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Carbonate-modified CoFe-doped Ni2P@Ni12P5 core-shell heterostructure for ultrastable seawater oxygen evolution
Xingrong Zhang, Wenquan Zhang, Yanru Geng, Xien Liu*, Liqiang Hou*
https://doi.org/10.1016/j.cjsc.2026.101127
Seawater electrolysis; Oxygen evolution reaction; Nickel phosphide; Core-shell structure; Carbonate modification
ABSTRACT
Transition metal phosphides are intrinsically active for the oxygen evolution reaction (OER) yet suffer from severe and irreversible oxidation into oxides/hydroxides in seawater, leading to active-metal dissolution and structural collapse. Herein, we construct a carbonate-modified CoFe co-doped Ni2P@Ni12P5 core–shell heterostructure (CoFe-Ni2P@Ni12P5-Ci) that robustly preserves the parent phosphide phase under seawater oxidation. Co/Fe doping induces a lattice-matched Ni2P@Ni12P5 interface for efficient electron transport, while the surface-anchored carbonate layer plays a dual role: its strong negative charge electrostatically repels Cl- to suppress chlorine evolution, while simultaneously acting as a passivation barrier that delays lattice-oxygen penetration and metal leaching, thereby significantly inhibiting oxidative phase transformation. Operando Raman spectroscopy reveals that NiOOH formation is delayed to 1.6 V for CoFe-Ni2P@Ni12P5-Ci, compared to 1.3 V and 1.1 V for the unmodified and undoped controls, respectively. The catalyst requires an overpotential of only 352 mV at 1000 mA cm-2 in simulated seawater and delivers remarkable durability exceeding 1800 h at an industrial-level current density of 1 A cm-2, while preserving the bulk phosphide structure and significantly suppressing surface reconstruction.
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CN 35–1112/TQ, ISSN 0254–5861, Online ISSN: 2949-768X Copyright @ 2022 Chinese Journal of Structural Chemistry-www.Chinese Journal of Structural Chemistry.net. All Rights Reserved 闽ICP备2022002645号-1