Tailoring Pt‐Ni/Fe Coordination in Single‐Atom Pt/NiFe LDH With Facile Synthesis for Efficient and Long‐Term Alkaline Water Electrolysis

Abstract Efficient and durable alkaline water electrolysis at industrial current densities remains a key challenge due to sluggish oxygen evolution kinetics and poor stability of hydrogen evolution reaction (HER) catalysts in alkaline media. Herein, a unique Pt–Ni/Fe coordinated single‐atom Pt catalyst anchored on nickel‐iron layered double hydroxide (ePt/NiFe LDH), is reported synthesized via a facile electrodeposition process within 30 min. Unlike the conventional Pt‐O‐M (metal) coordination, the newly discovered Pt–Ni/Fe bonding structure significantly modulates the electronic structure of the NiFe active sites, thereby synergistically enhancing both HER and OER activities. Benefiting from this optimized coordination environment and the nanoflower architecture, the ePt/NiFe LDH@e‐nf electrode delivers outstanding overall water splitting performance, achieving a low cell voltage of 1.42 V at 10 mA cm −2 and 1.54 V at 100 mA cm −2 without iR compensation. More importantly, it maintains ultrastable operation over 1440 h at an industrial‐level current density of 500 mA cm −2 , outperforming commercial Pt/C–RuO₂ benchmarks. This work demonstrates a promising strategy for designing high‐performance and durable single‐atom catalysts for practical alkaline water electrolysis applications.