Evolutionary Reinforcement of Polymer Networks: A Stepwise‐Enhanced Strategy for Ultrarobust Eutectogels

Abstract

Gel materials are appealing due to their diverse applications in biomedicine, soft electronics, sensors, and actuators. Nevertheless, the existing synthetic gels are often plagued by feeble network structures and inherent defects associated with solvents, which compromise their mechanical load‐bearing capacity and cast persistent doubts about their reliability. Herein, combined with attractive deep eutectic solvent (DES), a stepwise‐enhanced strategy is presented to fabricate ultrarobust eutectogels. It focuses on the continuous modulation and optimization of polymer networks through complementary annealing and solvent exchange processes, which drives a progressive increase in both quantity and mass of the interconnected polymer chains at microscopic scale, hence contributing to the evolutionary enhancement of network structure. The resultant eutectogel exhibits superb mechanical properties, including record‐breaking strength (31.8 MPa), toughness (76.0 MJ m−3), and Young's modulus (25.6 MPa), together with exceptional resistance ability to tear and crack propagation. Moreover, this eutectogel is able to be further programmed through photolithography to in situ create patterned eutectogel for imparting specific functionalities. Enhanced by its broad applicability to various DES combinations, this stepwise‐enhanced strategy is poised to serve as a crucial template and methodology for the future development of robust gels.

Dynamically Cross-Linked Double-Network Hydrogels with Matched Mechanical Properties and Ideal Biocompatibility for Artificial Blood Vessels

“…Figure b shows the XRD patterns of the prepared PCO hydrogels with varying ratios of raw materials. The crystalline peaks formed at 20.42 and 40° in PVA indicate its semicrystalline nature, corresponding to characteristic reflection planes of semicrystalline PVA (101) and (102) planes . The addition of CMCS leads to a gradual decrease in the peak intensity at 20.42 and 40°, indicating a reduction in the crystallinity of PVA and suggesting the formation of an interpenetrating network composed of PVA and CMCS scaffolds.…”

“…The crystalline peaks formed at 20.42 and 40°in PVA indicate its semicrystalline nature, corresponding to characteristic reflection planes of semicrystalline PVA (101) and (102) planes. 33 The addition of CMCS leads to a gradual decrease in the peak intensity at 20.42 and 40°, indicating a reduction in the In addition, a TGA test was performed to characterize the thermal stability of the PCO hydrogels with different raw material ratios. As shown in Figure 1c,d, the weight loss during the first stage increased with increasing CMCS content, which might be attributed to the cleavage of the glycosidic linkage.…”

A flexible, stretchable and wearable strain sensor based on physical eutectogels for deep learning-assisted motion identification

“…21,22 DES not only shows a high inherent electrical conductivity, weak volatility, and high thermal stability but also exhibits cost-effectiveness, facile operation, non-toxicity, and eco-friendliness. 23,24 Thus, eutectogels are extremely suitable to substitute temperatureintolerant hydrogels 25 and high-cost ionogels 26 as flexible ionic conductors. 27 Typically, eutectogels can be categorized into two types: chemical eutectogels and physical eutectogels.…”

High Strength and Toughness Polymeric Triboelectric Materials Enabled by Dense Crystal-Domain Cross-Linking

“…Polymeric network architecture intimately governs energy dissipation capabilities. 21,22 Meticulously designed networks enable the balancing of high strength and toughness, unlocking avenues for broad-spectrum mechanical property regulation. Studies employing ionic or crystalline domain cross-linking have successfully constructed dense, interconnected networks, imbuing materials with tunable strength and elastic modulus, thereby expanding their application potential.…”

“…Polymeric network architecture intimately governs energy dissipation capabilities. , Meticulously designed networks enable the balancing of high strength and toughness, unlocking avenues for broad-spectrum mechanical property regulation. Studies employing ionic or crystalline domain cross-linking have successfully constructed dense, interconnected networks, imbuing materials with tunable strength and elastic modulus, thereby expanding their application potential. − Furthermore, strategies like dynamic nanoconfinement, multiple hydrogen bond interactions, and physical cross-linking have been harnessed to engineer flexible polymeric materials boasting exceptional mechanical properties, serving as valuable references for regulating the mechanics of polymeric triboelectric materials.…”