Advancing electrocatalytic urea synthesis: Insights from 2D benzenehexathiolate coordination nanosheets

Urea, widely used in agriculture and industry, is conventionally produced at substantial energy consumption and CO2 emissions. The use of green and renewable electricity for electrochemical urea synthesis has emerged as an appealing alternative. A variety of catalysts have been explored for urea synthesis. A two-dimensional metal benzenehexathiolato (BHT) coordination nanosheet has high electrical conductivity and diverse coordination structures, making this type of nanostructure an ideal platform for urea synthesis electrocatalysis. Herein, density functional theory (DFT) simulations were employed to probe their electrochemical stability and reaction mechanisms. For Cu-BHT and Ni-BHT, low limiting potentials and C-N coupling barriers were observed, which indicate promising catalytic performance. S-ligands within TM-BHT improved stability and catalytic performance. As a result of this study, advanced catalysts and novel urea synthesis mechanisms can be designed and explored in the future.