We report significantly enhanced electrochemical CO reduction (ECR) to CH by tuning the interface of a metal oxide composite (CuO/HfO), enabling a CH faradaic efficiency as high as 62.6 ± 1.3% at 300 mA cm, in contrast to only 11.6 ± 1.6% over pure CuO. Collective knowledge from multiple control experiments, density functional theory calculations, and operando Raman study reveals that the CuO-HfO interface greatly strengthens CO adsorption and the binding of *CO for further C-C coupling to yield CH.
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