Theoretical study of K3Sb/graphene heterostructure for electrochemical nitrogen reduction reaction

Instead of the energy-intensive Haber-Bosch process, electrochemical nitrogen reduction reaction (NRR) is an exciting new carbon neutral technique for ammonia synthesis under ambient conditions. In this work, we investigated K-based electrocatalysts theoretically and demonstrated that K3Sb/graphene performs excellent activity and inhibits hydrogen evolution on alternating reaction pathway. The first hydrogenation step from N-2* to NNH* was found to be the most energetic and limiting step (0.61 eV). Graphene substrate plays the critical role to promote electronic conductivity between K3Sb and dinitrogen.

Automated summary

Electrochemical nitrogen reduction reaction (NRR) is a promising carbon-neutral technique for ammonia synthesis at ambient conditions. In this study, K3Sb/graphene is investigated as an electrocatalyst, showing excellent activity and inhibiting hydrogen evolution in the alternating reaction pathway. The first hydrogenation step is identified as the most energetic and limiting step (0.61 eV), with graphene playing a critical role in promoting electronic conductivity between K3Sb and dinitrogen.