Abstract
In this work, carbon nanotubes with fluorine-rich surface are firstly developed as advanced metal-free catalysts for the electrocatalytic synthesis of urea via co-activation of CO2 and NO3 under ambient conditions. A high yield rate of 6.36 mmol h~(-1) g_(cat.)~(-1) with a corresponding Faradaic efficiency of 18.0% was achieved for the urea formation at - 0.65 V vs. reversible hydrogen electrode. Density functional theory calculations indicate the formation of ~*CO and ~*NH2 intermediates is favorable on F-doped C active sites ('C-F2' moieties), facilitating the C-N coupling reaction to form urea.