Remote spin-state engineering of Fe2Ni clusters via a graphdiyne–MXene heterointerface for boosted N2 reduction

Abstract

Electrochemical ammonia synthesis is restricted by sluggish N₂ activation and competing hydrogen evolution. Spin-polarised DFT reveals that the graphdiyne substrate triggers a low- (3.01μ_B) to high-spin (6.91μ_B) transition in Fe₂Ni/MXene, markedly enhancing N₂ activation and hydrogenation. The hybrid catalyst exhibits a low onset potential of 0.39 V per RHE with suppressed hydrogen evolution, highlighting remote substrate-induced spin engineering for catalyst design.