem electrode strategy allows the advantage of in-situ generation of CO over NiOx/Ni-N-C vicinities and its rapid consumption and conversion by CuOx/Cu/C catalytic sites into profitable C2+ products.
C.A., R.M, I.S., and B.J acknowledge funding by the BMBF in the framework of the NanomatFutur project “MatGasDif” (03XP0263). V.C. is grateful to IMPRS-SURMAT for a Ph.D. fellowship.
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