1.四川轻化工大学 材料科学与工程学院 自贡 643000
2.四川大学高分子研究所 先进高分子材料全国重点实验室 成都 610065
E-mail: wjt@suse.edu.cn
jjma@suse.edu.cn
ningchen@scu.edu.cn
收稿:2025-11-17,
录用:2025-12-30,
网络首发:2026-02-09,
纸质出版:2026-04-20
移动端阅览
廖锋, 李怡俊, 吴津田, 马建军, 陈宁. 双重动态键协同构筑高自修复及高离子通导离子凝胶. 高分子学报, 2026, 57(4), 914-926.
Liao, F.; Li, Y. J.; Wu, J. T.; Ma, J. J.; Chen, N. Ionogel with synergistic dual dynamic bonds for high self-healing and ionic conductivity. Acta Polymerica Sinica (in Chinese), 2026, 57(4), 914-926.
廖锋, 李怡俊, 吴津田, 马建军, 陈宁. 双重动态键协同构筑高自修复及高离子通导离子凝胶. 高分子学报, 2026, 57(4), 914-926. DOI: 10.11777/j.issn1000-3304.2025.25292. CSTR: 32057.14.GFZXB.2025.7545.
Liao, F.; Li, Y. J.; Wu, J. T.; Ma, J. J.; Chen, N. Ionogel with synergistic dual dynamic bonds for high self-healing and ionic conductivity. Acta Polymerica Sinica (in Chinese), 2026, 57(4), 914-926. DOI: 10.11777/j.issn1000-3304.2025.25292. CSTR: 32057.14.GFZXB.2025.7545.
离子凝胶因其高安全性和宽电化学窗口,在储能领域展现出广阔的应用前景. 然而,现有离子凝胶往往难以同时兼顾高强度与动态特性,导致力学性能、自修复能力和离子电导率之间难以平衡. 针对这一挑战,本工作设计了一种新型离子凝胶电解质,兼具良好柔性、高机械强度、宽电化学窗口以及快速自修复功能. 该电解质采用双重动态交联机制构建自修复体系:一方面引入咪唑-锌(Im-Zn)金属配位作用,形成动态高强度交联网络;另一方面,利用离子液体(IL)与聚合物链上―CF
3
基团之间产生的离子-偶极(Ion-D)相互作用,调控链段运动能力,从而优化离子传输性能. 基于该结构,离子凝胶实现了高达94%的自修复效率和80 kPa的拉伸强度. 此外,该材料还具备0.36 mS/cm的高离子电导率、0.46的锂离子迁移数以及4.32 V的宽电化学窗口,可全面改善固态
锂电池的性能. 基于该离子凝胶组装的Li/LiFePO
4
全电池在0.5 C倍率下循环500圈后,容量保持率仍高达80%. 本工作揭示了超分子结构设计对离子凝胶中离子传输行为和链段运动特性的调控机制,为高性能储能材料的发展提供了理论支撑.
Ionogels
known for their high safety and wide electrochemical windows
show great potential in energy storage. However
existing ionogels often struggle to balance high strength with dynamic properties
making it difficult to achieve an optimal combination of mechanical performance
self-healing capability
and ionic conductivity. To address this challenge
this study presents a novel ionogel electrolyte that integrates good flexibility
high mechanical strength
a wide electrochemical window
and rapid self-healing functionality. The self-healing system of the electrolyte is constructed through a dual dynamic crosslinking mechanism: on one hand
imidazole-zinc (Im-Z) metal coordination is introduced to form a dynamic high-strength crosslinked network; on the other hand
ion-dipole (Ion-D) interactions between the ionic liquid (IL) and ―CF
3
groups on the polymer chains are utilized to regulate chain segment mobility
thereby optimizing ion transport performance. Owing to this structure
the ionogel achieved a high self-healing efficiency of 94% and a tensile strength of 80 kPa. Moreover
the material e
xhibits a high ionic conductivity of 0.36 mS/cm
lithium-ion transference number of 0.46
and wide electrochemical window of 4.32 V
all of which contribute to the comprehensive improvements in the performance of solid-state lithium batteries. A Li/LiFePO
4
full cell assembled with this ionogel maintained a capacity retention rate as high as 80 % after 500 cycles at 0.5 C. This study elucidates the regulatory mechanism of supramolecular structural design on ion transport behavior and chain segment dynamics in ionogels
providing a theoretical basis for developing high-performance energy storage materials.
