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Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries.

ABSTRACT: Solid polymer electrolytes with large-scale processability and interfacial compatibility are promising candidates for solid-state lithium metal batteries. Among various systems, poly(vinylidene fluoride)-based polymer electrolytes with residual solvent are appealing for room-temperature battery operations. However, their porous structure and limited ionic conductivity hinder practical application. Herein, we propose a phase regulation strategy to disrupt the symmetry of poly(vinylidene fluoride) chains and obtain the dense composite electrolyte through the incorporation of MoSe₂ sheets. The electrolyte with high dielectric constant can optimize the solvation structures to achieve high ionic conductivity and low activation energy. The in-situ reactions between MoSe₂ and Li metal generate Li₂Se fast conductor in solid electrolyte interphase, which improves the Coulombic efficiency and interfacial kinetics. The solid-state Li||Li cells achieve robust cycling at 1 mA cm^-2, and the Li||LiNi_0.8Co_0.1Mn_0.1O₂ full cells show practical performance at high rate (3C), high loading (2.6 mAh cm^-2) and in pouch cell.

SUBMITTER: Wu Q

PROVIDER: S-EPMC10562402 | biostudies-literature | 2023 Oct

REPOSITORIES: biostudies-literature

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Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries.

Wu Qian Q Fang Mandi M Jiao Shizhe S Li Siyuan S Zhang Shichao S Shen Zeyu Z Mao Shulan S Mao Jiale J Zhang Jiahui J Tan Yuanzhong Y Shen Kang K Lv Jiaxing J Hu Wei W He Yi Y Lu Yingying Y

Nature communications 20231009 1

Solid polymer electrolytes with large-scale processability and interfacial compatibility are promising candidates for solid-state lithium metal batteries. Among various systems, poly(vinylidene fluoride)-based polymer electrolytes with residual solvent are appealing for room-temperature battery operations. However, their porous structure and limited ionic conductivity hinder practical application. Herein, we propose a phase regulation strategy to disrupt the symmetry of poly(vinylidene fluoride) ...[more]

PMID: 37813846

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Project description:Safety concerns of traditional liquid electrolytes, especially when paired with lithium (Li) metal anodes, have stimulated research of solid polymer electrolytes (SPEs) to exploit the superior thermal and mechanical properties of polymers. Polyphosphazenes are primarily known for their use as flame retardant materials and have demonstrated high Li-ion conductivity owing to their highly flexible P = N backbone which promotes Li-ion conduction via inter- and intrachain hopping along the polymer backbone. While polyphosphazenes are largely unexplored as SPEs in the literature, a few existing examples showed promising ionic conductivity. By anchoring the anion to the polymer backbone, one may primarily allow the movement of Li ions, alleviating the detrimental effects of polarization that are common in conventional dual-ion conducting SPEs. Anion-anchored SPEs, known as single Li-ion conducting solid polymer electrolytes (SLiC-SPEs), exhibit high Li-ion transference numbers (tLi+), which limits Li dendrite growth, thus further increasing the safety of SPEs. However, previously reported SLiC-SPEs suffer from inadequate ionic conductivity, small electrochemical stability windows (ESWs), and limited cycling stability. Herein, we report three polyphosphazene-based SLiC-SPEs comprising lithiated polyphosphazenes. The SLiC polyphosphazenes were prepared through a facile synthesis route, opening the door for enhanced tunability of polymer properties via facile macromolecular nucleophilic substitution and subsequent lithiation. State-of-the-art characterization techniques, such as differential scanning calorimetry (DSC), electrochemical impedance spectroscopy (EIS), and solid-state nuclear magnetic resonance spectroscopy (ssNMR) were employed to probe the effect of the polymer structure on Li-ion dynamics and other electrochemical properties. Produced SPEs showed thermal stability up to ∼208 °C with ionic conductivities comparable to that of the best-reported SLiC-SPEs that definitively comprise no solvents or plasticizers. Among the three lithiated polyphosphazenes, the SPE containing dilithium poly[bis(trifluoroethylamino)phosphazene] (pTFAP2Li) exhibited the most promising electrochemical characteristics with tLi+ of 0.76 and compatibility with both Li metal anodes and LiFePO4 (LFP) cathodes; through 40 cycles at 100 °C, the PEO-pTFAP2Li blend showed 81.2% capacity utilization and 86.8% capacity retention. This work constitutes one of the first successful demonstrations of the cycling performance of a true all-solid-state Li-metal battery using SLiC polyphosphazene SPEs.

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Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries.

Publications

Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries.

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