具有宽电化学窗口和增强机械强度的复合固态聚合物电解质及其在锂离子电池中的应用

鲍镜羽; 于彩梅; 龚雪; 刘洪煦; 任世杰

doi:10.11777/j.issn1000-3304.2026.25253

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具有宽电化学窗口和增强机械强度的复合固态聚合物电解质及其在锂离子电池中的应用

研究论文 | 更新时间：2026-03-09

- 具有宽电化学窗口和增强机械强度的复合固态聚合物电解质及其在锂离子电池中的应用
- Composite Solid-state Polymer Electrolytes with a Wide Electrochemical Window and Enhanced Mechanical Strength for Lithium-ion Battery Applications
- 高分子学报 2026年页码：1-13
- 作者机构：
  
  1.四川大学高分子科学与工程学院先进高分子材料全国重点实验室成都 610065
  2.天府绛溪实验室成都 641419
- 作者简介：
  
  E-mail: hongxuliu@scu.edu.cn;
  E-mail: rensj@scu.edu.cn
- 基金信息：
  
  国家自然科学基金项目(22375136);先进高分子材料全国重点实验室(sklpme2023-2-08)
- DOI：10.11777/j.issn1000-3304.2026.25253
  中图分类号：
- CSTR：32057.14.GFZXB.2026.7558
- 收稿：2025-11-21，
  
  录用：2026-01-23，
  
  网络首发：2026-03-08，
- 稿件说明：
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鲍镜羽, 于彩梅, 龚雪, 刘洪煦, 任世杰. 具有宽电化学窗口和增强机械强度的复合固态聚合物电解质及其在锂离子电池中的应用. 高分子学报, doi: 10.11777/j.issn1000-3304.2026.25253.

Bao, J. Y., Yu, C. M., Gong, X., Liu, H. X., Ren, S. J. Composite solid-state polymer electrolytes with a wide electrochemical window and enhanced mechanical strength for lithium-ion battery applications. Acta Polymerica Sinica (in Chinese), doi: 10.11777/j.issn1000-3304.2026.25253.
鲍镜羽, 于彩梅, 龚雪, 刘洪煦, 任世杰. 具有宽电化学窗口和增强机械强度的复合固态聚合物电解质及其在锂离子电池中的应用. 高分子学报, doi: 10.11777/j.issn1000-3304.2026.25253. DOI： CSTR： 32057.14.GFZXB.2026.7558.

Bao, J. Y., Yu, C. M., Gong, X., Liu, H. X., Ren, S. J. Composite solid-state polymer electrolytes with a wide electrochemical window and enhanced mechanical strength for lithium-ion battery applications. Acta Polymerica Sinica (in Chinese), doi: 10.11777/j.issn1000-3304.2026.25253. DOI： CSTR： 32057.14.GFZXB.2026.7558.

摘要

基于聚氧化乙烯(PEO)的全固态聚合物电解质与液态电解质相比具有更优异的安全性，成为当前的研究热点. 然而，其较低的离子电导率以及机械强度不足等问题，严重制约了该类材料的实际应用. 针对这一技术瓶颈，本研究采用静电纺丝技术，成功制备了一种新型PEO基含三维复合纤维网络的固态电解质，通过引入超交联聚合物修饰的纳米颗粒，有效构建了稳定、高机械强度的骨架结构，为锂离子传输提供了连续且高效的通道. 实验结果表明，复合电解质PVDF-PEO-SiO

@HCPs-10%展现出卓越的综合性能：具有5.5 V (versus Li/Li⁺)的宽电化学窗口；在40 ℃条件下实现了1.41×10

-4

S·cm

-1

的高离子电导率；机械强度提升至4.01 MPa. 同时基于该电解质组装的LiFePO

//Li电池也表现出优异的电化学性能：LiFePO

/PPH-10%/Li电池在2 C的高倍率充放电条件下，仍能保持147.5 mAh·g

-1

的高比容量，且具备出色的循环稳定性. 本工作突出了超交联纳米颗粒增强纤维电解质在解决基于PEO体系长期存在问题中的有效性. 其设计策略为开发具有更高安全性、更优离子电导率和更强机械性能的新一代固态电解质提供了一条新的路径.

