Reversing Pt/C Degradation Via Ni(OH)2‐Wrapping Induced Spreading of Electric Field for Alkaline Hydrogen Evolution Reaction

Abstract Low mass activity due to unfavorable water dissociation and insufficient stability are two primary challenges for Pt catalysts. Herein, we find that the specific adsorption of solvent molecules in the inner Helmholtz plane (IHP) leads to local environmental degradation in the Pt/C catalyst. So, we propose an encapsulation‐confined strategy, by which a poriferous Ni(OH) 2 on Pt nanocages (thereafter Pt/Ni(OH) 2 ) was spatially wrapped to regulate charge transfer. As the heterogeneous interface enables spreading the surface electric field, the wrapped Ni(OH) 2 layer not only optimizes the proton‐coupled electron dynamics but also stabilizes the Pt sites via undifferentiated adsorption of solvent molecules in the IHP, as demonstrated by using identical location transmission electron microscopy (IL‐TEM). Consequently, the Pt/Ni(OH) 2 (11.85 mA/mg Pt at an overpotential of 70 mV) achieves an excellent mass activity of 12.74 times higher than the commercial Pt/C and long‐term durability in 1 M KOH. Our work has gained insights into the architecture of microenvironments‐involved interfaces.