Improving dissociation and diffusion of lithium ions is the key to solving the practical application of polymer-based solid-state electrolytes (SSE). Here, a low-cost three-dimensional hydroxyapatite (HAP) nanowire is used in polyethene oxide to obtain an enhanced lithium-ion electrolyte. The oxygen-rich interface of HAP provides an integrated dissociation-diffusion platform for lithium salts. The TFSI- anions tend to coordinate with calcium ions, which makes it easier for lithium ions to escape and stay in a free state. The lateral nucleus in the HAP polyethene electrolyte regulates the diffusion from spherical diffusion into linear planar diffusion, which is confirmed by chronoamperometry curves and in situ observation. The stability of the electrolyte at high voltages is improved by inhibiting the superoxide radicals of polyethene oxide chains, which is demonstrated by nuclear magnetic resonance and electron paramagnetic resonance spectroscopy methods. The initial specific charge capacity of the Li/SPE/LiFePO4 cell with HAP-modified polyethene oxide at 2 C is 148.8 mA h/g, and its initial Coulombic efficiency is 95.17%. After 100 cycles, the specific discharge capacity is 125.5 mA h/g with 99.91% retention per cycle. This oxygen-rich interface strategy would guide the discovery of novel materials for polymer-based SSE.
Keywords: electron paramagnetic resonance; hydroxyapatite; nucleation kinetics; oxygen-rich interface; solid-state electrolytes.