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Softness is a crucial criterion in assessing the comfort and usability of tissue paper. Flexible fibers contribute to the softness of the tissue paper by allowing the sheets to conform to the contours of the skin without feeling rough or abrasive. This study focuses on developing innovative CGG/APAM/PDA hydrogels with interpenetrating networks consisting of cationic guar gum, anionic polyacrylamide, and polydopamine for cellulase immobilization, aimed at improving bamboo fiber flexibility. Cellulase biomolecules are efficiently immobilized on CGG/APAM/PDA hydrogels through the Schiff base reaction. Immobilized cellulases have a wider pH applicability than free cellulases, good storage stability, and can maintain high relative activity at relatively high temperatures. The treatment of bamboo fibers with immobilized cellulase results in a significant increase in flexibility, reaching 6.90 × 10 14  N·m 2 , which is 7.18 times higher than that of untreated fibers. The immobilization of cellulases using CGG/APAM/PDA hydrogels as carriers results in a substantial enhancement of storage stability, pH applicability, and inter-fiber bonding strength, as well as the capacity to sustain high relative enzymatic activity at elevated temperatures. The immobilization of cellulase within CGG/APAM/PDA interpenetrating network hydrogels presents a viable strategy for enhancing bamboo fiber flexibility, thereby expanding the accessibility of tissue products., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Electromagnetic hydrogels have attracted significant attention due to their vast potential in soft robotics, biomedical engineering, and energy harvesting. To facilitate future commercialization via large-scale industrial processes, we present a facile concept that utilizes the specialized knowledge of papermaking to fabricate hydrogels with multifunctional electromagnetic properties. The principles of papermaking wet end chemistry, which involves the handling of interactions among cellulosic fibers, fines, polymeric additives, and other components in aqueous systems, serves as a key foundation for this concept. Notably, based on these principles, the versatile use of chemical additives in combination with cellulosic materials enables the tailored design of various products. Our methodology exploits the unique hierarchically pitted and hollow tube-like structures of papermaking grade cellulosic fibers with discernible pits, enabling the incorporation of magnetite nanoparticles through lumen loading. By combining microscale softwood-derived cellulosic fibers with additives, we achieve dynamic covalent interactions that transform the cellulosic fiber slurry into an impressive hydrogel. The cellulosic fibers act as a skeleton, providing structural support within the hydrogel framework and facilitating the dispersion of nanoparticles. In accordance with our concept, the typical hydrogel exhibits combined attributes, including electrical conductivity, self-healing properties, pH responsiveness, and dynamic rheologic behavior. Our approach not only yields hydrogels with interesting properties but also aligns with the forefront of advanced cellulosic material applications. These materials hold the promise in remote strain sensing devices, electromagnetic navigation systems, contactless toys, and flexible electronic devices. The concept and findings of the current work may shed light on materials innovation based on traditional pulp and paper processes. Furthermore, the facile processes involved in hydrogel formation can serve as valuable tools for chemistry and materials education, providing easy demonstrations of principles for university students at different levels., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