Abstract

Poly(ethylene oxide) (PEO)-based all-solid-state polymer electrolytes have attracted considerable attention as safer alternatives to liquid electrolytes. Nevertheless

their practical applications are severely hindered by the low ionic conductivity and poor mechanical strength. To overcome these limitations

we herein fabricated a novel PEO-based electrolyte with three-dimensional composite fiber-networks

via

electrospinning. By incorporating hypercrosslinked polymer-modified nanoparticles

a mechanically robust framework was established

which simultaneously enhanced structural stability and provided continuous

efficient ion-conduction pathways. As a result

the composite electrolyte

PVDF-PEO-SiO

@HCPs-10%

displayed a wide electrochemical stability window of 5.5 V (versus Li/Li⁺)

a high ionic conductivity of 1.41×10

-4

S·cm

-1

at 40 ℃

and an improved tensile strength of 4.01 MPa. When assembled into LiFePO

//Li cells

the electrolyte enabled excellent electrochemical performance

achieving a high specific capacity of 147.5 mAh·g

-1

at a rate of 2.0 C

along with outstanding cycling stability. This work highlights the effectiveness of hyper-crosslinked nanoparticle-reinforced fiber electrolytes in addressing the long-standing challenges of PEO-based electrolyte systems. The proposed design strategy offers a promising avenue toward the development of next-generation solid-state electro

lytes with superior safety

ionic conductivity

and mechanical robustness.

关键词

Keywords

references

Armand M. ; Tarascon , J. M. Building better batteries . Nature , 2008 , 451 ( 7179 ), 652 - 657 . doi: 10.1038/451652a http://dx.doi.org/10.1038/451652a

Wang Z. Y. ; Guo Q. Y. ; Jiang R. R. ; Deng S. G. ; Ma J. F. ; Cui P. ; Yao X. Y. Porous poly(vinylidene fluoride) supported three-dimensional poly(ethylene glycol) thin solid polymer electrolyte for flexible high temperature all-solid-state lithium metal batteries . Chem. Eng. J. , 2022 , 435 , 135106 . doi: 10.1016/j.cej.2022.135106 http://dx.doi.org/10.1016/j.cej.2022.135106

Guo Q. Y. ; Xu F. L. ; Shen L. ; Deng S. G. ; Wang Z. Y. ; Li M. Q. ; Yao X. Y. 20 μ m-thick Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 -based flexible solid electrolytes for all-solid-state lithium batteries . Energy Mater. Adv. , 2022, 2022 , 2022 / 9753506 . doi: 10.34133/2022/9753506 http://dx.doi.org/10.34133/2022/9753506

Liang H. M. ; Wang L. ; Wang A. P. ; Song Y. Z. ; Wu Y. Z. ; Yang Y. ; He X. M. Tailoring practically accessible polymer/inorganic composite electrolytes for all-solid-state lithium metal batteries: a review . Nanomicro Lett. , 2023 , 15 ( 1 ), 42 . doi: 10.1007/s40820-022-00996-1 http://dx.doi.org/10.1007/s40820-022-00996-1

Watanabe T. ; Inafune Y. ; Tanaka M. ; Mochizuki Y. ; Matsumoto F. ; Kawakami H. Development of all-solid-state battery based on lithium ion conductive polymer nanofiber framework . J. Power Sources , 2019 , 423 , 255 - 262 . doi: 10.1016/j.jpowsour.2019.03.066 http://dx.doi.org/10.1016/j.jpowsour.2019.03.066

