One-dimensional screw-like MoS2 with oxygen partially replacing sulfur as an electrocatalyst for the N2 reduction reaction

Electrocatalytic nitrogen reduction reaction (NRR) is considered to be an energy-saving method for the production of NH3. However, it is still very challenging to achieve a high NH3 yield and efficiency under ambient conditions. Herein, we for the first time synthesize one-dimensional screw-like MoS2 with oxygen partially replacing sulfur (1D-MoS2-xOy) nanosheets by a one-step solvothermal method as an efficient non-noble metal electrocatalyst for NRR. In a 0.1 M HCl solution, 1D-MoS2-xOy exhibits excellent NRR performance, with a remarkable average ammonia yield rate of 5.56 × 10-8 mol s−1 cm−2 at −0.35 V, and a high Faradaic efficiency of 9.86% at −0.3 V. The isotope labeling experiment proves that the generation of NH3 is completely derived from the feed-in N2. Density functional theory calculations show that MoS2 with oxygen partially replacing sulfur can reduce the Gibbs free energy of the potential determination step (PDS). Besides, the unique screw-like structure can provide more N2 adsorption sites for NRR. This work proposes a promising strategy for the reasonable design of non-precious metal-based NRR electrocatalysts.