Treatment of infected wound by simultaneously eliminating bacteria and inducing angiogenesis to promote wound tissue regeneration remains a clinical challenge. Dynamic and reversable hydrogels can adapt to irregular wound beds, which have raised great attention as wound dressings. Herein, a sprayable chitosan-based hydrogel (HPC/CCS/ODex-IGF1) was developed using hydroxypropyl chitosan (HPC), caffeic acid functionalized chitosan (CCS), oxidized dextran (ODex) to crosslink through the dynamic imine bond, which was pH-responsive to the acidic microenvironment and could controllably release insulin growth factor-1 (IGF1). The HPC/CCS/ODex-IGF1 hydrogels not only showed self-healing, self-adaptable and sprayable properties, but also exhibited excellent antibacterial ability, antioxidant property, low-cytotoxicity and angiogenetic activity. In vivo experiments demonstrated that hydrogels promoted tissue regeneration and healing of bacteria-infected wound with a rate of approximately 98.4 % on day 11 by eliminating bacteria, reducing inflammatory and facilitating angiogenesis, demonstrating its great potential for wound dressing., Competing Interests: Declaration of competing interest The author declare that they have no competing financial interests or personal relationships that could have appeared to influence the work reported in the paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Hydrogels are highly sought-after absorbent materials for absorbent pads; however, it is still challenging to achieve a satisfactory balance between mechanical performance, water absorption capacity, and active functionalities. In this work, we presented double-network hydrogels synthesized through acrylic acid (AA) polymerization in the presence of quaternized cellulose nanofibrils (QCNF) and Fe 3+ . Spectroscopic and microscopic analyses revealed that the combined QCNF and Fe 3+ facilitated the formation of double-network hydrogels with combined chemical and physical crosslinking. The synergistic effect of QCNF and Fe 3+ resulted in impressive mechanical properties, including tensile strength of 1.98 MPa, fracture elongation of 838.8 %, toughness of 7.47 MJ m -3 , and elastic modulus of 0.35 MPa. In comparison to the single-network PAA hydrogel, the PAA/QCNF/Fe 3+ (PQFe) hydrogels showed higher and relatively stable swelling ratios under varying pH levels and saline conditions. The PQFe hydrogels exhibited notable antioxidant activity, as evidenced by the 2,2-diphenyl-1-picrylhydrazyl (DPPH) assay, and demonstrated effective antibacterial activity against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). These hydrogels show promising potential as an absorbent interlayer in absorbent pads for active food packaging., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier Ltd.)

In this study, we address the challenge of developing highly conductive hydrogels with enhanced stretchability for use in wearable sensors, which are critical for the precise detection of human motion and subtle physiological strains. Our novel approach utilizes amylopectin, a biopolymer, for the uniform integration of liquid metal gallium into the hydrogel matrix. This integration results in a conductive hydrogel characterized by remarkable elasticity (up to 7100 % extensibility) and superior electrical conductance (Gauge Factor = 31.4), coupled with a minimal detection limit of less than 0.1 % and exceptional durability over 5000 cycles. The hydrogel demonstrates significant antibacterial activity, inhibiting microbial growth in moist environments, thus enhancing its applicability in medical settings. Employing a synthesis process that involves ambient condition polymerization of acrylic acid, facilitated by a hydrophobic associative framework, this hydrogel stands out for its rapid gelation and robust mechanical properties. The potential applications of this hydrogel extend beyond wearable sensors, promising advancements in human-computer interaction through technologies like wireless actuation of robotic systems. This study not only introduces a viable material for current wearable technologies but also sets a foundation for future innovations in bio-compatible sensors and interactive devices., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Biomass-based hydrogels have displayed excellent potential in flexible strain sensors due to their adequacy, biocompatibility, nontoxic and degradability. Nevertheless, their inferior mechanical properties, particularly at cryogenic temperatures, impeded their extensive utilization. Herein, we reported a rationally designed strain sensor fabricated from a gelatin and cellulose-derived hydrogel with superior mechanical robustness, cryogenic endurance, and flexibility, owing to a triple dynamic bond strategy (TDBS), namely the synergistic reinforcement among potent hydrogen bonds, imine bonds, and sodium bonds. Beyond conventional sacrificing bonds consisting of hydrogen bonds, dynamic covalent bonds and coordinate bonds, synergetic triple dynamic bonds dominated by strong hydrogen bonds and assisted by imine and sodium bonds with higher strength can dissipate more mechanical energy endowing the hydrogel with 38-fold enhancement in tensile strength (6.4 MPa) and 39-fold improvement in toughness (2.9 MPa). We further demonstrated that this hydrogel can work as a robust and biodegradable strain sensor exhibiting remarkable flexibility, broad detection range, considerable sensitivity and excellent sensing stability. Furthermore, owing to the improved nonfreezing performance achieved from incorporating sodium salts, the sensor delivered outstanding sensing properties under subzero conditions such as -20 and -4 °C. It is anticipated that the TDBS can create diverse high-performance soft-electronics for broad applications in human-machine interfaces, energy and healthcare.

