Mechanical Training Enabled Reinforcement of Polyrotaxane-Containing Hydrogel.

Many strategies have been developed for constructing anisotropic hydrogels, however, it remains a challenge to fabricate hydrogels with anisotropic nanocrystalline domains from intrinsically soft networks. Here, we report a naphthotube-based polyrotaxane-containing hydrogel that can be reinforced via mechanical training. During the training process, the hydrogel can adopt reorientation of polymer chains to form anisotropic structures driven by external uniaxial force. Due to the multiple hydrogen bonding sites and movable feature of naphthotube, the sliding of naphthotube on PEG chains simultaneously inducing the zipping of adjacent polymer chains to form densely anisotropic nanocrystalline domains through hydrogen bonded networks. Thus, the trained hydrogel exhibits an enhanced tension stress of ≈110 kPa, which realize a remarkable enhancement of ≈10 times compare to initial state. This study provides a new tactic for improving the mechanical performance of soft materials.

Mechanical Training-Driven Structural Remodeling: A Rational Route for Outstanding Highly Hydrated Silk Materials.

Highly hydrated silk materials (HHSMs) have been the focus of extensive research due to their usefulness in tissue engineering, regenerative medicine, and soft devices, among other fields. However, HHSMs have weak mechanical properties that limit their practical applications. Inspired by the mechanical training-driven structural remodeling strategy (MTDSRS) in biological tissues, herein, engineered MTDSRS is developed for self-reinforcement of HHSMs to improve their inherent mechanical properties and broaden potential utility. The MTDSRS consists of repetitive mechanical training and solvent-induced conformation transitions. Solvent-induced conformation transition enables the formation of ß-sheet physical crosslinks among the proteins, while the repetitive mechanical loading allows the rearrangement of physically crosslinked proteins along the loading direction. Such synergistic effects produce strong and stiff mechanically trained-HHSMs (MT-HHSMs). The fracture strength and Young's modulus of the resultant MT-HHSMs (water content of 43 ± 4%) reach 4.7 ± 0.9 and 21.3 ± 2.1 MPa, respectively, which are 8-fold stronger and 13-fold stiffer than those of the as-prepared HHSMs, as well as superior to most previously reported HHSMs with comparable water content. In addition, the animal silk-like highly oriented molecular crosslinking network structure also provides MT-HHSMs with fascinating physical and functional features, such as stress-birefringence responsibility, humidity-induced actuation, and repeatable self-folding deformation.

Strengthen oriented poly (L-lactic acid) monofilaments via mechanical training.

Polymer materials have found extensive applications in the clinical and medical domains due to their exceptional biocompatibility and biodegradability. Compared to metallic counterparts, polymers, particularly Poly (L-lactic acid) (PLLA), are more suitable for fabricating biodegradable stents. As a viscoelastic material, PLLA monofilaments exhibit a creep phenomenon under sustained tensile stress. This study explores the use of creep to enhance the mechanical attributes of PLLA monofilaments. By subjecting the highly oriented monofilaments to controlled, constant force stretching, we achieved notable improvements in their mechanical characteristics. The results, as confirmed by tensile testing and dynamic mechanical analysis, revealed a remarkable 67 % increase in total elongation and over a 20 % rise in storage modulus post-mechanical training. Further microscopic analyses, including Atomic Force Microscopy (AFM) and Scanning Electron Microscopy (SEM), revealed enhanced spacing and cavity formation. These mechanical advancements are attributed to the unraveling and a more orderly arrangement of molecular chains in the amorphous regions. This investigation offers a promising approach for augmenting the mechanical properties of PLLA monofilaments, potentially benefiting their application in biomedical engineering.

Tough and stretchable all-κ-carrageenan hydrogel based on the cooperative effects between chain conformation transition and stepwise mechanical training.

The traditional κ-carrageenan (κCG)-based hydrogel obtained from hot water can rupture easily under mechanical loading. To address this vulnerability, here we presented a robust all-κCG hydrogel without employing the second synthetic network. By simply regulating the polymer chains from random coil to stiff chain conformation in NaOH/urea solvent system via the freeze-thawing process, the as-prepared hydrogel with homogeneous structure can display an enhanced stretchability from 42.1 to 156 %, while maintaining the similar fracture stress. Moreover, upon the stepwise mechanical training and subsequent incubation in KCl aqueous solution, more helical segments of κCG were aligned and involved into the association domains, thus leading to the increment in both the crystallinity and anisotropy. Consequently, a fast self-strengthening behavior occurred, and a more stretchable (fracture strain up to 396 %), strong (stress âˆ¼ 0.55 MPa) and tough (∼1.52 MJ m-3) κCG hydrogel was obtained. In comparison to the traditional one, the fracture strain and toughness are increased by 8.5 and 11.5 times, respectively. In addition, this κCG hydrogel can demonstrate good recovery and shape-memory behaviors under medium deformation. Hence, this tough all-κCG hydrogel is expected to be tailored into the biomaterials as the wearable device, artificial tendon, and cartilage in the future.

Ultra-strong hydroxypropyl cellulose/polyvinyl alcohol composite hydrogel by combination of triple-network and mechanical training.

To develop the hydrogels with high mechanical strength and excellent conductivity is always a challenging topic. In this study, the ultra-strong hydroxypropyl cellulose (HPC)/polyvinyl alcohol (PVA) composite hydrogels were prepared by combination of the triple-network and mechanical training. The proposed composite hydrogels were achieved by physically crosslinking HPC with PVA to form the first crosslinking network, in which the HPC fibers could decrease the crosslinking density of PVA matrix and generate a lot of water-rich porous area. Then, 2-hydroxyethyl acrylate (HEA), acrylamide (AM) and aluminium chloride diffused into the first network to fabricate the chemical crosslinking network and ionically cross-linked domains. The formation of triple-network enhanced the mechanical strength and toughness to 1.87 MPa and 339.09 kJ/m3, respectively. Especially, the crystalline domains of PVA chains could improve the hydrogel's fatigue resistance, and the orderly arrangement of the crystalline domains achieved through mechanical training process could further enhance the mechanical strength. The mechanical strength of pre-stretched composite hydrogel was increased up to 2.8 MPa. The composite hydrogels exhibit great applications in sensors, human-machine interactions, and wearable devices.