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The development of conductive, soft, ultra-stretchable, and asymmetrically adhesive hydrogels is difficult and essential for both wearable electronics and anti-adhesion tissue dressings. In particular, there is still no simple, effective and universal approach to construct an asymmetrically adhesive multifunctional hydrogel. Here, we first synthesized lignosulfonate sodium (LS)-doped PAA hydrogels with uniform adhesion (adhesive strength: ~30.5 kPa), conductivity (~0.45 S/m), stretchability (up to ~2250%), and low compressive modulus (~20 kPa). In the second step, an oriented soaking of Fe 3+ onto the upper surface of the resultant composite hydrogel renders the upper surface non-adhesive. This novel strategy masterfully delivers asymmetric adhesion behavior to the upper and bottom surfaces of the same hydrogel (~0 kPa adhesive strength for the upper surface; strong adhesive strength of ~27 kPa for the bottom surface). The asymmetric adhesive hydrogel has proven to adhere well onto the human skin and achieve waste-barrier. Importantly, this hydrogel assembled pressure sensor demonstrates excellent anti-interference and wearable comfort., (Copyright © 2021 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.)

Inspired by mussel adhesion chemistry and ion electronics, a novel Ca2+-tannic acid@ sulfonated lignin-polyacrylamide (TA@SL-PAM) hydrogel was prepared via Ca2+-TA@SL composites and the PAM system, where a Ca2+-TA@SL composite was fabricated via TA doping with SL and the subsequent adsorption of Ca2+. The properties of the hydrogel were thoroughly investigated and the hydrogel was presented as multifunctional. The introduction of Ca2+-TA@SL composites endowed the hydrogel with excellent conductivity, adhesion and ultraviolet (UV) resistance, and improved antioxidant and antibacterial properties. More importantly, the Ca2+-TA@SL-PAM hydrogel electrode could accurately detect physiological signals of human (e.g., electrocardiogram (ECG), electromyography (EMG). [ABSTRACT FROM AUTHOR]

[Display omitted] Hydrogel devices still cannot overcome the dehydration puzzle. This problem can be solved by using green deep eutectic solvents (DES) instead of water, but the formed gel lacks enough strength and functionality. Herein, we successfully assembled a function-integrated stable anhydrous gel in DES system using active MXene as a function-filler. First, Mxene can catalyze the rapid polymerization of monomers at room temperature. Then, it can also assemble/crosslink the gel through strong interactions with the polymer chains, which endow the gel with great stretchability (∼1750%), self-healing (∼100%), conductivity (1.5 × 10-2 S·m−1), and adhesion (∼7 kPa;pigskin). In addition, the gel also inherits the environmental adaptability of DES, which can achieve nearly 100% weight retention at 40 °C, even 80 °C. Importantly, the application potential of stable functionalized gels in ultra-anti-dryness bioelectrodes, self-healing strain sensors, and electric-generators have been explored and successively demonstrated. The rapid fabrication of functional materials in this new solvent system can be extended to other anhydrous polymer gels for on-demand development. [ABSTRACT FROM AUTHOR]

Ti 3 C 2 T x (MXene), a new kind of 2D ceramic nanosheets, is receiving more and more attention in the fields of medicine, biology, energy, electronics, etc. However, the preparation and application of MXene in hydrogel is still in its infancy period. Here, we review the latest progress (after 2018) related to MXene hydrogels in time. Aiming at the key issue of the dispersion stability of MXene in hydrogel systems, the preparation strategy, mechanism, advantages and disadvantages of MXene hydrogels are sorted out in detail, and the potential application prospects of MXene composite hydrogel are introduced. Finally, future viewpoints are put forward for the dispersion stability challenges that need solving in the design of MXene hydrogel. [ABSTRACT FROM AUTHOR]

• The asymmetric hydrogel is adjusted and assembled by lignin and cellulose derivatives. • The hydrogel exhibits completely asymmetric adhesion, strength, and electriferous. • The hydrogel-based sensor has excellent skin adaptability and application stability. • The hydrogel can be applied to self-adhesive bioelectrodes and self-powered sensors. Mechanical adaptability, great wearability, application stability, and self-powered sensing characteristics are important requirements for hydrogel-based strain sensors. In this study, a novel double-layer hydrogel was fabricated with asymmetrical adhesion, strength, and electriferous properties. Wherein, the lignosulfonate sodium (LS)-borax mediated bottom hydrogel layer exhibits excellent softness (Young's modulus: ~14.2 kPa) and skin-adhesion (Adhesive strength: ~18.7 kPa) while the quaternary hydroxyethyl cellulose (QHEC) mediated top hydrogel layer demonstrates great mechanical strength (Young's modulus: ~101.3 kPa) and non-adhesive (Adhesive strength: ~2.2 kPa) properties. These complementary asymmetrical adhesion and strength properties endow the hydrogel-based sensor with exceptionally stable sensing performance and adaptive wearability; moreover, the lignocellulosic materials utilization plays a significant role in the designability, antibacterial and biodegradable properties. In addition, the synergy of negative LS (-) and positive QHEC (+) particles enables the double-layer hydrogel great self-powered sensing because of the directional movement of free ions initiated by the external mechanical stimulus. This study presents a hierarchical design idea of wearable electronics, which will have potential applications in many fields from wearable bioelectrodes to self-powered sensors. [ABSTRACT FROM AUTHOR]

