Reviving Oxygen Evolution Electrocatalysis of Bulk La-Ni Intermetallics via Gaseous Hydrogen Engineering.

Chen, Ziliang; Yang, Hongyuan; Mebs, Stefan; Dau, Holger; Driess, Matthias; Wang, Zhaowu; Kang, Zhenhui; Menezes, Prashanth W · Adv Mater · 2023

basic_science · Level V

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Abstract

A hydrogen processing strategy is developed to enable bulk LaNi<sub>5</sub> to attain high activity and long-term stability toward the electrocatalytic oxygen evolution reaction (OER). By a combination of in situ Raman and quasi in situ X-ray absorption (XAS) spectra, secondary-electron-excited scanning transmission electron microscopy (STEM) patterns as well as the Rietveld method and density functional theory (DFT) calculations, it is discovered that hydrogen-induced lattice distortion, grain refinement, and particle cracks dictate the effective reconstruction of the LaNi<sub>5</sub> surface into a porous hetero-nanoarchitecture composed of uniformly confined active γ-NiOOH nanocrystals by La(OH)<sub>3</sub> layer in the alkaline OER process. This significantly optimizes the charge transfer, structural integrity, active-site exposure, and adsorption energy toward the reaction intermediates. Benefiting from these merits, the overpotential (322 mV) at 100 mA cm<sup>-2</sup> for the hydrogen-processed OER catalyst deposited on nickel foam is reduced by 104 mV as compared to the original phase. Notably, it exhibits remarkable stability for 10 days at an industrial-grade current density of more than 560 mA cm<sup>-2</sup> in alkaline media.