Composition regulation of polyacrylonitrile-based polymer electrolytes enabling dual-interfacially stable solid-state lithium batteries

Liu, Xiaoning; Bi, Zhijie; Wan, Yong; Guo, Xiangxin

doi:10.1016/j.jcis.2024.03.166

Journal of Colloid and Interface Science

2024

DOI: 10.1016/j.jcis.2024.03.166

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Composition regulation of polyacrylonitrile-based polymer electrolytes enabling dual-interfacially stable solid-state lithium batteries

Xiaoning Liu,

Zhijie Bi,

Yong Wan

et al.

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Cited by 5 publications

References 69 publications

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Liberating Lithium Ions from Polymer Matrix via Harnessing Ion‐Dipole Interaction Toward Stable Solid‐State Lithium Metal Batteries

Zhang,

Luo,

et al. 2024

Adv Funct Materials

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Although polymer electrolytes have shown great potential in solid‐state lithium metal batteries (LMBs), the polymer chain segments anchor the movement of lithium ions (Li+), which induces the low ionic conductivity of the electrolytes and limits their application. Herein, a strategy of harnessing ion‐dipole interactions is proposed to liberate lithium ions from polymer chains. The adiponitrile (ADN) molecular dipole with strong bond dipole moment (C≡N, 11.8 × 10−30 C m) is introduced into the polyvinylidene fluoride‐co‐hexafluoropropylene (PVDF‐HFP) polymer matrix, achieving an electrolyte with high ionic conductivity of 5.1 × 10−4 S cm−1 at 30 °C. It is demonstrated that the strong ion‐dipole interaction between C≡N and Li+ weakens the ion‐dipole interaction of F···…Li+, facilitating Li+ dissociation and liberating Li+ from polymer chains. Moreover, a hybrid and unsaturated solvation structure is formed with the ADN molecular dipole, PVDF‐HFP polymer chain, and TFSI− anion, corresponding to the solvent‐separated ion pair (SSIP) solvation structure. Thus, the obtained electrolyte realizes high ionic conductivity and lithium‐ion transference number (0.74). Consequently, the assembled lithium symmetric cell delivers stable Li stripping/plating reversibility over 900 h. Additionally, the Li|LiFePO4 full cells exhibit long‐term cycling stability at 0.5 C over 300 cycles with a capacity retention of 96.4% and ultralong cycling of 1000 cycles at a high rate (5 C).

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Liberating Lithium Ions from Polymer Matrix via Harnessing Ion‐Dipole Interaction Toward Stable Solid‐State Lithium Metal Batteries

Zhang,

Luo,

et al. 2024

Adv Funct Materials

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Modification engineering of “polymer‐in‐salt” electrolytes toward high‐stability solid‐state lithium batteries

Chang,

Liu,

Jia

et al. 2024

EcoEnergy

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Solid‐state lithium batteries have been regarded as a promising candidate to become the power supply for electric vehicles and smart grids due to their high energy density and reliable safety. The solid polymer electrolytes (SPEs) with light and thin features show distinctive potential in boosting the available energy density at battery level, whereas their ionic conductivity smaller than 10−4∼10−5 S cm−1 at room temperature constrains the ionic transfer kinetics, leading to low power density and short cycling life. To overcome such problem, the increase of lithium‐salt concentration over 50 wt% evokes the conversion from “salt‐in‐polymer” to “polymer‐in‐salt” (PIS) of SPEs, which can make additional ionic migration pathway and thus the improved ionic conductivity. However, the abundant lithium‐salt may also cause the reduced electrochemical window as well as mechanical properties, which restricts the compatibility with high‐voltage cathodes and lowers the operation safety. In this review, the structures and characteristics of PIS electrolytes have been elucidated through clarifying the correlation between lithium‐salt and polymer matrix. Then, the recent modification engineering progresses on PIS electrolytes are addressed from the aspects of component regulations including polymer matrices, lithium salts and fillers, novel preparation techniques, and extended application scenarios. The crucial challenges and possible research directions are finally proposed for the PIS electrolytes regarding both science and practical perspectives.

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Improving diffusion kinetics of zinc ions/stabilizing zinc anode by molecular slip mechanism and anchoring effect in supramolecular zwitterionic hydrogels

Liu,

Zhang,

Peng

et al. 2025

Journal of Colloid and Interface Science

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Composition regulation of polyacrylonitrile-based polymer electrolytes enabling dual-interfacially stable solid-state lithium batteries

Cited by 5 publications

References 69 publications

Liberating Lithium Ions from Polymer Matrix via Harnessing Ion‐Dipole Interaction Toward Stable Solid‐State Lithium Metal Batteries

Liberating Lithium Ions from Polymer Matrix via Harnessing Ion‐Dipole Interaction Toward Stable Solid‐State Lithium Metal Batteries

Modification engineering of “polymer‐in‐salt” electrolytes toward high‐stability solid‐state lithium batteries

Improving diffusion kinetics of zinc ions/stabilizing zinc anode by molecular slip mechanism and anchoring effect in supramolecular zwitterionic hydrogels

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