• MXene can catalyze the ultrafast preparation of hydrogels by redox reaction. • MXene can regulate the internal structure and properties of the hydrogel. • Composite hydrogel has great stretchability (1400%) and recoverability. • Composite hydrogel can be used as a bioelectronic with adjustable adhesion. Re-stacking of 2D Ti 3 C 2 T X (MXene) nanosheets seriously limits their applications and development of effective strategies to overcome this issue remains challenging. Thus, an efficient method was proposed to rapidly fabricate (<20 min) a MXene nanosheets-catalyzed self-assembled, poly-acrylic acid (PAA) hydrogel with excellent conductivity, stretchability (~1400%), and anti-aggregation (>60 d) properties. In the proposed strategy, in-situ growth of TiO 2 nanoparticles (NPs) on MXene surfaces could effectively overcome the nanosheets restacking in solvents. Moreover, the reductive TiO 2 @MXene nanosheets not only catalyze the dissociation of the initiator generating sufficient radicals by redox reaction to initiate the ultrafast polymerization of AA monomers without heating, but also cross-link polymer chains (via chemical bonding) to produce hydrogel in a time scale of minutes instead of hours. Therefore, the MXene-catalyzed ultrafast self-assembly design effectively overcame the problem associated with the re-aggregation of nanosheets in hydrogels. More importantly, the structural, mechanical, swelling, adhesive, and conductive performances of the hydrogel could be adjusted by altering the TiO 2 @MXene contents. This strategy should be extended to almost all types of MXene-radical polymerized hydrogels with tunable structures and performances that have potential applications in the field of wearable bioelectronics. [ABSTRACT FROM AUTHOR]

• The redox SL-Fe3+ chelates can shorten the hydrogel gelation time by 99.67%. • The hydrogel obtained stretchable, conductive, adhesive, and UV-blocking properties. • The green SL-Fe3+ chelates imparts excellent self-healing properties of the hydrogel. • The rapid preparation of soft multifunctional coatings electronics was proposed. Developing an ecological and economical method for fabrication and application of polymer hydrogels is important for the hydrogel/coating electronics. Here, a dynamic oxidation and coordination system composed of sulfonated lignin (SL) and Fe3+ was introduced to assemble multifunctional Fe-SL-g-polyacrylic acid (PAA) hydrogel at 20 ℃ in a time scale of minutes instead of hours. The SL-Fe3+ system can rapidly activate the ammonium persulfate (APS, initiator), and then it instantaneously provides abundant semiquinone and hydroxyl radicals to accelerate the formation of polymer chains. Moreover, the functional SL-Fe3+ chelates can also reversibly crosslink the polymer chains to form multifunctional hydrogels. Surprisingly, the resultant hydrogel obtained charming extension ratio (up to 1680%), conductivity (up to 7.0 × 10-2 S·m−1), and adhesive strength (up to 36.4 kPa). This technology was also applied to rapidly fabricate a transparent (up to 81%, thickness: 2 mm), UV-blocking (up to 99.7%, thickness: 2 mm), adhesive, and conductive hydrogel coating on substrates. Besides, the dynamic coordination inside the hydrogel imparts desirable self-healing capabilities to damaged network, with up to 98.5% recovery in conductivity and 85.7% in extension ratio. In short, this technology based on the sustainable SL-Fe3+ system greatly facilitates the rapid and low-cost preparation of multifunctional hydrogel/coatings, which have promising industrial applications in human–machine electronics. [ABSTRACT FROM AUTHOR]

The restacking tendency of 2D Ti 3 C 2 T X (MXene) sheets is the main obstacle preventing their application as functional materials in hydrogel. Herein, we fabricated novel ultra-stable 3D MXene-polyacrylamide (PAM) nanocomposite hydrogels inspired by the structure of a spider web. In particular, MXene nanosheets were uniformly located in a gel medium by precise alignment of sonication treatments, followed by the in-situ self-assembly of PAM hydrogel. In this instance, the MXene nanosheets are well-confined and trapped (via strong interactions) by the interwoven spider web-like structure of the PAM chains, which grow in-situ on the surface of the nanosheets. This approach proved effective to solve problems associated with the poor stability of MXene nanosheets in the hydrogel; more prominently, the tight cross-linked structure endows the MXene-PAM hydrogel with anti-compressive and anti-swelling capabilities; the continuous distribution of MXene nanosheets connected by the PAM network creates electron transport pathways and proton transport bridges in the hydrogel. Therefore, the hydrogel can be employed as a temperature and strain sensor or as a component of moist-electric nanogenerator. Image 1 • A temporary alignment and permanent in-situ fixation design was proposed. • Spider web-inspired anti-aggregation robust MXene hydrogel was constructed. • The DFT study predicts the formation for the bionic networks. • The hydrogel can be employed as sensor or moist-electric nanogenerator. [ABSTRACT FROM AUTHOR]