Abstract
As the sole metal that could reduce CO2 to substantial amounts of hydrocarbons, Cu plays an important role in electrochemical CO2 reduction, despite its low energy efficiency. Surface morphology modification is an effective method to improve its reaction activity and selectivity. Different from the pretreated modification method, in which the catalysts self-reconstruction process was ignored, we present operando synthesis by simultaneous electro-dissolution and electro-redeposition of copper during the CO2 electroreduction process. Through controlling the cathodic potential and CO2 flow rate, various high-curvature morphologies including microclusters, microspheres, nanoneedles, and nanowhiskers have been obtained, for which the real-time activity and product distribution is analyzed. The best CO2 electro-reduction activity and favored C2H4 generation activity, with around 10% faradic efficiency, can be realized through extensively distributed copper nanowhiskers synthesized under 40 mL/min flow rate and −2.1 V potential.
Highlights
Excessive CO2 emission has caused severe climate and environment problems, which is breaking the sustainability of human society
I-t curves at different bias and potentials during operando of copper to evaluate the activity of CO2 reduction reaction (CO2 RR), a gas chromatograph (GC)synthesis was connected to thewere vent shown of H-type evaluate the activity of CO
Films four samples swept to different end potentials had a similar granular morphology with the similar
Summary
Excessive CO2 emission has caused severe climate and environment problems, which is breaking the sustainability of human society. The bromide-promoted morphology of copper dendrites was proven to be a highly selective electrocatalyst, which reduced CO2 to ethylene with a faradic efficiency of 57% at a high current density of 170 mA/cm2 [21]. The selectivity of these kinds of copper electrodes was caused by the high-index faces and the under-coordinated sites on the high-curvature structures; the identification of active sites and the recognition of corresponding catalytic mechanisms were generally based on such pretreated morphology. The correlation between the property and structure of such kind of copper catalyst is straightforward, which improves the understanding of CO2 RR mechanism and offers guidelines of rational design for advanced electrocalysts
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