Sulfur dots–graphene nanohybrid: a metal-free electrocatalyst for efficient N₂-to-NH₃ fixation under ambient conditions

Abstract

NH3 is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber-Bosch process with huge CO2 emission. Electrochemical N2 reduction offers a carbon-neutral process to convert N2 to NH3 under ambient conditions, but it requires efficient and stable catalysts to drive the N2 reduction reaction. Herein, we report that a sulfur dots-graphene nanohybrid acts as a metal-free electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. When operated in 0.5 M LiClO4, this electrocatalyst achieves a large NH3 yield of 28.56 μg h-1 mgcat.-1 and a high Faradaic efficiency of 7.07% at -0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.