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

CuNi@C/N-npG has been designed for CO2RR with superior ethanol selectivity of 96.6% at −0.78 V versus RHE. The stronger metal-support interaction increases the intrinsic activity and promotes the stability through the effective regulation of surface electronic structure and electron transfer during the catalytic process. The controllable transition of reaction intermediates improve s the activity and selectivity for ethanol production. 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 demon strated 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 electroca...
Source: Small - Category: Nanotechnology Authors: Tags: Research Article Source Type: research
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