Interfacial Engineering of Ru/Ni Hetero‐Nanoparticles Embedded in N‐Doped Hollow Carbon Polyhedron/Nanotubes Integrated Hierarchical Structures for pH‐Universal Hydrogen Evolution

ABSTRACT The development of low‐budget, efficient, and robust pH‐universal hydrogen evolution reaction (HER) electrocatalysts is greatly essential for making water splitting a viable technology to produce hydrogen. Herein, we report the ingenious design of an advanced HER electrocatalyst composed of Ru/Ni hetero‐nanoparticles in situ encapsulated in N‐doped hollow carbon polyhedron/nanotubes integrated hierarchical superstructures (abbreviated as Ru/Ni@N‐CP CNTs‐0.50 hereafter). The concurrent implementation of interfacial engineering, nanoscale hollowing design, and carbon‐support hybridization renders the resultant Ru/Ni@N‐CP CNTs‐0.50 with modified electronic structure, enriched active sites, and shortened electron/mass transport pathways. Density functional theory (DFT) computations further demonstrate that the construction of Ru/Ni heterojunction can lower the energy barrier for H 2 O dissociation and optimize H* adsorption strength, thereby accelerating HER kinetics. Thanks for the composition and architectural advantages, the well‐designed Ru/Ni@N‐CP CNTs‐0.50 catalyst demonstrates exceptional HER activity, requiring overpotentials of only 29 and 40 mV to achieve a current density of 10 mA cm − 2 in 0.5 M H 2 SO 4 and 1.0 M KOH, respectively. This work reveals a sustainable method for the fabrication of multi‐component Ru‐based electrocatalysts and presents a further deep understanding of synergistic electronic engineering to boost hydrogen evolution.