Yun Y. S. ; Choi J. A. ; Kim D. W. Lithium polymer batteries assembled with in situ cross-linked gel polymer electrolytes containing ionic liquid . Macromol. Res. , 2013 , 21 ( 1 ), 49 - 54 . doi: 10.1007/s13233-013-1001-1 http://dx.doi.org/10.1007/s13233-013-1001-1
Hyun W. J. ; Thomas C. M. ; Hersam M. C. Nanocomposite ionogel electrolytes for solid-state rechargeable batteries . Adv. Energy Mater. , 2020 , 10 ( 36 ), 2002135 . doi: 10.1002/aenm.202070149 http://dx.doi.org/10.1002/aenm.202070149
Lu Y. Y. ; Korf K. ; Kambe Y. ; Tu Z. Y. ; Archer L. A. Ionic-liquid-nanoparticle hybrid electrolytes: applications in lithium metal batteries . Angew. Chem. Int. Ed. , 2014 , 53 ( 2 ), 488 - 492 . doi: 10.1002/anie.201307137 http://dx.doi.org/10.1002/anie.201307137
Osada I. ; De Vries H. ; Scrosati B. ; Passerini S. Ionic-liquid-based polymer electrolytes for battery applications . Angew. Chem. Int. Ed. , 2016 , 55 ( 2 ), 500 - 513 . doi: 10.1002/anie.201504971 http://dx.doi.org/10.1002/anie.201504971
Yang X. F. ; Liu G. Q. ; Peng L. ; Guo J. H. ; Tao L. ; Yuan J. Y. ; Chang C. Y. ; Wei Y. ; Zhang L. N. Highly efficient self-healable and dual responsive cellulose-based hydrogels for controlled release and 3D cell culture . Adv. Funct. Mater. , 2017 , 27 ( 40 ), 1703174 . doi: 10.1002/adfm.201703174 http://dx.doi.org/10.1002/adfm.201703174
Armand M. ; Endres F. ; MacFarlane D. R. ; Ohno H. ; Scrosati B. Ionic-liquid materials for the electrochemical challenges of the future . Nat. Mater. , 2009 , 8 ( 8 ), 621 - 629 . doi: 10.1038/nmat2448 http://dx.doi.org/10.1038/nmat2448
Dubal D. P. ; Chodankar N. R. ; Kim D. H. ; Gomez-Romero P. Towards flexible solid-state supercapacitors for smart and wearable electronics . Chem. Soc. Rev. , 2018 , 47 ( 6 ), 2065 - 2129 . doi: 10.1039/c7cs00505a http://dx.doi.org/10.1039/c7cs00505a
Li J. ; Qiao J. L. ; Lian K. Hydroxide ion conducting polymer electrolytes and their applications in solid supercapacitors: a review . Energy Storage Mater. , 2020 , 24 , 6 - 21 . doi: 10.1016/j.ensm.2019.08.012 http://dx.doi.org/10.1016/j.ensm.2019.08.012
Guo P. L. ; Su A. Y. ; Wei Y. J. ; Liu X. K. ; Li Y. ; Guo F. F. ; Li J. ; Hu Z. Y. ; Sun J. Q. Healable, highly conductive, flexible, and nonflammable supramolecular ionogel electrolytes for lithium-ion batteries . ACS Appl. Mater. Interfaces , 2019 , 11 ( 21 ), 19413 - 19420 . doi: 10.1021/acsami.9b02182 http://dx.doi.org/10.1021/acsami.9b02182
Sun Y. X. ; Gao L. J. ; Xie H. M. ; Liu J. Self-healing poly(ionic liquid) gel polymer electrolytes for high-performance lithium metal batteries enabled by ion-dipole interactions . J. Power Sources , 2025 , 649 , 237465 . doi: 10.1016/j.jpowsour.2025.237465 http://dx.doi.org/10.1016/j.jpowsour.2025.237465
Deng W. N. ; Liu W. M. ; Zhu H. ; Chen L. ; Liao H. Y. ; Chen H. Click-chemistry and ionic cross-linking induced double cross-linking ionogel electrolyte for flexible lithium-ion batteries . J. Energy Storage , 2023 , 72 , 108509 . doi: 10.1016/j.est.2023.108509 http://dx.doi.org/10.1016/j.est.2023.108509
