Insights of active sites separation mechanism for highly efficient electrocatalytic N2 reduction to ammonia over glucose-induced metallic MoS2
Ruoqi Liu, Hao Fei, Jian Wang, Ting Guo, Fangyang Liu, Jiayi Wang, Zhuangzhi Wu, Dezhi Wang
Abstract
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 .