Effects of the Amylose/Amylopectin Ratio of Starch on Borax-Crosslinked Hydrogels.

Herein, we simultaneously prepared borax-crosslinked starch-based hydrogels with enhanced mechanical properties and self-healing ability via a simple one-pot method. The focus of this work is to study the effects of the amylose/amylopectin ratio of starch on the grafting reactions and the performance of the resulting borax-crosslinked hydrogels. An increase in the amylose/ amylopectin ratio increased the gel fraction and grafting ratio but decreased the swelling ratio and pore diameter. Compared with hydrogels prepared from low-amylose starches, hydrogels prepared from high-amylose starches showed pronouncedly increased network strength, and the maximum storage modulus increased by 8.54 times because unbranched amylose offered more hydroxyl groups to form dynamic borate ester bonds with borate ions and intermolecular hydrogen bonds, leading to an enhanced crosslink density. In addition, all the hydrogels exhibited a uniformly interconnected network structure. Furthermore, owing to the dynamic borate ester bonds and hydrogen bonds, the hydrogel exhibited excellent recovery behavior under continuous step strain, and it also showed thermal responsiveness.

Lignin-based vitrimer containing dynamic borate ester bonds with intrinsic photoconversion and excellent photothermal remoldability.

The development of photoresponsive shape memory materials based on the photothermal conversion properties of lignin and the low activation energy of the dynamic covalent borate bond is of great importance. In this paper, a kind of lignin-based vitrimer polymer (LBP) containing dynamic boronic ester bonds was prepared by a "sulfhydryl-epoxy" click reaction and etherification reaction. The results show that the rigid segment EP-EL (lignin-based epoxy resin) and BDB (2,2'-(1,4-phenylene)-bis-[4-mercapto-1,3,2-dioxaneborane]) with benzene ring structure can impart tensile strength (20.8 MPa) to the LBP, while the flexible segment PEG imparts good elongation at break (15 %). The dynamic binding and dissociation exchange mechanism of the boronic ester bonds enables LBP to exhibit thermal remodelling properties (up to 36.2 %) and water-assisted self-healing properties at room temperature (up to 49.0 %). In addition, LBP exhibits excellent thermal and light-responsive shape memory properties due to its own photothermal conversion performance (photothermal conversion efficiency up to 18.2 %) and the dynamic boronic ester bond thermal activation bond exchange mechanism. The insulating properties of LBP make it suitable for use in high temperature protection circuit devices and light-responsive circuit devices. This study provides new insights into the design and application of Vitrimer and photoresponsive shape memory polymers, and also offers a new avenue for high-value utilization of lignin.

Multifunctional Self-Healing Dual Network Hydrogels Constructed via Host-Guest Interaction and Dynamic Covalent Bond as Wearable Strain Sensors for Monitoring Human and Organ Motions.

Hydrogel-based flexible strain sensors have shown great potential in body movement tracking, early disease diagnosis, noninvasive treatment, electronic skins, and soft robotics. The good self-healing, biocompatible, sensitive and stretchable properties are the focus of hydrogel-based flexible strain sensors. Dual network (DN) hydrogels are hopeful to fabricate self-healing hydrogels with the above properties. Here, multifunctional DN hydrogels are prepared via a combination of host-guest interaction of ß-cyclodextrin and ferrocene with dynamic borate ester bonds of poly(vinyl alcohol) and borax. Carbon nanotubes are used to endow the DN hydrogels with good conductivity. The obtained DN composite hydrogels possess good biocompatibility, stretchability (436%), fracture strength (41.0 KPa), self-healing property (healing efficiency of 95%), and high tensile strain sensitivity (gauge factor of 5.9). The DN composite hydrogels are used as flexible strain sensors to detect different human motions. After cutting, the healed hydrogels also can monitor human motions and have good stability. In addition, the hydrogel sensors may track the respiratory movement of a pig lung in vitro. This work exhibits new ideas and approaches to develop multifunctional self-healing hydrogels for constructing flexible strain sensors.