Sulfur vacancy engineering of MoS2 via phosphorus incorporation for improved electrocatalytic N2 reduction to NH3

Abstract Electrocatalytic N2 reduction reaction (NRR) serves as a promising approach for converting N2 to NH3 in a sustainable way to replace the energy-intensive Haber-Bosch process. MoS2-based electrocatalysts hold great potentials in catalyzing N2 reduction due to their similarity with active MoFe-co in biological nitrogenase. In this work, we reported a sulfur vacancy-rich MoS2 as an excellent electrocatalyst for NRR, where the sulfur vacancies (SVs) were easily controlled by regulating the amount of P dopants. MoS2 with abundant SVs (P-M-1) achieved a large NH3 yield rate of 60.27 µg h−1 mg−1cat. and high Faradaic efficiency of 12.22% towards NRR. Further mechanistic study revealed that P dopants not only created SVs as the active centers but also modulated the electronic structure for the enhanced adsorption and activation of N2 molecules, thus immensely promoting the catalytic performance of NRR.