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 N 2 reduction reaction (NRR) is expected to be realized by optimizing the active sites to boost the sluggish N 2 adsorption and the hydrogenation process without interference by the thermodynamically favored hydrogen evolution reaction (HER). Herein, a phase engineering strategy for MoS 2 toward NRR is reported. The 1T phase are found to enhance the NRR activity with strong N 2 adsorption. Then, the active site separation can weaken the competitive adsorption between H+ and N 2 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 MoS 2 /C-0.4 possesses a high ammonia yield rate of 80.38 μg h – 1 mg – 1 cat. and Faradaic efficiency (FE) of 23.76%, outperforming almost all MoS 2 -based electrocatalysts and beyond. This work sheds light on synchronizing the catalytic activity and selectivity for catalytic reactions. [Display omitted] • A high 1T content of 81.45% is obtained by the phase engineering of MoS 2. • 1T-MoS 2 can enhance the NRR activity with strong N 2 adsorption. • Active site separation of Mo-edge and basal plane can improve the NRR selectivity. • Basal plane accelerates the hydrogenation process of NRR as a H-provider. • MoS 2 /C-0.4 exhibits a high NH 3 yield rate of 80.38 μg h – 1 mg – 1 cat. and FE of 23.76%. [ABSTRACT FROM AUTHOR]