Ultrafine Pt Nanoparticles Anchored on 2D Metal−Organic Frameworks as Multifunctional Electrocatalysts for Water Electrolysis and Zinc–Air Batteries

Abstract Multifunctional electrocatalysts are crucial to cost‐effective electrochemical energy conversion and storage systems requiring mutual enhancement of disparate reactions. Embedding noble metal nanoparticles in 2D metal–organic frameworks (MOFs) are proposed as an effective strategy, however, the hybrids usually suffer from poor electrochemical performance and electrical conductivity in operating conditions. Herein, ultrafine Pt nanoparticles strongly anchored on thiophenedicarboxylate acid based 2D Fe‐MOF nanobelt arrays (Pt@Fe‐MOF) are fabricated, allowing sufficient exposure of active sites with superior trifunctional electrocatalytic activity for hydrogen evolution, oxygen evolution, and oxygen reduction reactions. The interfacial Fe─O─Pt bonds can induce the charge redistribution of metal centers, leading to the optimization of adsorption energy for reaction intermediates, while the dispersibility of ultrafine Pt nanoparticles contributes to the high mass activity. When Pt@Fe‐MOF is used as bifunctional catalysts for water‐splitting, a low voltage of 1.65 V is required at 100 mA cm⁻² with long‐term stability for 20 h at temperatures (65 °C) relevant for industrial applications, outperforming commercial benchmarks. Furthermore, liquid Zn–air batteries with Pt@Fe‐MOF in cathodes deliver high open‐circuit voltages (1.397 V) and decent cycling stability, which motivates the fabrication of flexible quasisolid‐state rechargeable Zn–air batteries with remarkable performance.