Experimental screening of intermetallic alloys for electrochemical CO2 reduction

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Abstract

In this study, we experimentally screen a promising class of intermetallic alloys for the electrochemical reduction of CO2 toward hydrocarbon products. Based on previous DFT-based screening papers, combinations of strongly CO-binding metals such as iron, cobalt, and nickel with weakly CO-binding metals such as gallium, aluminium or zinc were selected as potentially promising catalytic materials. Despite the challenging production of these alloys, we report a general two-step synthesis method for intermetallic alloys and discuss the specific synthesis conditions that must be taken into account when synthesising these materials. After their synthesis, we use a recently developed differential electrochemical mass spectrometry (DEMS) setup to rapidly quantify the CO2 reduction products over a range of potentials. Almost all newly developed intermetallic catalysts are shown to produce methane and ethylene, while the CoSn catalyst showed higher selectivity towards formate production. However, all tested catalysts mostly produced hydrogen and only reduce CO2 to a small extent, despite the favourable computational screening results. We discuss possible reasons for this discrepancy and outline a more holistic approach for linking future DFT studies with experiments.