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锂金属电池聚合物基复合固态电解质多尺度协同性能提升研究

作者：张振益，郭晶莹，张毅，陈琳，夏磊，董鹏程，王建川，魏子栋

单位：重庆大学化学化工学院特种化学电源全国重点实验室，重庆 400044

关键词：锂金属电池；聚合物电解质；静电纺丝；原位聚合

DOI号： 10.16159/j.cnki.issn1007-8924.2026.02.014

分类号： TQ028； TM911； O63

出版年,卷(期):页码： 2026,46(2):131-142

摘要：

聚合物电解质具有良好的机械性能和加工特性，有望助力实现锂金属电池的商业化应用，但其室温离子电导率普遍偏低，难以满足电池室温运行需求。本研究提出一种多尺度结构设计策略，成功构建了一种“刚柔并济”的聚合物基复合电解质。该电解质以静电纺丝制备的聚合物/陶瓷复合纤维毡作为刚性骨架，通过原位聚合形成含氟交联聚合物网络，并与固态增塑剂及微量界面改性剂复合。该设计协同增强了电解质的机械性能、离子传导能力和电极/电解质界面稳定性。电化学测试表明，基于该电解质组装的电池表现出优异的循环稳定性和高容量保持率。本工作为发展高安全性、高能量密度锂金属电池的电解质体系提供了新思路。

Polymer electrolytes hold great promise for enabling the commercialization of lithium metal batteries due to their favorable mechanical properties and processability. However, their generally low room-temperature ionic conductivity remains a critical challenge for practical operation. This study proposed a multiscale structural design strategy to construct a polymer-based composite solid-state electrolyte with rigidity-flexibility dual features. The electrolyte incorporated an electrospun polymer/ceramic composite fiber mat as a rigid framework, within which a fluorinated cross-linked polymer network was formed via in situ polymerization. This polymer matrix was further integrated with solid-state plasticizers and a trace amount of interfacial modifier. This design synergistically enhanced the mechanical properties, ionic conductivity, and electrode/electrolyte interfacial stability of the electrolyte. Electrochemical tests demonstrated that cells assembled with this electrolyte exhibited exceptional cycling stability and high capacity retention. This work provides a new pathway for developing electrolyte systems toward high-safety, high-energy-density lithium metal batteries.

基金项目：

国家自然科学基金（22478043, 22478044）

作者简介：

张振益(2001-)，男，江西鹰潭人，博士研究生,主要研究方向为锂金属电池聚合物基固态电解质；郭晶莹(1997-)，女，四川渠县人，硕士,主要研究方向为锂金属电池聚合物基固态电解质

参考文献：

[1]Park H, Tamwattana O, Kim J, et al. Probing lithium metals in batteries by advanced characterization and analysis tools[J]. Adv Energy Mater, 2020, 11(15): 2003039.
[2]Yang C, Jiang Z, Chen X, et al. Lithium metal based battery systems with ultra-high energy density beyond 500 W·h/kg[J]. Chem Commun, 2024, 60(75): 10245-10264.
[3]Shin H R, Yun J, Lee J W. Mechanistic insight into Li-host interactions in carbon hosts for reversible Li metal storage[J]. ECSMA, 2022, 01(2): 271.
[4]Wu X, Jie X, Liang X, et al. Polymer/ceramic gel electrolyte with in-situ interface forming enhances the performance of lithium metal batteries[J]. J Energy Storage, 2024, 78: 110107.
[5]Song Y, Su M, Xiang H, et al. PEO-based solid-state polymer electrolytes for wide-temperature solid-state lithium metal batteries[J]. Small, 2024, 21(3): e2408045.
[6]Gao S S, Wang W S, Xing H R, et al. Electrospun PEO/PVDF blend solid polymer electrolytes with improved electrochemical performances for lithium metal batteries[J]. J Mater Sci, 2025, 60(10): 1-17.
[7]Watanabe M, Kanba M, Nagaoka K, et al. Ionic conductivity of hybrid films based on polyacrylonitrile and their battery application[J]. J Appl Polym Sci, 1982, 27(11): 4191-4198.
[8]Fang X G, Wang X B, Yuan S D, et al. Designing “polymer-in-salt” electrolyte based on PAN LiTFSI with carbon nanotubes as a filler for lithium metal battery[J]. Mater Res Bull, 2025, 188: 113400.
[9]Yang W, Liu Y, Sun X, et al. Solvation-tailored PVDF-based solid-state electrolyte for high voltage lithium metal batteries[J]. Angew Chem Int Ed, 2024, 136(18): e202401428.
[10]Guo Y B, Zhang M, Ge Z, et al. Electrostatic force-tailored PEO-based solid electrolyte with fast Li+ transport for ultra-robust lithium metal batteries[J]. Adv Funct Mater, 2025: 2419998.
[11]Zhao Y, Da X, Qin Y, et al. Nonflammable PVDF-based gel polymer electrolytes modified by dimethyl methylphosphate for wide temperature range, long cycle-life and high-safety lithium metal batteries[J]. Sci China Mater, 2024, 67(12): 3994-4004.
[12]Xian C, Zhang S, Liu P, et al. An advanced gel polymer electrolyte for solid-state lithium metal batteries[J]. Small, 2024, 20(15): 2306381.
[13]Peng H, Long T, Peng J, et al. Molecular design for in-situ polymerized solid polymer electrolytes enabling stable cycling of lithium metal batteries[J]. Adv Energy Mater, 2024, 14(22): 2400428.
[14]Kim E, Jamal H, Jeon I, et al. Functionality of 1-butyl-2,3-dimethylimidazolium bromide (BMI-Br) as a solid plasticizer in PEO-based polymer electrolyte for highly reliable lithium metal batteries[J]. Adv Energy Mater, 2023, 13(47): 2301674.
[15]Zhu T, Liu G, Chen D, et al. Constructing flame-retardant gel polymer electrolytes via multiscale free radical annihilating agents for Ni-rich lithium batteries[J]. Energy Storage Mater, 2022, 50: 495-504.
[16]Wen K, Tan X, Chen T, et al. Fast Li-ion transport and uniform Li-ion flux enabled by a double layered polymer electrolyte for high performance Li metal battery[J]. Energy Storage Mater, 2020, 32: 55-64.
[17]Gopalan A I, Santhosh P, Manesh K M, et al. Development of electrospun PVDF-PAN membrane-based polymer electrolytes for lithium batteries[J]. J Membr Sci, 2008, 325(2): 683-690.
[18]Wang H, Song J, Zhang K, et al. A strongly complexed solid polymer electrolyte enables a stable solid state high-voltage lithium metal battery[J]. Energy Environ Sci, 2022, 15(12): 5149-5158.
[19]Luo D, Zheng L, Zhang Z, et al. Constructing multi-functional solid electrolyte interface via in situ polymerization for dendrite-free and low N/P ratio lithium metal batteries[J]. Nat Commun, 2021, 12(1): 186.
[20]Li Z, Zhou X Y, Guo X. High-performance lithium metal batteries with ultraconformal interfacial contacts of quasi-solid electrolyte to electrodes[J]. Energy Storage Mater, 2020, 29: 149-155.
[21]Steinruck H G, Cao C, Lukatskaya M R, et al. Interfacial speciation determines interfacial chemistry: X-ray-induced lithium fluoride formation from water-in-salt electrolytes on solid surfaces[J]. Angew Chem Int Ed, 2020, 59(51): 23180-23187.
[22]Yamada Y, Usui K, Sodeyama K, et al. Hydrate-melt electrolytes for high-energy-density aqueous batteries[J]. Nat Energy, 2016, 1(10): 16129.

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