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Polyampholyte (PA) hydrogels are randomly copolymerized from anionic and cationic monomers, showing good mechanical properties owing to the existence of numerous ionic bonds in the networks. However, relatively tough PA gels can be synthesized successfully only at high monomer concentrations (CM), where relatively strong chain entanglements exist to stabilize the primary supramolecular networks. This study aims to toughen weak PA gels with relatively weak primary topological entanglements (at relatively low CM) via a secondary equilibrium approach. According to this approach, an as-prepared PA gel is first dialyzed in a FeCl3 solution to reach a swelling equilibrium and then dialyzed in sufficient deionized water to remove excess free ions to achieve a new equilibrium, resulting in the modified PA gels. It is proved that the modified PA gels are eventually constructed by both ionic and metal coordination bonds, which could synergistically enhance the chain interactions and enable the network toughening. Systematic studies indicate that both CM and FeCl3 concentration (CFeCl3) influence the enhancement effectiveness of the modified PA gels, although all the gels could be dramatically enhanced. The mechanical properties of the modified PA gel could be optimized at CM = 2.0 M and CFeCl3 = 0.3 M, where the Young’s modulus, tensile fracture strength, and work of tension are improved by 1800%, 600%, and 820%, respectively, comparing to these of the original PA gel. By selecting a different PA gel system and diverse metal ions (i.e., Al3+, Mg2+, Ca2+), we further prove that the proposed approach is generally appliable. A theoretical model is used to understand the toughening mechanism. This work well extends the simple yet general approach for the toughening of weak PA gels with relatively weak chain entanglements.

Hydrogels with high mechanical strength, good crack resistance, and good adhesion are highly desirable in various areas, such as soft electronics and wound dressing. Yet, these properties are usually mutually exclusive, so achieving such hydrogels is difficult. Herein, we fabricate a series of strong, tough, and adhesive composite hydrogels from polyampholyte (PA) gel reinforced by nonwoven cellulose-based fiber fabric (CF) via a simple composite strategy. In this strategy, CF could form a good interface with the relatively tough PA gel matrix, providing high load-bearing capability and good crack resistance for the composite gels. The relatively soft, sticky PA gel matrix could also provide a large effective contact area to achieve good adhesion. The effect of CF content on the mechanical and adhesion properties of composite gels is systematically studied. The optimized composite gel possesses 35.2 MPa of Young’s modulus, 4.3 MPa of tensile strength, 8.1 kJ m−2 of tearing energy, 943 kPa of self-adhesive strength, and 1.4 kJ m−2 of self-adhesive energy, which is 22.1, 2.3, 1.8, 6.0, and 4.2 times those of the gel matrix, respectively. The samples could also form good adhesion to diverse substrates. This work opens a simple route for fabricating strong, tough, and adhesive hydrogels.

With increasing global energy consumption, oil/gas drilling has gradually expanded from conventional shallow reservoirs to deep and ultra-deep reservoirs. However, the harsh geological features including high temperature and high salinity in ultra-deep reservoirs have become a critical challenge faced by water-based drilling fluids (WDFs), which seriously deteriorate the rheology and fluid loss properties, causing drilling accidents, such as wellbore instability and formation collapse. In this study, a novel temperature- and salt-resistant micro-crosslinked polyampholyte gel was synthesized using N,N-dimethylacrylamide, diallyldimethyl ammonium chloride, 2-acrylamido-2-methylpropanesulfonic acid, maleic anhydride and chemical crosslinking agent triallylamine through free radical copolymerization. Due to the synergistic effect of covalent micro-crosslinking and the reverse polyelectrolyte effect of amphoteric polymers, the copolymer-based drilling fluids exhibit outstanding rheological and filtration properties even after aging at high temperatures (up to 200 °C) and high salinity (saturated salt) environments. In addition, the zeta potential and particle size distribution of copolymer-based drilling fluids further confirmed that the copolymer can greatly improve the stability of the base fluid suspension, which is important for reducing the fluid-loss volume of WDFs. Therefore, this work will point out a new direction for the development of temperature- and salt-resistant drilling fluid treatment agents.