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

Abstract

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 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.