Extremely Tough and Stretchable Hydrophobic Deep Eutectic Solvent-Based Gels with Strong Adhesion and Moisture Resistance for Wearable Strain Sensors

Wu, Linlin; Gao, Yifeng; Wang, Rui; Yu, Kaixuan; Ma, Xiaofeng; Fang, Ying; Dou, Qiang

doi:10.1021/acsapm.3c02361

Cited by 6 publications

References 51 publications

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Applications of Functional Polymeric Eutectogels

Nicolau,

Mutch,

Thickett

2024

Macromol. Rapid Commun.

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Over the past two decades, deep eutectic solvents (DESs) have captured significant attention as an emergent class of solvents that have unique properties and applications in differing fields of chemistry. One area where DES systems find utility is the design of polymeric gels, often referred to as “eutectogels,” which can be prepared either using a DES to replace a traditional solvent, or where monomers form part of the DES themselves. Due to the extensive network of intramolecular interactions (e.g., hydrogen bonding) and ionic species that exist in DES systems, polymeric eutectogels often possess appealing material properties—high adhesive strength, tuneable viscosity, rapid polymerization kinetics, good conductivity, as well as high strength and flexibility. In addition, non‐covalent crosslinking approaches are possible due to the inherent interactions that exist in these materials. This review considers several key applications of polymeric eutectogels, including organic electronics, wearable sensor technologies, 3D printing resins, adhesives, and a range of various biomedical applications. The design, synthesis, and properties of these eutectogels are discussed, in addition to the advantages of this synthetic approach in comparison to traditional gel design. Perspectives on the future directions of this field are also highlighted.

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Applications of Functional Polymeric Eutectogels

Nicolau,

Mutch,

Thickett

2024

Macromol. Rapid Commun.

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Tough and Stretchable Zwitterionic Eutectogels via Copolymerization‐Induced Phase Separation in a Targeted Deep Eutectic Solvent

Wang,

Gao,

et al. 2024

Macromol. Rapid Commun.

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Deep eutectic solvent (DES)‐based eutectogels show significant promise for flexible sensors due to their high ionic conductivity, non‐volatility, biocompatibility, and cost‐effectiveness. However, achieving tough and stretchable eutectogels is challenging, as the highly polar DES tends to screen noncovalent bonds, such as hydrogen and ionic bonds, between polymer chains, limiting their mechanical strength. In this work, this issue is addressed by leveraging the limited solubility of zwitterionic polymers in a specific DES to induce phase separation, promoting dipole–dipole interactions between polymer chains. These interactions improve energy dissipation under mechanical stress, allowing the creation of tough and stretchable P(MAA‐co‐VIPS)/TBAC‐EG eutectogels through a copolymerization‐induced phase separation approach. Methacrylic acid (MAA) and sulfobetaine vinylimidazole (VIPS) are copolymerized within a tetrabutylammonium chloride‐ethylene glycol (TBAC‐EG) DES, resulting in a bicontinuous network. The bicontinuous structure consists of a PVIPS‐rich phase that enhances toughness via dipole–dipole interactions, and a PMAA solvent‐rich phase that enables high stretchability. The resulting eutectogel demonstrates excellent mechanical properties, including a strength of 1.76 MPa, toughness of 16.61 MJ m⁻3, and remarkable stretchability of 1293%, along with self‐recovery, self‐healing, and shape‐memory capabilities. The zwitterionic polymer‐specific DES design opens up broad application potential for these eutectogels in diverse fields.

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