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Developing novel non-precious metal-based catalysts is crucial to achieving low-cost, stable, and industrial-grade overall water splitting. Although NiSe2 shows significant promise as an electrocatalyst due to its excellent electrical conductivity and stability in acidic and alkaline environments, its performance is limited by inherently poor activity. In this study, a nanorod-shaped CoxNi1-xSe2@Co(OH)2/nickel foam (CNSC/NF) alkaline water-splitting catalyst was constructed in situ through a hydrothermal-gamma radiation method. The gamma radiation imparted NiSe2 with an "island-like" amorphous/crystalline heterostructure and a high density of atomic-level Ni-Se-Co electron bridge structures. The dense "ball-stick" configuration and heterointerfaces in CNSC/NF jointly enhanced structural stability for ampere-level water splitting. CNSC/NF achieved a current density of 1 A cm-2 at a cell voltage of only 2.15 V for over 1000 h under rigorous working conditions. Experimental and theoretical analyses revealed that the amorphous Ni-Se-Co electron bridges triggered asymmetric d-p-d orbital hybridization via electron-directed transfer, effectively facilitating H2O dissociation and adsorption for *H/*OOH intermediates. The rapid oxidative reconstruction of active Ni-Se-Co sites further improved the intrinsic activity. This work proposes a convenient strategy to fabricate an efficient, durable NiSe2-based catalyst and provides insights into the effects and evolution of amorphous atomic doping during water-splitting process.
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APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
ISSN: 0926-3373
Year: 2025
Volume: 372
2 0 . 3 0 0
JCR@2023
CAS Journal Grade:1
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