Highly Transparent, Adhesive, and Mechanically Robust Eutectogel <italic style="font-style: italic">via</italic> Metal-coordination Physical Crosslinking for Reliable Flexible Strain Sensors

Jian-Ping Peng; Jia-Huan Xie; Zi-Yi Dai; Tong-Gen Li; Tong-Ling Liu; Wei-Hao Wang; Shi-Yu Zhang; Zhen-Kai Huang

doi:10.1007/s10118-025-3406-7

Your Location：

Home >

Browse articles >

Highly Transparent, Adhesive, and Mechanically Robust Eutectogel via Metal-coordination Physical Crosslinking for Reliable Flexible Strain Sensors

RESEARCH ARTICLE | Updated：2025-09-26

- Highly Transparent, Adhesive, and Mechanically Robust Eutectogel via Metal-coordination Physical Crosslinking for Reliable Flexible Strain Sensors
- Chinese Journal of Polymer Science Vol. 43, Issue 10, Pages: 1894-1903(2025)
- Affiliations：
  
  a.School of Environment and Chemical Engineering, Foshan University, Foshan 528000, China
  b.School of Materials and Energy, Foshan University, Foshan 528000, China
- Author bio：
  
  hzk@fosu.edu.cn
- Funds：
- DOI：10.1007/s10118-025-3406-7
  CLC： [M
- Received：16 May 2025，
  
  Revised：2025-06-25，
  
  Accepted：27 June 2025，
  
  Published Online：10 September 2025，
  
  Published：05 October 2025
- Accepted：
Scan QR Code
Peng, J. P.; Xie, J. H.; Dai, Z. Y.; Li, T. G.; Liu, T. L.; Wang, W. H.; Zhang, S. Y.; Huang, Z. K. Highly transparent, adhesive, and mechanically robust eutectogel via metal-coordination physical crosslinking for reliable flexible strain sensors. Chinese J. Polym. Sci. 2025, 43, 1894–1903

Jian-Ping Peng, Jia-Huan Xie, Zi-Yi Dai, et al. Highly Transparent, Adhesive, and Mechanically Robust Eutectogel via Metal-coordination Physical Crosslinking for Reliable Flexible Strain Sensors[J]. Chinese journal of polymer science, 2025, 43(10): 1894-1903.
Peng, J. P.; Xie, J. H.; Dai, Z. Y.; Li, T. G.; Liu, T. L.; Wang, W. H.; Zhang, S. Y.; Huang, Z. K. Highly transparent, adhesive, and mechanically robust eutectogel via metal-coordination physical crosslinking for reliable flexible strain sensors. Chinese J. Polym. Sci. 2025, 43, 1894–1903 DOI： 10.1007/s10118-025-3406-7.

Jian-Ping Peng, Jia-Huan Xie, Zi-Yi Dai, et al. Highly Transparent, Adhesive, and Mechanically Robust Eutectogel via Metal-coordination Physical Crosslinking for Reliable Flexible Strain Sensors[J]. Chinese journal of polymer science, 2025, 43(10): 1894-1903. DOI： 10.1007/s10118-025-3406-7.

摘要

A green eutectogel exhibiting high transparency

mechanical strength

stretchability

ionic conductivity

leakage-resistance

interfacial adhesion

and cryogenic tolerance has been developed. A flexible sensor based on the eutectogel demonstrates ideal linear sensitivity

a broad response range

reliable stability

and quick responsiveness

enabling precise monitoring of human motion and information transmission.

Abstract

Eutectogels are considered to have immense application potential in the field of flexible wearable ionotronic devices because of their excellent ionic conductivity

thermal and electrochemical stability

and non-volatility. However

most existing technologies still struggle to achieve synergistic optimization of key performance indicators

such as high mechanical strength and ionic conductivity. To address this challenge

this study successfully prepared a green eutectogel material with outstanding comprehensive properties by leveraging the high solubility of glycerol in a polymerizable deep eutectic solvent (DES) composed of acrylic acid and choline chloride. The resulting eutectogels exhibited a high transparency (89%)

high mechanical strength (up to 2.8 MPa)

and exceptional tensile performance (up to 1385%). The fabricated flexible sensor demonstrated ideal linear sensitivity (gauge factor: 0.88)

a broad response range (1%–100%)

and reliable stability (over 1000 cycles)

enabling the precise monitoring of human motion (

e.g.

finger bending and wrist rotation). The flexible strain sensor based on this eutectogel is expected to show promising prospects for medical monitoring

human-machine interaction

and industrial sensing applications.

