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Lignin, as the most abundant aromatic biopolymer, is being widely studied to replace phenol and some other petroleum-based materials in the polymer industry. However, the low substitution of lignin and high levels of additives greatly limited the applications of lignin-based materials. Herein, we first propose a simple but effective hydrothermal method assisted synthesis for the fabrication of self-crosslinked lignin-based hydrogels (Lig-Scgel) with super-high-contents (75 wt%) of lignin and controllable mechanical properties. The self-crosslink mechanism was inspired by the repolymerization of lignins under a hydrothermal environment. The employment of self-condensation of lignin subunits in the synthesis of Lig-Scgel can significantly improve the degree of crosslinking, thereby greatly reducing the addition of toxic crosslinkers. The appearances, microstructures, crosslink densities, and mechanical properties of Lig-Scgels can be well controlled by simply altering the hydrothermal temperatures. This strategy not only promotes green and large-scale applications of lignin but also provides insights in the development of environment-friendly polymeric materials., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Soft and elastic polymer hydrogel materials are booming in the fields of wearable biomimetic skin, sensors, robotics, and bioelectrodes. Currently, many researchers are exploring new chemistries for the preparation of hydrogels to improve their performance. In the present study, we design and develop a strategy to prepare lignin reinforced hydrogels based on disulfide bond crosslinking mechanisms, and resultant hydrogels exhibit excellent stretchability, with tensile strain of up to 1085.4%, and high adhesion (with the highest T-peel strength of up to 432.2 N/m to pigskin). The underlying mechanism is based on the disulfide bonds that act as crosslinkers in the as-prepared hydrogel, and they can be easily cleaved and re-formed under mild conditions. Thanks to the presence of lignin, the as-obtained hydrogels also have excellent UV shielding effect. When assembled into a strain sensor, they can output stable and sensitive sensing signals, with gauge factor (GF) of 2.72 (strain: 0-72.8%). Furthermore, a simple and effective strategy to construct asymmetric adhesive hydrogels was adopted, which is based on directional soaking of the top portion of the hydrogel in a high-concentrated calcium chloride solution. The asymmetric hydrogel strain sensor transmits accurate and stable signals without the interference of various contaminants., (Copyright © 2022 Elsevier B.V. All rights reserved.)

In recent years, various biomacromolecule-based hydrogels have been extensively and deeply studied in the field of wearable electronics. However, the application of lignin-based hydrogels in flexible devices is still in its infancy. This is mainly due to the significant differences in physical and chemical properties of industrially extracted lignin. In order to seek the universal applicability of diversified lignin in the preparation of hydrogel electronics, we mainly paid attention to the natural physical and chemical properties of lignin to discuss feasible solutions for functional gel design. These properties include chemical reactivity, UV shielding, antibacterial, bio-degradability, anti-oxidation, etc. Finally, in view of lignin's unique properties and the demand for high-quality flexible electronics, some insights are proposed regarding the future research and development directions of lignin-based hydrogel electronics., Competing Interests: Declaration of competing interest The authors declare no competing financial interest., (Copyright © 2021 Elsevier B.V. All rights reserved.)

This study demonstrated a facile method to synthesize lignin-based carbon dots (L-CDs) first. Results indicated that the L-CDs had a diameter of 2-5 nm and a graphene-like crystalline structure. It was found that under the optimal synthesis conditions, the fluorescence lifetime of L-CDs was about 12 ns. Within the range of pH 1-10, the fluorescence intensity of the L-CDs and pH value followed a linear relationship. With the contribution of L-CDs, pH/temperature dual responsive hydrogel was synthesized. The elastic modulus G' of hydrogel was much higher than viscous modulus G″. When the PVA content was larger than 10 wt%, the temperature sensitivity and water retention rate gradually decreased. The skeleton of hydrogels had a typical porous honeycomb structure, which made it possible to control its internal pore size by adjusting the content of PVA. There was a linear relationship between the fluorescence intensity of hydrogels and pH value in the range of pH 1-7. Therefore, the pH/temperature dual responsive hydrogel presented a new route for designing tissue engineering scaffolds and drug carriers., (Copyright © 2021 Elsevier B.V. All rights reserved.)