Yu Z. C. ; Wu P. Y. Underwater communication and optical camouflage ionogels . Adv. Mater. , 2021 , 33 ( 24 ), 2008479 . doi: 10.1002/adma.202008479 http://dx.doi.org/10.1002/adma.202008479
Li R. J. ; Fang Z. ; Wang C. ; Zhu X. L. ; Fu X. L. ; Fu J. J. ; Yan W. W. ; Yang Y. Six-armed and dicationic polymeric ionic liquid for highly stretchable, nonflammable and notch-insensitive intrinsic self-healing solid-state polymer electrolyte for flexible and safe lithium batteries . Chem. Eng. J. , 2022 , 430 , 132706 . doi: 10.1016/j.cej.2021.132706 http://dx.doi.org/10.1016/j.cej.2021.132706
Kidambi S. S. ; Lee D. K. ; Ramamoorthy A. Interaction of Cd and Zn with biologically important ligands characterized using solid-state NMR and ab initio calculations . Inorg. Chem. , 2003 , 42 ( 9 ), 3142 - 3151 . doi: 10.1021/ic026287d http://dx.doi.org/10.1021/ic026287d
Cho S. ; Lee H. ; Je S. ; Lee J. ; Bae S. ; Kim T. A. ; Lee J. Enhancing shock wave energy dissipation in metallosupramolecular polymer by tuning metal-imidazole coordination interactions . Polym. Test. , 2025 , 150 , 108885 . doi: 10.1016/j.polymertesting.2025.108885 http://dx.doi.org/10.1016/j.polymertesting.2025.108885
Qiu W. L. ; Chen G. Q. ; Zhu H. ; Zhang Q. ; Zhu S. P. Enhanced stretchability and robustness towards flexible ionotronics via double-network structure and ion-dipole interactions . Chem. Eng. J. , 2022 , 434 , 134752 . doi: 10.1016/j.cej.2022.134752 http://dx.doi.org/10.1016/j.cej.2022.134752
Jiang Y. ; Zhao S. Q. ; Xiao X. Y. ; Pi J. Q. ; Wang Y. L. ; Yi N. ; Zou L. J. ; Xu Z. X. ; Xiao Y. H. ; Ao X. ; Ding G. N. ; Zhou W. H. ; Zhou N. G. ; Xue Z. G. Poly(benzoxazine)-based gel polymer electrolytes for lithium metal batteries with ultralong lifespans . Angew. Chem. Int. Ed. , 2025 , 64 ( 42 ), e 202510997 . doi: 10.1002/anie.202510997 http://dx.doi.org/10.1002/anie.202510997
Li Y. W. ; Xu S. K. ; Zhang Y. Y. ; Du R. ; Li R. ; Xing Y. J. Rich active sites ZIF-8 base on imidazole-based deep eutectic solvents for rapid adsorption of acid fuchsin and competitive adsorption . Microporous Mesoporous Mater. , 2025 , 381 , 113351 . doi: 10.1016/j.micromeso.2024.113351 http://dx.doi.org/10.1016/j.micromeso.2024.113351
Gao L. J. ; Jiang W. B. ; Zhang X. R. ; Sun Y. X. ; Chen K. ; Li W. L. ; Xie H. M. ; Liu J. A self-healing poly(ionic liquid) block copolymer electrolyte enabled by synergetic dual ion-dipole interactions . Chem. Eng. J. , 2024 , 479 , 147822 . doi: 10.1016/j.cej.2023.147822 http://dx.doi.org/10.1016/j.cej.2023.147822
Guo Y. B. ; Zhang M. ; Ge Z. ; Fang Z. X. ; Xu Z. Q. ; Wu J. T. ; Wu M. Q. Electrostatic force-tailored PEO-based solid electrolyte with fast Li + transport for ultra-robust lithium metal batteries . Adv. Funct. Mater. , 2025 , 35 ( 23 ), 2419998 . doi: 10.1002/adfm.202419998 http://dx.doi.org/10.1002/adfm.202419998
陈心怡 , 李瑀 , 封伟 . 基于两性离子的自修复准固态聚合物电解质 . 高分子学报 , 2022 , 53 ( 11 ), 1349 - 1357 . doi: 10.11777/j.issn1000-3304.2022.22091 http://dx.doi.org/10.11777/j.issn1000-3304.2022.22091
巫文强 . 可逆交联功能含氟弹性体的制备与研究 . 四川大学博士学位论文 , 2023 .