关键词

Keywords

references

Ma, H.; Wang, M.; Hou, J.; Wang, X.; Sun, P.; Wang, F. Strong and tough water-tolerant conductive eutectogels with phase-separated hydrophilic/hydrophobic dual ionic channels. Adv. Mater. 2025 , 37 , 2500770..

Tang, N.; Jiang, Y.; Wei, K.; Zheng, Z.; Zhang, H.; Hu, J. Evolutionary reinforcement of polymer networks: a stepwise-enhanced strategy for ultrarobust eutectogels. Adv. Mater. 2024 , 36 , 2309576..

Criado-Gonzalez, M.; Alegret, N.; Fracaroli, A. M.; Mantione, D.; Guzmán-González, G.; Del Olmo, R.; Tashiro, K.; Tomé, L. C.; Picchio, M. L.; Mecerreyes, D. Mixed conductive, injectable, and fluorescent supramolecular eutectogel composites. Angew. Chem. Int. Ed. 2023 , 62 , e202301489..

Fan, K.; Wei, W.; Zhang, Z.; Liu, B.; Feng, W.; Ma, Y.; Zhang, X. Highly stretchable, self-healing, and adhesive polymeric eutectogel enabled by hydrogen-bond networks for wearable strain sensor. Chem. Eng. J. 2022 , 449 , 137878..

Wu, W.; Li, D.; Gao, C.; Wu, H.; Bo, Y.; Zhang, J.; Ci, L.; Zhang, J. Eutectogel electrolyte constructs robust interfaces for high-voltage safe lithium metal battery. Adv. Sci. 2024 , 11 , 2310136..

Wang, J.; Zhang, S.; Ma, Z.; Yan, L. Deep eutectic solvents eutectogels: progress and challenges. Green Chem. Eng. 2021 , 2 , 359−367..

Li, W.; Wang, X.; Liu, Z.; Zou, X.; Shen, Z.; Liu, D.; Li, L.; Guo, Y.; Yan, F. Nanoconfined polymerization limits crack propagation in hysteresis-free gels. Nat. Mater. 2024 , 23 , 131−138..

Pan, Z.; Fu, Q. Q.; Wang, M. H.; Gao, H. L.; Dong, L.; Zhou, P.; Cheng, D. D.; Chen, Y.; Zou, D. H.; He, J. C.; Feng, X.; Yu, S. H. Designing nanohesives for rapid, universal, and robust hydrogel a dhesion. Nat. Commun. 2023 , 14 , 5378..

Wang, Y.; Xu, Z.; Lovrak, M.; le Sage, V. A. A.; Zhang, K.; Guo, X.; Eelkema, R.; Mendes, E.; van Esch, J. H. Biomimetic strain-stiffening self-assembled hydrogels. Angew. Chem. Int. Ed. 2020 , 59 , 4830−4834..

Fu, M.; Sun, Z.; Liu, X.; Huang, Z.; Luan, G.; Chen, Y.; Peng, J.; Yue, K. Highly stretchable, resilient, adhesive, and self-healing ionic hydrogels for thermoelectric application. Adv. Funct. Mater. 2023 , 33 , 2306086..

Huang, Z.; Deng, Z.; Liu, X.; Huang, T.; Hu, Y.; Chen, Y.; Liu, Y.; Guo, Z. H.; Yue, K. Highly stretchable, strain-stiffening, self-healing ionic conductors for wearable sensors. Chem. Eng. J. 2022 , 449 , 137633..

Yang, C.; Suo, Z. Hydrogel ionotronics. Nat. Rev. Mater. 2018 , 3 , 125−142..

Luo, C.; Huang, Z.; Guo, Z. H.; Yue, K. Recent progresses in liquid-free soft ionic conductive elastomers. Chin. J. Chem. 2023 , 41 , 835−860..

Luo, C.; Chen, Y.; Huang, Z.; Fu, M.; Ou, W.; Huang, T.; Yue, K. A fully self-healing and highly stretchable liquid-free ionic conductive elastomer for soft ionotronics. Adv. Funct. Mater. 2023 , 33 , 2304486..

He, S.; Cheng, Q.; Liu, Y.; Rong, Q.; Liu, M. Intrinsically anti-freezing and anti-dehydration hydrogel for multifunctional wearable sensors. Sci. China Mater. 2022 , 65 , 1980−1986..

