Defect-rich ZnS nanoparticles supported on reduced graphene oxide for high-efficiency ambient N2-to-NH3 conversion

Electrochemical N 2 reduction is developing as an appealing carbon-neutral strategy for NH 3 artificial synthesis but seriously influenced by requiring high-efficiency electrocatalysts for the N 2 activation at ambient conditions. Here, we reported that defective-rich ZnS nanoparticles supported on reduced graphene oxide (DR ZnS-rGO) acts as a high-efficiency electrocatalyst for ambient N 2 -to-NH 3 conversion with excellent selectivity. In 0.1 M HCl, such DR ZnS-rGO presents a large NH 3 yield of 51.2 μg h –1 mg cat. –1 (−0.15 V vs . reversible hydrogen electrode, RHE) and a high faradic efficiency of 28.2 % (−0.10 V vs . RHE), as well as high electrochemical and structure stability. Isotopic labelling samples experiments reveal that the synthetic NH 3 directly arise from the supplied N 2 . Density functional theory calculations demonstrated that the engineering S vacancies in DR ZnS-rGO not only provide reaction sites for N 2 -to-NH 3 conversion but activate of N 2 molecules.