Co(acac)<sub>2</sub>-Mediated Regulation of Li<sub>2</sub>O<sub>2</sub> Gradient Growth in Lithium-Oxygen Batteries.

Zheng, Xingzi; Su, Peiyuan; Xu, Jingshen; Kong, Qingyu; Yue, Jianing; Su, Wenli; Zhang, Jihao; Li, Siao et al. · Nano Lett · 2025

basic_science · Level V

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Abstract

In Li-O<sub>2</sub> batteries, Li<sub>2</sub>O<sub>2</sub> serves as the primary cathodic material but its wide band gap imparts insulating properties. Regulating the composition and morphology of Li<sub>2</sub>O<sub>2</sub> enables the construction of a novel cathodic structure with exceptional electrochemical performance. Herein, we introduce an organic salt containing cobalt ions, cobalt acetylacetonate (Co(acac)<sub>2</sub>), into the cathodic electrolyte. We exploit its cation migration characteristics under an electric field to facilitate the generation and decomposition of Co-doped Li<sub>2</sub>O<sub>2</sub>, achieving gradient control and optimized growth of Li<sub>2</sub>O<sub>2</sub>. Moreover, the Co(acac)<sub>2</sub> molecule stabilizes the properties of LiO<sub><i>x</i></sub> species and mitigates side reaction. In situ UV-vis and XANES spectra reveal direct interactions between Co(acac)<sub>2</sub> and O<sub>2</sub><sup>-</sup>/LiO<sub>2</sub>, highlighting the superior reversibility of Co(acac)<sub>2</sub> enhanced Li-O<sub>2</sub> batteries. Both experimental and theoretical results indicate that this novel Li-O<sub>2</sub> battery system exhibits rapid reaction kinetics, with a reduced overpotential of 520 mV and extended cyclability, surpassing 400 cycles with lower polarization.