Electrocatalytic reduction of CO2 into high-value multi-carbon (C2+) al-cohols is still challenging, and this is mainly due to the higher energy barrier for generating alcohols over ethylene (C2H4) and the competi-tive reactions. Herein, the defect-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 C2+ prod-ucts 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 con-version 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 defects and that halogen ion doping would promote the formation of favor-able 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 alco-hols.
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