Electrochemical-driven reconstruction for efficient reduction of carbon dioxide into alcohols

摘要

Electrocatalytic reduction of CO2 into high-value multi-carbon (C_(2+)) alcohols is still challenging, and this is mainly due to the higher energy barrier for generating alcohols over ethylene (C2H4) and the competitive reactions. Herein, the deflect-rich copper electrode derived from surface reconstruction under in situ electrochemical conditions was synthesized, and it exhibited excellent catalytic efficiency for reducing CO2 into high-value alcohols. The faradaic efficiency (FE) of C_(2+) products is up to 70.5, with a high FE(alcohols)/FE(C2H4) ratio of 6.2. The solar-driven electrocatalytic cell enables a high solar-to-energy conversion efficiency of 4.0 for reducing CO2 into alcohols. In situ spec-troscopic investigations and theoretical calculations reveal that the modulation of Cu(I)/Cu(0) interfaces with abundant structural deflects and that halogen ion doping would promote the formation of favorable intermediates for the subsequent coupling reaction of selective alcohol generation. The results provide an aid to refine the interfacial structure and composition for improving reduction of CO2 into alcohols.