In this study, the quaternized carboxymethyl chitosan (QCMCS), oxidized hyaluronic acid (OHA), 3,3'-dithiobis-(propionohydrazide) (DTP) were used as raw materials for the synthesis of hydrogels with excellent properties as carriers for drug release. The hydrogels were prepared by a simple "one-pot" method without external stimuli on the basis of interactions between formed dynamic covalent bonds (imine bonds, acylhydrazone bonds, disulfide bonds) and hydrogen bonds. The hydrogels had rapid self-healing properties, with a self-healing rate of 96 % after 30 min, as well as good pH responsiveness and excellent cytocompatibility (up to 98 % cell survival). The compressive stress of the hydrogels reached 423 kPa. Moreover, a representative drug (acetylsalicylic acid) demonstrated sustained release in the hydrogels (>72 h). The drug release behaviour was shown to be consistent with the Fick diffusion mechanism by kinetic modelling. Collectively, the findings demonstrate that the QCMCS + OHA + DTP injectable self-healing hydrogels are a potential material for the construction of pH-controlled drug delivery platforms., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

Photoinduced metal-free ATRP has been successfully applied to fabricate thermo-responsive cellulose graft copolymer (PNIPAM- g -Cell) using 2-bromoisobuturyl bromide-modified cellulose as the macroinitiator. The polymerization of N-isopropylacrylamide (NIPAM) from cellulose was efficiently activated and deactivated with UV irradiation in the presence of an organic-based photo-redox catalyst. Both FTIR and 13 C NMR analysis confirmed the structural similarity between the obtained PNIPAM- g -Cell and that synthesized via traditional ATRP methods. When the concentration of the PNIPAM- g -Cell is over 5% in water, it forms an injectable thermos-responsive hydrogel composed of micelles at 37 °C. Since organic photocatalysis is a metal-free ATRP, it overcomes the challenge of transition-metal catalysts remaining in polymer products, making this cellulose-based graft copolymer suitable for biomedical applications. In vitro release studies demonstrated that the hydrogel can continuously release DOX for up to 10 days, and its cytotoxicity indicates that it is highly biocompatible. Based on these findings, this cellulose-based injectable, thermo-responsive drug-loaded hydrogel is suitable for intelligent drug delivery systems.

Conductive hydrogels have received increasing attention in the field of wearable electronics, but they also face many challenges such as temperature tolerance, biocompatibility, and stability of mechanical properties. In this paper, a double network hydrogel of MXene/TEMPO bacterial cellulose (TOBC) system is proposed. Through solvent replacement, the hydrogel exhibits wide temperature tolerance (-20-60 °C) and stable mechanical properties. A large number of hydrogen bonds, MXene/TOBC dynamic three-dimensional network system, and micellar interactions endow the hydrogel with excellent mechanical properties (elongation at break ~2800 %, strength at break ~420 kPa) and self-healing ability. The introduction of tannic acid prevents the oxidation of MXene and the loss of electrical properties of the hydrogel. In addition, the sensor can also quickly (74 ms) and sensitive (gauge factor = 15.65) wirelessly monitor human motion, and the biocompatibility can well avoid the stimulation when it comes into contact with the human body. This series of research work reveals the fabrication of MXene-like flexible wearable electronic devices based on self-healing, good cell compatibility, high sensitivity, wide temperature tolerance and durability, which can be used in smart wearable, wireless monitoring, human-machine Interaction and other aspects show great application potential., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Inspired by the mussel, tannic acid (TA) was modified onto the surface of self-made cellulose nanofibrils (CNFs) to prepare TA@CNFs, which was introduced into borax crosslinked polyvinyl alcohol (PVA) to prepare PTC double-network hydrogel with self-healing properties. Through the comparative observation of TEM images and infrared spectra before and after tannic acid modification, the formation of TA@CNFs was proved. The introduction of TA@CNFs greatly increases the fracture stress of PTC hydrogel, which is more than 10 times higher than that of PVA hydrogel without TA@CNFs, and has high fracture strain (1723 %). Moreover, PTC hydrogel has the ability of rapid self-healing, which can heal to the original form within two minutes. In addition, the temperature response ability of PTC hydrogel makes it capable of reshaping. The self-adhesion ability of PTC hydrogel enables it to adhere to the human epidermis to detect motion signals, as sensitive and as stable as a flexible sensor., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Pectin-crosslinked gum ghatti hydrogel (PGH) has been synthesized utilizing pectin and gum ghatti through an uncomplicated and inexpensive copolymerization method. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM-elemental mapping), Brunauer-Emmett-Teller (BET), and X-ray photoelectron spectroscopy (XPS) characterization techniques have been employed to determine various structural, chemical and compositional characteristics of fabricated PGH. Three different weight ratios (1:1, 2:1, or 1:2 for pectin and gum ghatti, respectively) were employed to synthesize three distinct types of PGH. Swelling studies has been done to determine the best ratios for PGH fabrication. PGH has been assessed as an adsorbent for the removal of malachite green dye from aqueous solutions. The effects of PGH dosage (100-400 mg/L), dye concentration (10-160 mg/L), pH (2-9 pH), adsorption time (0-480 min), and temperature (25-55 °C) has been examined through batch solutions. According to Langmuir isotherm analysis, the maximum adsorption capacity is 658.1 mg/g. By using pseudo-second-order kinetics and the Freundlich adsorption isotherm, the adsorption process could be well explained. After five consecutive cycles, PGH had an adsorption percentage of 86.917 % for the malachite green dye. It is safe for the environment and may be used to remove malachite green (MG) dye from aqueous solutions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

