Low-temperature plasma-assisted pulsed laser deposition of Ni₃N and Ni-Co alloy thin films for alkaline hydrogen evolution in water electrolysis
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更新:2026-10-06 17:30:32 浏览:7次
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摘要
To address the sluggish kinetics of the alkaline hydrogen evolution reaction (HER), the high cost of Pt-based catalysts, and the binder-related limitations of conventional powder electrodes, this work integrates LP-PLD-based fabrication of Ni₃N and Ni-Co alloy thin films as binder-free non-noble-metal electrodes and systematically investigates their structure, morphology, electronic structure, and alkaline HER performance. For Ni₃N films, the N₂ flow rate dominates the phase composition and crystallinity; at 150 sccm, the Ni₃N phase achieves optimal crystallinity with a dense surface. Under optimized conditions (150 sccm N₂, 150 W laser power), the film delivers an overpotential of only 120.4 mV at 10 mA cm⁻² and a Tafel slope of 90.71 mV dec⁻¹ in 1 M KOH, a 53.8% reduction compared with pure Ni foam, and retains 98.8% of its current after 25 h. For Ni-Co alloy films, stepwise alternate deposition enables precise control of the Ni/Co molar ratio, yielding phase-pure, binder-free, elementally homogeneous fcc Ni-Co solid-solution films with strong metallurgical bonding to the substrate. The optimized Ni:Co = 3:1 electrode exhibits an overpotential of 104.3 mV at 10 mA cm⁻², a Tafel slope of 80.7 mV dec⁻¹, and an overpotential increase of less than 7 mV after 50 h of continuous operation. DFT calculations reveal that Ni-Co alloying shifts the d-band center to an optimal position, balances H* adsorption/desorption, and reduces the Volmer water-dissociation barrier from 0.45 eV for pure Ni to 0.17 eV. These results demonstrate that LP-PLD combined with parameter and composition engineering provides a controllable, binder-free, and effective strategy for high-performance, durable, and low-cost non-noble-metal thin-film electrodes for electrochemical water splitting.
关键词
low-temperature plasma-assisted pulsed laser deposition; Ni₃N thin films; Ni-Co alloy films; hydrogen evolution reaction; density functional theory
稿件作者
Liu Sen
Beijing institute of graphical communication
忠伟 刘
北京印刷学院
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