Publication date: 10th November 2021
Electrocatalytic CO2 reduction (eCO2R) to valuable chemicals and fuels is of fundamental scientific and technological interest. However, it remains a huge challenge to control the selectivity of eCO2R toward certain products with near unity efficiency. Bimetallic electrocatalysts have been regarded as one of the most promising strategies to improve the selectivity of eCO2R, since the introduction of a second metal tunes the adsorption energy of key intermediates (e.g. CO and hydrogen). Here, we fabricated a bimetallic system of Sn-doped CuO nanoparticles for electrochemical CO2 conversion. Electrochemical measurements demonstrate that introduction of a trace amount (0.4 %) of Sn enhances the Faradaic Efficiency (FE) of CO up to 98% at –0.75 V vs. RHE cathodic bias, with a stable performance over the course of 15 h. A volcano-shape relationship is found between the CO enhancement and the percentage of Sn (0-0.8%), with maximum FE for 0.4% Sn doping. Time-dependent in situ Raman spectroscopy measurements reveal the subsequent reduction of CuO and SnO2 domains, which tunes the adsorption of CO at the catalyst surface. Our work showcases the potential of bimetallic electrocatalysts to boost the eCO2R selectivity, and reveals the dynamic restructuring of the electrocatalyst under operating conditions through time-dependent Raman spectroscopy.
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