A MoS2 nanosheet-reduced graphene oxide hybrid: an efficient electrocatalyst for electrocatalytic N2 reduction to NH3 under ambient conditions

NH3 production heavily relies on the traditional Haber-Bosch process, which is not only energy-intensive (1-3% of human's energy consumption) but also carbon-intensive (1.6% of global CO2 emissions). Electrochemical reduction offers a sustainable and eco-friendly alternative for NH3 synthesis. Despite tremendous efforts, developing N2 reduction reaction (NRR) electrocatalysts with high activity and durability remains a great challenge. Here, we firstly report a MoS2 nanosheet-reduced graphene oxide hybrid (MoS2-rGO) as a highperformance catalyst for the NRR. In 0.1 M LiClO4, this catalyst attains a high faradaic efficiency of 4.58% and a highNH(3) yield of 24.82 mg h(-1) mg(cat.)(-1) at -0.45 V vs. the reversible hydrogen electrode. Notably, such MoS2-rGO shows high electrochemical stability during electrolysis and recycling tests. Density functional theory calculations reveal that the potential-determining step of the proton-electron coupling transferring process is *NHNH2 -> *NH2NH2, and the following hydrogenation steps are feasible.