Whba R. ; Su'ait M. S. ; TianKhoon L. ; Ibrahim S. ; Mohamed N. S. ; Ahmad A. In-situ UV cured acrylonitrile grafted epoxidized natural rubber (ACN-g-ENR)-LiTFSI solid polymer electrolytes for lithium-ion rechargeable batteries . React. Funct. Polym. , 2021 , 164 , 104938 . doi: 10.1016/j.reactfunctpolym.2021.104938 http://dx.doi.org/10.1016/j.reactfunctpolym.2021.104938
Li F. D. ; Nguyen G. T. M. ; Vancaeyzeele C. ; Vidal F. ; Plesse C. Photopolymerizable ionogel with healable properties based on dioxaborolane vitrimer chemistry . Gels , 2022 , 8 ( 6 ), 381 . doi: 10.3390/gels8060381 http://dx.doi.org/10.3390/gels8060381
Wang Z. Y. ; Wang Y. M. ; Zhai P. ; Poldorn P. ; Jungsuttiwong S. ; Yuan S. A cation-dipole-reinforced elastic polymer electrolyte enabling long-cycling quasi-solid-state lithium metal batteries . J. Energy Chem. , 2022 , 75 , 340 - 348 . doi: 10.1016/j.jechem.2022.08.042 http://dx.doi.org/10.1016/j.jechem.2022.08.042
Wang C. ; Li R. J. ; Chen P. ; Fu Y. S. ; Ma X. Y. ; Shen T. ; Zhou B. J. ; Chen K. ; Fu J. J. ; Bao X. F. ; Yan W. W. ; Yang Y. Highly stretchable, non-flammable and notch-insensitive intrinsic self-healing solid-state polymer electrolyte for stable and safe flexible lithium batteries . J. Mater. Chem. A , 2021 , 9 ( 8 ), 4758 - 4769 . doi: 10.1039/d0ta10745j http://dx.doi.org/10.1039/d0ta10745j
赵姣 , 孙少妮 , 姜春胜 , 孙丽丽 , 曹学飞 . 具有多刺激响应行为和自修复能力的纤维素纳米晶增强聚乙烯醇水凝胶 . 北京林业大学学报 , 2025 . 47 ( 6 ), 152 - 161 . doi: 10.12171/j.1000-1522.20250104 http://dx.doi.org/10.12171/j.1000-1522.20250104
Cai Y. C. ; Hou Y. P. ; Lu Y. ; Zhang Q. ; Yan Z. H. ; Chen J. Ionic liquid electrolyte with weak solvating molecule regulation for stable Li deposition in high-performance Li-O 2 batteries . Angew. Chem. Int. Ed. , 2023 , 62 ( 17 ), e 202218014 . doi: 10.1002/anie.202218014 http://dx.doi.org/10.1002/anie.202218014
Weng C. C. ; Ma L. ; Wang B. F. ; Meng F. Y. ; Yang J. Q. ; Ji Y. Y. ; Liu B. T. ; Mai W. J. ; Huang S. M. ; Pan L. K. ; Li J. L. Single-solvent ionic liquid strategy achieving wide-temperature and ultra-high cut-off voltage for lithium metal batteries . Energy Storage Mater. , 2024 , 71 , 103584 . doi: 10.1016/j.ensm.2024.103584 http://dx.doi.org/10.1016/j.ensm.2024.103584
Liu X. ; Zarrabeitia M. ; Mariani A. ; Gao X. P. ; Schütz H. M. ; Fang S. ; Bizien T. ; Elia G. A. ; Passerini S. Enhanced Li + transport in ionic liquid-based electrolytes aided by fluorinated ethers for highly efficient lithium metal batteries with improved rate capability . Small Meth. , 2021 , 5 ( 7 ), 2100168 . doi: 10.1002/smtd.202100168 http://dx.doi.org/10.1002/smtd.202100168
Zhu S. D. ; Chen J. Dual strategy with Li-ion solvation and solid electrolyte interphase for high Coulombic efficiency of lithium metal anode . Energy Storage Mater. , 2022 , 44 , 48 - 56 . doi: 10.1016/j.ensm.2021.10.007 http://dx.doi.org/10.1016/j.ensm.2021.10.007
Zhang W. N. ; Yang T. ; Liao X. B. ; Song Y. ; Zhao Y. All-fluorinated electrolyte directly tuned Li+ solvation sheath enabling high-quality passivated interfaces for robust Li metal battery under high voltage operation . Energy Storage Mater. , 2023 , 57 , 249 - 259 . doi: 10.1016/j.ensm.2023.02.027 http://dx.doi.org/10.1016/j.ensm.2023.02.027
Tian R. Z. ; Yin S. ; Wang Z. Y. ; Liu K. ; Zhang L. Q. ; Zhu L. Y. Improved interfacial contact and electrochemical performance of highly Ni-rich LiNi x CoyMn 1-x-yO2 (x > 90%) cathode in all-solid-state lithium battery. Energy Storage Mater. , 2024 , 68 , 103350 . doi: 10.1016/j.ensm.2024.103350 http://dx.doi.org/10.1016/j.ensm.2024.103350
Li T. ; Hu A. J. ; Li Y. J. ; Yang B. R. ; Li K. ; Chen K. ; Jiang J. Y. ; Li F. ; Seh Z. W. ; Wang J. ; Long J. P. Multifunctional polyfluoride ionogel-encapsulated lithium anodes for durable and safe pouch cells under harsh conditions . Adv. Funct. Mater. , 2025 , 35 ( 45 ), 2507310 . doi: 10.1002/adfm.202507310 http://dx.doi.org/10.1002/adfm.202507310
D'Angelo A. J. ; Panzer M. J. Design of stretchable and self-healing gel electrolytes via fully zwitteri onic polymer networks in solvate ionic liquids for Li-based batteries . Chem. Mater. , 2019 , 31 ( 8 ), 2913 - 2922 . doi: 10.1021/acs.chemmater.9b00172 http://dx.doi.org/10.1021/acs.chemmater.9b00172
0
浏览量
275
下载量
0
CSCD
关联资源
相关文章
相关作者
相关机构

京公网安备11010802046899号