One‐pot synthesis of <scp>PtNi</scp> /carbon composites derived from polytetrahydrofuran for bifunctional alkaline <scp>HER</scp> and <scp>ORR</scp>

Abstract Developing robust carbon‐supported electrocatalysts through simplified synthesis is crucial for scalable hydrogen‐energy technologies. Herein, we report a one‐pot, poly(tetrahydrofuran) (PTHF)‐derived PtNi/C architecture in which PTHF serves as a carbon precursor/support and enables in situ carbonization of PTHF to a carbon‐bridged nanoparticle network during Pt–Ni nucleation and alloying in a single thermal step. The resulting catalyst delivers efficient alkaline HER and, importantly, sustains hydrogen evolution deep into the high‐current‐density regime with strong operational durability, addressing a key limitation of many PtNi‐based catalysts commonly evaluated only at low currents. Impedance and surface‐accessibility analyses indicate that the integrated carbon framework lowers interfacial resistive losses and stabilizes electrode connectivity, thereby reducing voltage penalties under high‐rate operation. Beyond HER, the same junction‐engineered PtNi/C also shows promising alkaline ORR activity with a predominantly near four‐electron pathway, highlighting the broader utility of this carbon‐integration concept.