Wen J. ; Zhang R. ; Zhao Q. N. ; Liu W. ; Lu G. J. ; Hu X. L. ; Sun J. ; Wang R. H. ; Jiang X. P. ; Hu N. ; Liu J. L. ; Liu X. J. ; Xu C. H. Hydroxyapatite nanowire-reinforced poly(ethylene oxide)-based polymer solid electrolyte for application in high-temperature lithium batteries . ACS Appl. Mater. Interfaces , 2020 , 12 ( 49 ), 54637 - 54643 . doi: 10.1021/acsami.0c15692 http://dx.doi.org/10.1021/acsami.0c15692

Ma C. ; Cheng Y. Q. ; Chen K. ; Li J. C. ; Sumpter B. G. ; Nan C. W. ; More K. L. ; Dudney N. J. ; Chi M. F. Mesoscopic framework enables facile ionic transport in solid electrolytes for Li batteries . Adv. Energy Mater. , 2016 , 6 ( 11 ), 1600053 . doi: 10.1002/aenm.201600053 http://dx.doi.org/10.1002/aenm.201600053

Zhao Y. ; Yan J. H. ; Cai W. P. ; Lai Y. M. ; Song J. ; Yu J. Y. ; Ding B. Elastic and well-aligned ceramic LLZO nanofiber based electrolytes for solid-state lithium batteries . Energy Storage Mater. , 2019 , 23 , 306 - 313 . doi: 10.1016/j.ensm.2019.04.043 http://dx.doi.org/10.1016/j.ensm.2019.04.043

Li C. ; Huang Y. ; Feng X. S. ; Zhang Z. ; Gao H. ; Huang J. X. Silica-assisted cross-linked polymer electrolyte membrane with high electrochemical stability for lithium-ion batteries . J. Colloid Interface Sci. , 2021 , 594 , 1 - 8 . doi: 10.1016/j.jcis.2021.02.128 http://dx.doi.org/10.1016/j.jcis.2021.02.128

Chen D. L. ; Zhu T. ; Zhu M. ; Kang P. B. ; Yuan S. Q. ; Li Y. Y. ; Lan J. L. ; Yang X. P. ; Sui G. In situ constructing ultrathin, robust-flexible polymeric electrolytes with rapid interfacial ion transport in lithium metal batteries . Small Meth. , 2022 , 6 ( 12 ), 2201114 . doi: 10.1002/smtd.202201114 http://dx.doi.org/10.1002/smtd.202201114

Kato Y. ; Hori S. ; Saito T. ; Suzuki K. ; Hirayama M. ; Mitsui A. ; Yonemura M. ; Iba H. ; Kanno R. High-power all-solid-state batteries using sulfide superionic conductors . Nat. Energy , 2016 , 1 ( 4 ), 16030 . doi: 10.1038/nenergy.2016.30 http://dx.doi.org/10.1038/nenergy.2016.30

Wang C. W. ; Fu K. ; Kammampata S. P. ; McOwen D. W. ; Samson A. J. ; Zhang L. ; Hitz G. T. ; Nolan A. M. ; Wachsman E. D. ; Mo Y. F. ; Thangadurai V. ; Hu L. B. Garnet-type solid-state electrolytes: materials, interfaces, and batteries . Chem. Rev. , 2020 , 120 ( 10 ), 4257 - 4300 . doi: 10.1021/acs.chemrev.9b00427 http://dx.doi.org/10.1021/acs.chemrev.9b00427

Zhou B. H. ; Deng T. Z. ; Yang C. L. ; Wang M. X. ; Yan H. ; Yang Z. ; Wang Z. P. ; Xue Z. G. Self-healing and recyclable polymer electrolyte enabled with boronic ester transesterification for stabilizing ion deposition . Adv. Funct. Mater. , 2023 , 33 ( 13 ), 2212005 . doi: 10.1002/adfm.202212005 http://dx.doi.org/10.1002/adfm.202212005

