Insights of active sites separation mechanism for highly efficient electrocatalytic N2 reduction to ammonia over glucose-induced metallic MoS2

Substituting the Haber-Bosch process with electrocatalytic N2 reduction reaction (NRR) is expected to be realized by optimizing the active sites to boost the sluggish N2 adsorption and the hydrogenation process without interference by the thermodynamically favored hydrogen evolution reaction (HER). Herein, a phase engineering strategy for MoS2 toward NRR is reported. The 1T phase are found to enhance the NRR activity with strong N2 adsorption. Then, the active site separation can weaken the competitive adsorption between H+ and N2 reactant on the Mo-edge, improving the NRR selectivity. More importantly, the HER selective basal plane can serve as an H-provider to further accelerate the hydrogenation process of NRR. The optimal MoS2/C-0.4 possesses a high ammonia yield rate of 80.38 μg h–1 mg–1cat. and Faradaic efficiency (FE) of 23.76%, outperforming almost all MoS2-based electrocatalysts and beyond. This work sheds light on synchronizing the catalytic activity and selectivity for catalytic reactions.