Electrocatalytic Reduction of N Using Metal-Doped Borophene.

Ammonia synthesis is an essential process in chemistry and industry. However, it is limited by the lack of efficient catalysts and high energy costs. Developing highly efficient systems for ammonia synthesis is an important and long-standing challenge. In this paper, a large class of metal atoms (including 3d/4d transition metals and main group metals) anchored onto borophene have been studied as single atom catalysts for ammonia synthesis. After comprehensive computational screening and systematic evaluation, four candidates stand out. We predict that Mo, Mn, Tc, and Cr@BM-β will have superior performance for catalytic reduction of N to NH with low limiting potentials of -0.26, -0.32, -0.38, and -0.48 V, respectively. Furthermore, we studied the activity of the competitive HER on M@BM-β. The results implied that the two materials Mo@BM-β and Mn@BM-β showed HER suppression. These properties exceed most currently reported nitrogen reduction reaction electrocatalysts. Our results suggest the possibility of efficient electrochemical reduction of N to NH in a lower energy process.