Remote spin-state engineering of Fe2Ni clusters via 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 graphdiyne substrate triggers a low- (3.01 μB) to high-spin (6.91 μB) transition in Fe2Ni/MXene, markedly enhancing N2 activation and hydrogenation. The hybrid catalyst achieves a low onset potential of 0.39 V/RHE with suppressed hydrogen evolution, highlighting remote substrate-induced spin engineering for catalyst design.