Dual-Channel Regulation of Spin Polarization Achieves 1 + 1 > 2 Electrocatalytic Performance in Spinel Ferrites.

Zhu, Jinli; Peng, Xuebing; Xi, Pinxian; Jia, Chenglong; Gao, Daqiang · Nano Lett · 2025

basic_science · Level V

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Abstract

Electron spin polarization enhances the kinetics of the oxygen evolution reaction (OER), a rate-limiting step that restricts the energy efficiency of water splitting. Here, a dual-channel spin-regulated strategy combining chiral-induced spin selectivity (CISS) and external magnetic field (<i>M</i><sub><i>H</i></sub>)-induced spin polarization synergistically reduces the overpotential and enhances durability in spinel-based ferromagnetic materials. Chiral molecule-modified CoFe<sub>2</sub>O<sub>4</sub> under <i>M</i><sub><i>H</i></sub> (CFO-L-M) achieves a 90 mV reduction in overpotential compared to unmodified CFO, which is primarily ascribed to the synergistic "1 + 1 > 2" effect arising from the dual-spin channel mechanism. Theoretical calculations show that surface spin states critically influence adsorbate binding, with spin selectivity and polarization being activated during the first electron transfer step, ultimately producing triplet O<sub>2</sub>. This study elucidates spin-related OER kinetics, offering a foundation for designing advanced spin-dependent electrocatalysts.