电催化N2还原反应(NRR)可以在温和的条件下利用可再生的电力将氮气和质子从电解质水溶液转化为氨,被认为是一种非常有前景的替代哈伯法合成氨技术.但是这项技术也面临巨大的挑战,因为N2分子中的N≡N键非常牢固,需要高活性的催化剂才能将其断裂.和过渡金属相比,主族s区金属在NRR中很少被研究.本文采用第一性原理计算的方法,发现氧掺杂的石墨烯锚定的镁单原子催化剂(Mg-O4)是一种高活性的NRR电催化剂.理论计算结果表明,N2分子能有效地被Mg-O4活化,并通过非解离交替机制被还原成NH3.此外,分子动力学模拟结果显示Mg-O4具有高的稳定性.“,”The electrocatalytic nitrogen reduction reaction ( NRR ) can transform nitrogen and protons from aqueous electrolytes to ammonia by using renewable electricity under ambient conditions, which is a promising technology to replace the Haber-Bosch process. However, this technology is extremely challenging as it requires highly active electrocatalysts to break the stable triple-bonds of N2 . With p bands,main-group s-block metals have been rarely explored in NRR compared with transition metals. Herein, we employ first-principles calculations to propose a Mg single atom catalyst as a promising high-performance electrocatalyst for NRR, where Mg atom is coordinated with four oxygen atoms within graphene ( Mg-O4 ) . Our results reveal that N2 can be efficiently activated on Mg-O4 and reduced into NH3 through the alternating mechanism. Moreover, ab initio molecular dynamics simulations demonstrate the Mg-O4 structure has high stability.