Abstract
Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti3C2Tx MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at −0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O3 sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.
Highlights
Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies
Cu-SA/Ti3C2Tx exhibits some interlayer-stacked mesopores resulting from the nanosheet structure (Supplementary Fig. 3), which improves the accessibility of active sites, and the overall catalytic performance of the catalyst[36]
A Cu loading of 0.2 wt% was determined by inductively coupled plasma optical emission spectrometry (ICP-OES)
Summary
Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Cu-SA/Ti3C2Tx exhibits some interlayer-stacked mesopores resulting from the nanosheet structure (Supplementary Fig. 3), which improves the accessibility of active sites, and the overall catalytic performance of the catalyst[36]. C2H4 is exclusively produced as the gas product of COR for CuSA/Ti3C2Tx, obtaining a maximum FE of 71% at –0.7 V vs RHE, which is significantly larger than the highest value of 52.7% reported for Cu NPs44 (Supplementary Table 2).
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