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 high-performance catalyst for the NRR. In 0.1 M LiClO4, this catalyst attains a high faradaic efficiency of 4.58% and a high NH3 yield of 24.82 μg h−1 mgcat.−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.