Interfacial Disorder Platinum Boosts Trifunctional Performance for Hydrazine‐Assisted Self‐Driven Hydrogen Generation

Abstract The integration of hydrazine fuel cells with overall hydrazine splitting establishes a sustainable strategy for self‐driven hydrogen generation, yet faces fundamental challenges in synchronous trifunctional catalysis. Herein, carbon defects are engineered at adjacent Pt particles to reconfigure Pt atomic arrangements at interfaces, creating disordered Pt sites through controlled defect‐metal interactions. Mechanistic studies reveal these metastable configurations simultaneously optimize *H adsorption energy while accelerating *O 2 →*OOH hydrogenation and *N 2 H 4 →*N 2 H 3 dehydrogenation processes. The resultant catalyst achieves 1.08 mmol h −1 self‐driven H 2 production comparable with mixed noble metal electrode systems in integrated hydrogen evolution‐hydrazine oxidation‐oxygen reduction reaction performance. This innovation establishes a defect‐mediated atomic engineering paradigm for multi‐reaction cascade systems, demonstrating critical interfacial disorder‐performance relationships in sustainable energy conversion.