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Enhancing composite solid electrolyte performance via multiple hydrogen bond networks
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DOI：10.1016/j.jpowsour.2026.241404.png)
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Abstract
En 中文
Solid-state polymer electrolytes (SPEs) are attractive for next-generation energy storage due to their intrinsic safety and potential for high energy density. Nevertheless, their development is hindered by low ambient-temperature ionic conductivity, limited electrochemical stability, and poor thermal resilience. Here, We introduce hydroxyapatite (HAP) and thermoplastic polyurethane (TPU) into a PVDF-HFP matrix to construct multiple hydrogen-bonding networks. In cell assembly, a trace amount of liquid electrolyte was used exclusively to wet the electrode/electrolyte interface and facilitate initial electrochemical evaluation, while the intrinsic properties of the composite membrane (ionic conductivity, mechanical strength, and bulk ion transport) remain governed by the hydrogen-bonding network. Spectroscopic analyses confirm that the polar groups (C=O and ─NH) of TPU, the ─OH groups on HAP, and the ─F groups on PVDF-HFP interact via multiple hydrogen bonds, forming a three-dimensional cross-linked continuous ion transport network. This promotes Li+ dissociation, raising the lithium-ion (Li+) transference number (tLi+) to 0.712, and enhances tensile strength by 145% (from 3.1 to 7.6 MPa) via physical crosslinking. The network induces a thin, uniform, LiF-rich SEI/CEI layer, suppressing side reactions and concentration polarization. Li||PTLH-10||single-crystal NCM83 (SC-NCM83) cells retain 78.79% capacity after 300 cycles at 1 C, deliver 161.8 mAh g−1 at 5 C, and show excellent stability at 4.4 V and 45°C. This strategy not only facilitates Li + transport kinetics but also establishes a stable electrode/electrolyte interface, offering new design insights for high-energy-density, long-cycle-life solid-state lithium-ion batteries.
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