Yan, Y.; Duan, S.; Liu, B.; Wu, S.; Alsaid, Y.; Yao, B.; Nandi, S.; Du, Y.; Wang, T. W.; Li, Y.; He, X. Tough hydrogel electrolytes for anti-freezing zinc-ion batteries. Adv. Mater. 2023 , 35 , 2211673..

Xu, C.; Yang, K.; Zhu, G.; Ou, C.; Jiang, J.; Zhuravlev, E.; Zhang, Y. Anti-freezing multifunctional conductive hydrogels: from structure design to flexible electronic devices. Mater. Chem. Front. 2024 , 8 , 381−403..

Hu, F.; Huang, Z.; Luo, C.; Yue, K. High-sensitivity and ultralow-hysteresis fluorine-rich ionogel strain sensors for multi-environment contact and contactless sensing. Mater. Horiz. 2023 , 10 , 5907−5919..

Huang, Z.; Chen, Y.; Peng, J.; Huang, T.; Hu, F.; Liu, X.; Xu, L.; Yue, K. Highly stretchable ionotronic pressure sensors with broad response range enabled by microstructured ionogel electrodes. J. Mater. Chem. A 2023 , 11 , 7201−7212..

Xu, L. G.; Huang, Z. K.; Deng, Z. S.; Du, Z. K.; Sun, T. L.; Guo, Z. H.; Yue, K. A Transparent, highly stretchable, solvent-resistant, recyclable multifunctional ionogel with underwater self-healing and adhesion for reliable strain sensors. Adv. Mater. 2021 , 33 , 2105306..

Chen, Y.; Luo, C.; Hu, F.; Huang, Z.; Yue, K. Recent advances in fluorinated polymers: synthesis and diverse applications. Sci. China Chem. 2023 , 66 , 3347−3359..

Chen, Y. T.; Huang, Z. K.; Hu, F. Q.; Peng, J. P.; Huang, T. R.; Liu, X.; Luo, C.; Xu, L. G.; Yue, K. Microstructured polyfluoroacrylate elastomeric dielectric layer for highly stretchable wide-range capacitive pressure sensors. ACS Appl. Mater. Interfaces 2023 , 15 , 58700−58710..

Li, M.; Liu, Z.; Hu, Y.; Li, R. a.; Cao, Y. A hydrophobic eutectogel with exc ellent underwater self-adhesion, self-healing, Transparency, Stretchability, ionic Conductivity, and fully recyclability. Chem. Eng. J. 2023 , 472 , 145177..

Zhu, J.; Shao, C.; Hao, S.; Xue, K.; Zhang, J.; Sun, Z.; Xiao, L. P.; Ren, W.; Yang, J.; Cao, B.; Sun, R. Green synthesis of multifunctional cellulose-based eutectogel using a metal salt hydrate-based deep eutectic solvent for sustainable self-powered sensing. Chem. Eng. J. 2025 , 506 , 159636..

Prasad, K.; Mondal, D.; Sharma, M.; Freire, M. G.; Mukesh, C.; Bhatt, J. Stimuli responsive ion gels based on polysaccharides and other polymers prepared using ionic liquids and deep eutectic solvents. Carbohydr. Polym. 2018 , 180 , 328−336..

Ge, G.; Mandal, K.; Haghniaz, R.; Li, M.; Xiao, X.; Carlson, L.; Jucaud, V.; Dokmeci, M. R.; Ho, G. W.; Khademhosseini, A. Deep eutectic solvents-based ionogels with ultrafast gelation and high adhesion in harsh environments. Adv. Funct. Mater. 2023 , 33 , 2207388..

Liang, Y. F.; Huang, X. J.; He, Z. J.; Pan, H. S.; Fan, L.; Li, X. Q.; Jin, R. H. Antibacterial, nontoxic, antifreezing, and self-adhesive conductive eutectogel for strain sensor. ACS Appl. Polym. Mater. 2025 , 7 , 1818−1830..

Wang, Y.; Wang, J.; Ma, Z.; Yan, L. A highly conductive, self-recoverable, and strong eutectogel of a deep eutectic solvent with polymer crystalline domain regulation. ACS Appl. Mater. Interfaces 2021 , 13 , 54409−54416..

Zhang, H.; Tang, N.; Yu, X.; Li, M. H.; Hu, J. Strong and tough physical eutectogels regulated by the spatiotemporal expression of non-covalent interactions. Adv. Funct. Mater. 2022 , 32 , 2206305..

