Nitric oxide assists nitrogen reduction reaction on 2D MBene: A theoretical study

Electrocatalytic synthesis of ammonia as an environment-friendly and sustainable development method has received widespread attention in recent years. Two-dimensional (2D) materials are a promising catalyst for ammonia synthesis due to their large surface area. In this work, we have constructed a series of 2D metal borides (MBenes) with transition metal (TM) defects (TMd-MBenes) and comprehensively calculated the reactivity of electrocatalytic synthesis of ammonia-based on density functional theory. The results have demonstrated that the TMd-MBenes can effectively activate nitrogen oxide (NO) and nitrogen (N2) molecules thermodynamically. Particularly interesting, the co-chemisorption of O atoms, dissociated from NO, can facilitate the spilled of the inert N2 molecules into single N atoms, which can further hydrogenate into ammonia easily with an ultralow limiting potential of 0.59 V on TMd-MnB. Our research has not only provided clues for catalyst design for experimental study but also paved the way for the industrial application of electrocatalytic ammonia synthesis.