Regulated Surface Electronic States of CuNi Nanoparticles through Metal‐Support Interaction for Enhanced Electrocatalytic CO<sub>2</sub> Reduction to Ethanol
Kaiyue Zhang, Jing Wang, Weining Zhang, Hongfei Yin, Jiuhui Han, Xiaoyong Yang, Weiliu Fan, Yongzheng Zhang, Ping Zhang
Abstract
Abstract Developing stable catalysts with higher selectivity and activity within a wide potential range is critical for efficiently converting CO 2 to ethanol. Here, the carbon‐encapsulated CuNi nanoparticles anchored on nitrogen‐doped nanoporous graphene (CuNi@C/N‐npG) composite are designedly prepared and display the excellent CO 2 reduction performance with the higher ethanol Faradaic effiency (FE ethanol ≥ 60%) in a wide potential window (600 mV). The optimal cathodic energy efficiency (47.6%), Faradaic efficiency (84%), and selectivity (96.6%) are also obtained at −0.78 V versus reversible hydrogen electrode (RHE). Combining with the density functional theory (DFT) calculations, it is demonstrated that the stronger metal‐support interaction (Ni‐N‐C) can regulate the surface electronic structure effectively, boosting the electron transfer and stabilizing the active sites (Cu 0 ‐Cu δ+ ) on the surface of CuNi@C/N‐npG, finally realizing the controllable transition of reaction intermediates. This work may guide the designs of electrocatalysts with highly catalytic performance for CO 2 reduction to C 2+ products.