[Huo, X.; Wang, J.; Cong, Z.; Liu, C.; Cai, C.; Wang, Y.; Zhang, X.; Li, C.; Lan, S.; Niu, J. Strong and tough eutectogels with broad-range tunable mechanical properties via the hydrogen bond network-specific effect. Adv. Funct. Mater . 2025, DOI: 10.1002/adfm.202422464..

Dong, M.; Han, Y.; Hao, X. P.; Yu, H. C.; Yin, J.; Du, M.; Zheng, Q.; Wu, Z. L. Digital light processing 3d printing of tough supramolecular hydrogels with sophisticated architectures as impact-absorption elements. Adv. Mater. 2022 , 34 , 2204333..

Hu, J. Y.; Jiao, D.; Hao, X. P.; Kong, X.; Zhang, X. N.; Du, M.; Zheng, Q.; Wu, Z. L. A facile strategy to fabricate tough and adhesive elastomers by in situ formation of coordination complexes as physical crosslinks. Adv. Funct. Mater. 2023 , 33 , 2307402..

Huang, Y.; Xiao, L.; Zhou, J.; Liu, T.; Yan, Y.; Long, S.; Li, X. Strong tough polyampholyte hydrogels via the synergistic effect of ionic and metal–ligand bonds. Adv. Funct. Mater. 2021 , 31 , 2103917..

Yu, H. C.; Hao, X. P.; Zhang, C. W.; Zheng, S. Y.; Du, M.; Liang, S.; Wu, Z. L.; Zheng, Q. Engineering tough metallosupramolecular hydrogel films with kirigami structures for compliant soft electronics. Small 2021 , 17 , 2103836..

[Hu, Y.; Yang, W. H.; Zhan, J. M.; Pu, C. Y.; Zhong, L. F.; Hou, H. H. Eutectogels: recent advances and emerging biological applications. Adv. Funct. Mater . 2025 , DOI: 10.1002/adfm.202425778.

You, M.; Zhou, J.; Zao, Y.; Xu, J.; Jin, Y.; Li, D.; Xu, Z.; Chen, C. Green synthesis of multifunctional wood-based eutectogels via initiator-free solar polymerization. Chem. Eng. J. 2025 , 504 , 158902..

Cruz, H.; Jordão, N.; Branco, L. C. Deep eutectic solvents (DESs) as low-cost and green electrolytes for electrochromic devices. Green Chem. 2017 , 19 , 1653−1658..

Intasian, P.; Prakinee, K.; Phintha, A.; Trisrivirat, D.; Weeranoppanant, N.; Wongnate, T.; Chaiyen, P. Enzymes, in vivo biocatalysis, and metabolic engineering for enabling a circular economy and sustainability. Chem. Rev. 2021 , 121 , 10367−10451..

Gu, Y.; Jérôme, F. Glycerol as a sustainable solvent for green chemistry. Green Chem. 2010 , 12 , 1127−1138..

Hu, J.; Yao, X.; Li, T. Q.; Li, X. J.; Wei, W.; Liu, J. C. Supramolecular ionic gels with high elasticity and self-healing based on polymeric deep eutectic solvent for 3D-printable soft sensors. ACS Appl. Polym. Mater. 2023 , 5 , 9650−9658..

[Vorobiov, V. K.; Sokolova, M. P.; Bobrova, N. V.; Elokhovsky, V. Y.; Smirnov, M. A. Rheological properties and 3D-printability of cellulose nanocrystals/deep eutectic solvent electroactive ion gels. Carbohydr. Polym . 2022, 290 ..

[Lai, C. W.; Yu, S. S. 3D printable strain sensors from deep eutectic solvents and cellulose nanocrystals. ACS Appl. Mater. Interfaces 2020, 12 , 34235−34244..

Zeng, Q.; Lai, X.; Li, H.; Chen, Z.; Zeng, X.; Zhang, L. High fire-safety and multifunctional eutectogel for flexible quasi-solid-state supercapacitors. Adv. Funct. Mater. 2024 , 34 , 2411029..

Li, X. Y.; Yan, M. K.; Xiao, J.; Lian, H. L. Ultrafast fabrication of deep eutectic solvent flexible ionic gel with high-transmittance, freeze-resistant and conductivity by frontal polymerization. J. Colloid Interface Sci. 2023 , 650 , 1382−1392..

