Regulated Surface Electronic States of CuNi Nanoparticles through Metal‐Support Interaction for Enhanced Electrocatalytic CO2 Reduction to Ethanol

• DOI: 10.1002/smll.202300281
• Publication Date: 2023-04-19T03:56:02Z
• Authors: Kaiyue Zhang; Jing Wang; Weining Zhang; Hongfei Yin; Jiuhui Han; Xiaoyong Yang; Weiliu Fan; Yongzheng Zhang; Ping Zhang
• Keywords: 01 natural sciences; 0104 chemical sciences

AbstractDeveloping stable catalysts with higher selectivity and activity within a wide potential range is critical for efficiently converting CO2 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 CO2 reduction performance with the higher ethanol Faradaic effiency (FEethanol ≥ 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 (Cu0‐Cuδ+) 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 CO2 reduction to C2+ products.