Han J. ; Lee M. J. ; Lee K. ; Lee Y. J. ; Kwon S. H. ; Min J. H. ; Lee E. ; Lee W. ; Lee S. W. ; Kim B. J. Role of bicontinuous structure in elastomeric electrolytes for high-energy solid-state lithium-metal batteries (adv. mater. 1/2023) . Adv. Mater. , 2023 , 35 ( 1 ), 2370002 . doi: 10.1002/adma.202370002 http://dx.doi.org/10.1002/adma.202370002

Zhou Z. K. ; Tao Z. R. ; Chen R. Y. ; Liu Z. ; He Z. H. ; Zhong L. ; Li X. ; Chen G. X. ; Zhang P. Elastomeric electrolyte for high capacity and long-cycle-life solid-state lithium metal battery . Small Methods , 2023 , 7 ( 4 ), e 2201328 . doi: 10.1002/smtd.202201328 http://dx.doi.org/10.1002/smtd.202201328

Zhang W. Y. ; Su Z. ; Yi S. ; Chen H. L. ; Wang M. H. ; Niu B. ; Zhang Y. Y. ; Long D. H. Sandwich structured metal oxide/reduced graphene oxide/metal oxide-based polymer electrolyte enables continuous inorganic-organic interphase for fast lithium-ion transportation . Small , 2023 , 19 ( 19 ), e 2207536 . doi: 10.1002/smll.202207536 http://dx.doi.org/10.1002/smll.202207536

Zhou W. D. ; Wang S. F. ; Li Y. T. ; Xin S. ; Manthiram A. ; Goodenough J. B. Plating a dendrite-free lithium anode with a polymer/ceramic/polymer sandwich electrolyte . J. Am. Chem. Soc. , 2016 , 138 ( 30 ), 9385 - 9388 . doi: 10.1021/jacs.6b05341 http://dx.doi.org/10.1021/jacs.6b05341

Wu M. J. ; Liu D. ; Qu D. Y. ; Xie Z. Z. ; Li J. S. ; Lei J. H. ; Tang H. L. 3D coral-like LLZO/PVDF composite electrolytes with enhanced ionic conductivity and mechanical flexibility for solid-state lithium batteries . ACS Appl. Mater. Interfaces , 2020 , 12 ( 47 ), 52652 - 52659 . doi: 10.1021/acsami.0c15004 http://dx.doi.org/10.1021/acsami.0c15004

Zhang X. ; Liu T. ; Zhang S. F. ; Huang X. ; Xu B. Q. ; Lin Y. H. ; Xu B. ; Li L. L. ; Nan C. W. ; Shen Y. Synergistic coupling between Li 6.75 La 3Zr1.75Ta0.25O12 and poly(vinylidene fluoride) induces high ionic conductivity, strengthmechanical, and thermal stability of solid composite electrolytes. J. Am. Chem. Soc. , 2017 , 139 ( 39 ), 13779 - 13785 . doi: 10.1021/jacs.7b06364 http://dx.doi.org/10.1021/jacs.7b06364

Lin D. C. ; Yuen P. Y. ; Liu Y. Y. ; Liu W. ; Liu N. ; Dauskardt R. H. ; Cui Y. A silica-aerogel-reinforced composite polymer electrolyte with high ionic conductivity and high modulus . Adv. Mater. , 2018 , 30 ( 32 ), e 1802661 . doi: 10.1002/adma.201802661 http://dx.doi.org/10.1002/adma.201802661

Duan H. ; Yin Y. X. ; Shi Y. ; Wang P. F. ; Zhang X. D. ; Yang C. P. ; Shi J. L. ; Wen R. ; Guo Y. G. ; Wan L. J. Dendrite-free Li-metal battery enabled by a thin asymmetric solid electrolyte with engineered layers . J. Am. Chem. Soc. , 2018 , 140 ( 1 ), 82 - 85 . doi: 10.1021/jacs.7b10864 http://dx.doi.org/10.1021/jacs.7b10864

