Boosting electrochemical conversion of CO2 to ethanol through the confinement of pyridinic N-B layer on copper nanoparticles
Yuying Zhao, Qixin Yuan, Ruting Xu, Chenhao Zhang, Kang Sun, Ao Wang, Anqi Zhang, Ziyun Wang, Jianchun Jiang, Mengmeng Fan
Abstract
Developing efficient electrocatalysts for CO2 reduction has gained significant attention in the field of sustainable energy, especially the Cu-based catalysts for CO2 conversion to valuable alcohols. In this study, we developed Cu nanoparticles supported on pyridinic N-B doped graphene nanoribbons/amorphous carbon (Cu/BNC-1) as an electrocatalyst for CO2 reduction, exhibiting substantially improved ethanol (EtOH) conversion rate in terms of activity, selectivity, and stability. The Cu/BNC-1 achieved a remarkable 58.64% Faradaic efficiency (FE) for producing EtOH at -1.0 V vs. RHE with a current density of 20.4 mA cm-2 in 0.5 M KHCO3 electrolyte. In-situ Raman, FT-IR, and density functional theory (DFT) calculations demonstrated that the high C2+ product selectivity of Cu/BNC-1 attributed to the pyridinic N-B modulation, lowering the CO dimerization barrier. Moreover, the synergistic confinement effect of Cu and BNC can stabilize the C-O bond of the ⁎HOCCH intermediate, thereby increasing the yield of EtOH.