Developing highly efficient and durable electrocatalysts for hydrogen evolution reaction (HER) under both alkaline and acidic media is crucial for the future development of a hydrogen economy. However, state-of-the-art high-performance electrocatalysts recently developed are based on carbon carriers mediated by binding noble elements and their complicated processing methods are a major impediment to commercialization. Here, inspired by the high-entropy alloy concept with its inherent multinary nature and using a glassy alloy design with its chemical homogeneity and tunability, we present a scalable strategy to alloy five equiatomic elements, PdPtCuNiP, into a high-entropy metallic glass (HEMG) for HER in both alkaline and acidic conditions. Surface dealloying of the HEMG creates a nanosponge-like architecture with nanopores and embedded nanocrystals that provides abundant active sites to achieve outstanding HER activity. The obtained overpotentials at a current density of 10 mA cm −2 are 32 and 62 mV in 1.0 m KOH and 0.5 m H 2 SO 4 solutions, respectively, outperforming most currently available electrocatalysts. Density functional theory reveals that a lattice distortion and the chemical complexity of the nanocrystals lead to a strong synergistic effect on the electronic structure that further stabilizes hydrogen proton adsorption/desorption. This HEMG strategy establishes a new paradigm for designing compositionally complex alloys for electrochemical reactions.

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Fully crystallized alloys gained by annealing of metallic glasses show excellent rejuvenated catalytic capabilities for ultrafast activation of peroxide. As self-motivated galvanic cells form in the fully crystallized alloys, a grain growth contributing to extensively reduced grain boundaries greatly weakens electron trapping and promotes inner electron transportation, providing a significant insight into exploit novel catalysts.

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Metallic glass (MG), with the superiorities of unique disordered atomic structure and intrinsic chemical heterogeneity, is a new promising and competitive member in the family of environmental catalysts. However, what is at stake for MG catalysts is that their high catalytic efficiency is always accompanied by low stability and the disordered atomic configurations, as well as the structural evolution, related to catalytic performance, which raises a primary obstacle for their widespread applications. Herein, a non-noble and multicomponent Fe 83 Si 2 B 11 P 3 C 1 MG catalyst that presents a fascinating catalytic efficiency while maintaining remarkable stability for wastewater remediation is developed. Results indicate that the excellent efficiency of the MG catalysts is ascribed to a unique atomic coordination that causes an electronic delocalization with an enhanced electron transfer. More importantly, the in situ selfreconstructed hierarchical gradient structure, which comprises a top porous sponge layer and a thin amorphous oxide interfacial layer encapsulating the MG surface, provides matrix protection together with high permeability and more active sites. This work uncovers a new strategy for designing high-performance non-noble metallic catalysts with respect to structural evolution and alteration of electronic properties, establishing a solid foundation in widespread catalytic applications.

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Amorphous metal nanoparticles (A-NPs) have aroused great interest in their structural disordering nature and combined downsizing strategies (e.g. nanoscaling), both of which are beneficial for highly strengthened properties comparing to...