Improving the Nitrogen Reduction Reaction Performance of MoS<sub>2</sub> via a Synergetic Effect: A Density Functional Theory Study
Lanlan Chen, Yanan Zhou, Yifei Rao, Mingxin Qin, Bingbing Gong, Wenhua Zhang, Zhenyu Li
Abstract
Fe atom-decorated MoS2 has been discovered as a stable and noble-metal-free catalyst for nitrogen reduction reaction (NRR) at ambient conditions. In this work, the catalytic performance of Fe- and O-decorated planar and edge MoS2 for NRR is evaluated based on density functional theory calculations. Our calculations show that the synergetic effect between a single Fe atom and the directly bonded oxygen atoms in the Mo-edge of MoS2 (Fe1-1O, 2O, 3O, 4O@Mo-edge-MoS2) is actually responsible for the high-performance of the NRR, and the modest charge transfer between Fe and the support in Fe1-1O, 2O, 3O, 4O@Mo-edge-MoS2 will greatly promote the NRR activity and selectivity. Fe1-4O@Mo-edge-MoS2 presents the highest activity and selectivity among all our investigated models. Thus, modulating the oxygen coordination of single Fe atoms doped in Mo-edge-MoS2 to a modest level will greatly increase the NRR performance.