Zhu P. ; Yan C. Y. ; Dirican M. ; Zhu J. D. ; Zang J. ; Selvan R. K. ; Chung C. C. ; Jia H. ; Li Y. ; Kiyak Y. ; Wu N. Q. ; Zhang X. W. Li 0.33 La 0.557 TiO 3 ceramic nanofiber-enhanced polyethylene oxide-based composite polymer electrolytes for all-solid-state lithium batteries . J. Mater. Chem. A , 2018 , 6 ( 10 ), 4279 - 4285 . doi: 10.1039/c7ta10517g http://dx.doi.org/10.1039/c7ta10517g

Yu C. M. ; Gong X. ; Wang M. Y. ; Li L. Y. ; Ren S. J. Hyper-cross-linked nanoparticle reinforced composite polymer electrolytes with enhanced ionic conductivity and thermal stability for lithium-ion batteries . ACS Appl. Polym. Mater. , 2023 , 5 ( 2 ), 1509 - 1519 . doi: 10.1021/acsapm.2c01997 http://dx.doi.org/10.1021/acsapm.2c01997

Liao M. ; Ye L. ; Zhang Y. ; Chen T. Q. ; Peng H. S. The recent advance in fiber-shaped energy storage devices . Adv. Electron. Mater. , 2019 , 5 ( 1 ), 1800456 . doi: 10.1002/aelm.201800456 http://dx.doi.org/10.1002/aelm.201800456

Rodrigues M. F. ; Babu G. ; Gullapalli H. ; Kalaga K. ; Sayed F. N. ; Kato K. ; Joyner J. ; Ajayan P. M. A materials perspective on Li-ion batteries at extreme temperatures . Nat. Energy , 2017 , 2 ( 8 ), 17108 . doi: 10.1038/nenergy.2017.108 http://dx.doi.org/10.1038/nenergy.2017.108

Cao X. Y. ; Cheng J. M. ; Zhang X. B. ; Zhou D. ; Tong Y. F. Composite polymer electrolyte based on liquid crystalline copolymer with high-temperature stability and bendability for all-solid-state lithium-ion batteries . Int. J. Electrochem. Sci. , 2020 , 15 ( 1 ), 677 - 695 . doi: 10.20964/2020.01.32 http://dx.doi.org/10.20964/2020.01.32

Ma Y. X. ; Wan J. Y. ; Yang Y. F. ; Ye Y. S. ; Xiao X. ; Boyle D. T. ; Burke W. ; Huang Z. J. ; Chen H. ; Cui Y. ; Yu Z. A. ; Oyakhire S. T. ; Cui Y. Scalable, ultrathin, and high-temperature-resistant solid polymer electrolytes for energy-dense lithium metal batteries . Adv. Energy Mater. , 2022 , 12 ( 15 ), 2103720 . doi: 10.1002/aenm.202103720 http://dx.doi.org/10.1002/aenm.202103720

Luo S. Q. ; Zhao E. Y. ; Gu Y. X. ; Huang J. ; Zhang Z. X. ; Yang L. ; Hirano S. I. Rational design of fireproof fiber-network reinforced 3D composite solid electrolyte for dendrite-free solid-state batteries . Chem. Eng. J. , 2021 , 421 , 127771 . doi: 10.1016/j.cej.2020.127771 http://dx.doi.org/10.1016/j.cej.2020.127771

Shim J. ; Bae K. Y. ; Kim H. J. ; Lee J. H. ; Kim D. G. ; Yoon W. Y. ; Lee J. C. Solid polymer electrolytes based on functionalized tannic acids from natural resources for all-solid-state lithium-ion batteries . ChemSusChem , 2015 , 8 ( 24 ), 4133 - 4138 . doi: 10.1002/cssc.201501110 http://dx.doi.org/10.1002/cssc.201501110

