The carbon dioxide reduction reaction (CO 2 RR) driven by renewable electricity is a promising way to tackle the CO 2 emission woes and recycle use of CO 2 . The synthesis of electrocatalysts with high activity and selectivity for CO 2 RR to ethylene remains a great challenge. Herein, leaf-like CuO nanosheets are fabricated in situ on nitrogen-doped graphene (NG) by using a novel reduction-oxidation-reconstruction process. When used as a catalyst for the CO 2 RR in 0.1 M KHCO 3 , a high faradaic efficiency of approximately 30 % for ethylene with an ultra-high ethylene/methane ratio of 190 was achieved at À 1.3 V vs. the reversible hydrogen electrode. The SEM and TEM images confirm the leaf-like CuO nanosheets display highcurvature structures, while multiple distinguished grain boundaries constructed by CuO(110) and CuO(111) planes are verified by HRTEM. For the first time, we present a facile method to combine the high-curvature structure and the grain boundary to enhance the selectivity of the CO 2 RR to ethylene over a CuO catalyst.

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