Facile Synthesis of Pt–O–Ni Interfacial Sites on MOF‐Derived Carbon Nanomaterials for Efficient Alkaline Hydrogen Evolution

ABSTRACT Developing efficient and durable electrocatalysts for the alkaline hydrogen evolution reaction (HER) is critical for sustainable hydrogen production. In this work, one type of nitrogen‐doped carbon nanosheet derived from a nickel‐based metal‐organic framework (MOF) of Ni‐BTC‐bpy has been prepared, which enables atomic‐scale anchoring of platinum clusters. Subsequently, low‐temperature oxidation is carried out to create well‐defined Pt–O–Ni interfacial sites for efficient alkaline HER. This optimized catalyst of NBP‐NC‐Pt‐O achieves a low overpotential of 28 mV at a current density of 10 mA cm −2 in 1.0 M KOH, and demonstrates accelerated reaction kinetics compared to the commercial Pt/C. Meanwhile, it also exhibits satisfactory long‐term electrocatalytic stability, maintaining 94.3% of its initial activity even after 100‐h electrolysis. Furthermore, theoretical calculations indicate that the designed Pt–O–Ni interface connected by oxygen bridges not only reduces the energy barrier for water dissociation and subsequent hydrogen desorption, but also precisely regulates the electronic structure of the active sites to realize an almost optimal hydrogen adsorption free energy. Finally, this strategy can be widely applied to a series of Ni‐based coordination polymers (e.g., Ni‐ABDC, NiOF‐1, and Ni‐BTC) and shows excellent alkaline HER performance. This study establishes a general and scalable strategy for designing and synthesizing active, low‐platinum catalysts by leveraging synergistic metal‐support interactions in MOF‐derived architectures, with broad implications for sustainable energy conversion technologies.