Phosphides Derived from Nanosheets as Efficient Catalysts for the Hydrogen Evolution Reaction

In this study, we report a versatile strategy for the synthesis of two-dimensional metal-organic frameworks (MOFs) by coordinating nickel salts with 1,1′-ferrocenedicarboxylic acid on ultrathin Ni(OH) 2 nanosheets, offering precise structural control at the nanoscale. These MOFs are then utilized as precursors to construct NiP/NiFeP heterostructures through a carefully controlled phosphorization process, resulting in well-defined interfaces and a hierarchical architecture. The as-prepared NiP/NiFeP heterostructures exhibit outstanding catalytic performance for the hydrogen evolution reaction (HER) in alkaline media (1.0 M KOH), achieving a current density of 10 mA cm - 2 at an overpotential as low as 130 mV. The remarkable activity arises from the synergistic effects of multiple factors: the ferrocene units provide electron-rich pathways that accelerate charge transfer, Fe incorporation induces heterogeneity and abundant active sites, and the intimate interface between NiP and NiFeP enhances the overall catalytic kinetics. Moreover, the heterostructure demonstrates excellent stability under prolonged operation, indicating strong potential for practical applications. This work not only provides a new paradigm for designing MOF-derived heterostructures with tunable electronic structures and interfacial properties, but also offers insights into the rational development of high-efficiency electrocatalysts for sustainable hydrogen production and next-generation energy conversion technologies. The methodology presented here could inspire further exploration of multifunctional MOF-based materials for diverse catalytic and electrochemical applications.