Thackeray M. M. ; Wolverton C. ; Isaacs E. D. Electrical energy storage for transportation: approaching the limits of, and going beyond, lithium-ion batteries. Energy Environ. Sci ., 2012 , 5 ( 7 ), 7854 - 7863 . doi: 10.1039/c2ee21892e http://dx.doi.org/10.1039/c2ee21892e

Zhang D. C. ; Xu X. J. ; Huang X. Y. ; Shi Z. C. ; Wang Z. S. ; Liu Z. B. ; Hu R. Z. ; Liu J. ; Zhu M. A flexible composite solid electrolyte with a highly stable interphase for dendrite-free and durable all-solid-state lithium metal batteries . J. Mater. Chem. A , 2020 , 8 ( 35 ), 18043 - 18054 . doi: 10.1039/d0ta06697d http://dx.doi.org/10.1039/d0ta06697d

Gao L. ; Li J. X. ; Sarmad B. ; Cheng B. W. ; Kang W. M. ; Deng N. P. A 3D polyacrylonitrile nanofiber and flexible polydimethylsiloxane macromolecule combined all-solid-state composite electrolyte for efficient lithium metal batteries . Nanoscale , 2020 , 12 ( 26 ), 14279 - 14289 . doi: 10.1039/d0nr04244g http://dx.doi.org/10.1039/d0nr04244g

Li D. ; Chen L. ; Wang T. S. ; Fan L. Z. 3D fiber-network-reinforced bicontinuous composite solid electrolyte for dendrite-free lithium metal batteries . ACS Appl. Mater. Interfaces , 2018 , 10 ( 8 ), 7069 - 7078 . doi: 10.1021/acsami.7b18123 http://dx.doi.org/10.1021/acsami.7b18123

Zhang Z. ; YingHuang , Zhang G. Z. ; Chao L. Three-dimensional fiber network reinforced polymer electrolyte for dendrite-free all-solid-state lithium metal batteries . Energy Storage Mater. , 2021 , 41 , 631 - 641 . doi: 10.1016/j.ensm.2021.06.030 http://dx.doi.org/10.1016/j.ensm.2021.06.030

Hu J. K. ; He P. G. ; Zhang B. C. ; Wang B. Y. ; Fan L. Z. Porous film host-derived 3D composite polymer electrolyte for high-voltage solid state lithium batteries . Energy Storage Mater. , 2020 , 26 , 283 - 289 . doi: 10.1016/j.ensm.2020.01.006 http://dx.doi.org/10.1016/j.ensm.2020.01.006

Gao L. ; Li J. X. ; Ju J. G. ; Wang L. Y. ; Yan J. ; Cheng B. W. ; Kang W. M. ; Deng N. P. ; Li Y. T. Designing of root-soil-like polyethylene oxide-based composite electrolyte for dendrite-free and long-cycling all-solid-state lithium metal batteries . Chem. Eng. J. , 2020 , 389 , 124478 . doi: 10.1016/j.cej.2020.124478 http://dx.doi.org/10.1016/j.cej.2020.124478

Huo H. Y. ; Chen Y. ; Luo J. ; Yang X. F. ; Guo X. X. ; Sun X. L. Rational design of hierarchical "ceramic-in-polymer" and "polymer-in-ceramic" electrolytes for dendrite-free solid-state batteries . Adv. Energy Mater. , 2019 , 9 ( 17 ), 1804004 . doi: 10.1002/aenm.201804004 http://dx.doi.org/10.1002/aenm.201804004

Lv F. ; Liu K. X. ; Wang Z. Y. ; Zhu J. F. ; Zhao Y. ; Yuan S. Ultraviolet-cured polyethylene oxide-based composite electrolyte enabling stable cycling of lithium battery at low temperature . J. Colloid Interface Sci. , 2021 , 596 , 257 - 266 . doi: 10.1016/j.jcis.2021.02.095 http://dx.doi.org/10.1016/j.jcis.2021.02.095

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