Zhang, W.; Liu, X.; Wang, J.; Tang, J.; Hu, J.; Lu, T.; Suo, Z. Fatigue of double-network hydrogels. Eng. Fract. Mech. 2018 , 187 , 74−93..

Wang, J.; Wu, B.; Wei, P.; Sun, S.; Wu, P. Fatigue-free artificial ionic skin toughened by self-healable elastic nanomesh. Nat. Commun. 2022 , 13 , 4411..

Hou, J.; Zhang, X.; Wu, Y.; Jie, J.; Wang, Z.; Chen, G. Q.; Sun, J.; Wu, L. P. Amphiphilic and fatigue-resistant organohydrogels for small-diameter vascular grafts. Sci. Adv. 2022 , 8 , eabn5360..

Li, W.; Liu, X.; Deng, Z.; Chen, Y.; Yu, Q.; Tang, W.; Sun, T. L.; Zhang, Y. S.; Yue, K. Tough Bonding, on-demand debonding, and facile rebonding between hydrogels and diverse metal surfaces. Adv. Mater. 2019 , 31 , 1904732..

Huang, Z. K.; Xu, L. G.; Liu, P. J.; Peng, J. P. Transparent, mechanically robust, conductive, self-healable, and recyclable ionogels for flexible strain sensors and electroluminescent devices. RSC Adv. 2024 , 14 , 28234−28243..

[Huang, Z. K.; Xie, J. H.; Li, T. G.; Xu, L. G.; Liu, P. J.; Peng, J. P. Highly transparent, mechanically robust, and conductive eutectogel based on oligoethylene glycol and deep eutectic solvent for reliable human motions sensing. Polymers 2024, 16 , 2761..

Lu, Q.; Li, H.; Tan, Z. Zwitterionic eutectogel-based wearable strain sensor with superior stretchability, self-healing, self-adhesion, and wide temperature tolerance. ACS Appl. Mater. Interfaces 2023 , 15 , 34055−34063..

Yang, J.; Feng, Y.; Wang, B.; Miao, J.; Wei, S.; Li, H.; Mo, L.; Qin, Z. Tough, multifunctional, and green double-network binary solvent eutectogel with in-situ generation of lignin nanoparticles based on one-step dual phase separations for wearable flexible strain sensors. Chem. Eng. J. 2023 , 474 , 145544..

Wu, H.; Pang, Z.; Ji, L.; Pang, X.; Li, Y.; Yu, X. Strong adhesive, high conductive and environmentally stable eutectogel based on “Water in deep eutectic Solvent”: Ultrasensitive flexible temperature and strain sensors. Chem. Eng. J. 2024 , 497 , 154883..

Chen, H.; Zhang, F.; Zhang, Z.; Zhang, L. In-situ synthesis of biomimetic eutectogel sensors exhibiting softness, strain-stiffening, and anti-fatigue properties via a hierarchical bonding strategy. Chem. Eng. J. 2025 , 516 , 164085..

Zhou, N.; Cui, T.; Lei, Z.; Wu, P. Bioinspired learning and memory in ionogels through fast response and slow relaxation dynamics of ions. Nat. Commun. 2025 , 16 , 4573..

Views

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Utilizing Multilayer Design of Organic-Inorganic Hybrids to Enhance Wearable Strain Sensor in Humid Environment

Cellulose Solubility in Deep Eutectic Solvents: Inspecting Quantitative Hydrogen-Bonding Analysis

A Facile and Environment-friendly Method for Fabrication of Polymer Brush

Related Author

Hui Zhao

Robert K. Y. Li

Wei Wu

Peng Li

Wei-Chen Gao

Chen-Chen Lu

Bao-Qing Zhang

Kuang-Jie Xu

Related Institution

Guangxi Key Laboratory of Clean Pulp & Papermaking and Pollution Control, School of Light Industry and Food Engineering, Guangxi University

Guangxi Key Laboratory of Calcium Carbonate Resources Comprehensive Utilization, College of Materials and Chemical Engineering, Hezhou University

Department of Materials Science and Engineering, City University of Hong Kong, Tat Chee Avenue, Kowloon

CAS Key Laboratory of Engineering Plastics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, the Chinese Academy of Sciences

University of Chinese Academy of Sciences

⁰

Highly Transparent, Adhesive, and Mechanically Robust Eutectogel via Metal-coordination Physical Crosslinking for Reliable Flexible Strain Sensors

DOI：10.1007/s10118-025-3406-7

摘要

Abstract

关键词

Keywords

references