The unique features of self-healing hydrogels hold great potential for biomedical applications including injectable hydrogels for cancer treatment, procedures for tumor removal or resection. However, the fabrication of durable and multifunctional self-healing hydrogels composed of biocompatible, green building blocks via versatile synthetic methodology continues to pose a significant challenge. Here, we engineered dialdehyde cellulose (DAC, as a macromolecular bio-crosslinker), and electrosterically stabilized nanocrystalline cellulose (ENCC, as a ligand-targeted drug carrier) to facilitate a strategy for the construction of self-healing hydrogels. Benefiting from its high carboxyl group density, ENCC was functionalized with folic acid (FA) using a non-toxic DMTMM coupling agent and loaded with doxorubicin (DOX, a model drug) through electrostatic interactions. A natural self-healing hydrogel was prepared from carboxymethyl chitosan (CCTS) and DAC mixed with DOX-loaded FA-ENCC using dynamic Schiff-base and hydrogen linkages. A combination of active supramolecular and vital covalent junctions led to a soft (storage modulus ∼500 Pa) and durable material, with rapid (< 5 min) reconstruction of molecular structure from fractured and injected to intact forms. The DAC-CCTS hydrogel showed an appreciable loading capacity of ∼5 mg g -1 . Biocompatibility of the hydrogels was evaluated using cell viability and metabolic activity assays, showing lower metabolic activity due to sustained release of its cargo. These materials offer a versatile, sustainable, and green platform for the efficient construction of hydrogels, based on macro- and nano-engineered cellulose, the most abundant and easily accessible biopolymer., Competing Interests: Declaration of competing interest Ashok Kakkar reports financial support was provided by Natural Sciences and Engineering Research Council of Canada., (Copyright © 2024 Elsevier B.V. All rights reserved.)

β-Cyclodextrin (β-CD) is often used as a drug carrier for biomedical materials due to its unique cavity structure. Herein, β-CD was modified by acryloyl chloride and further copolymerized with N -isopropylacrylamide (NIPAM) and acrylic acid (AA) to obtain PNIPAM -co- β-CD-AC. The results showed that the critical phase transition temperature of PNIPAM/β-CD-AC could be controlled at 19 °C, and the fast sol-gel phase transition was realized in 2-10 s. The hydrophobic drug carried in this hydrogel can constantly be released for more than 6 days at pH values (pH 5.5-8), and the duration may match the recovery of the wound. As a dressing hydrogel, its rapid gel formation and inversion as well as shear-thinning behavior prevent secondary wound damage. The β-CD-based hydrogel also has good biocompatibility and antioxidant properties, which provide a good potential choice for wound dressings, especially for exposed wounds in winter.

Nowadays, the combined knowledge and experience in biomedical research and material sciences results in the innovation of smart materials that could efficiently overcome the problems of microbial contaminations. Herein, a new drug delivery platform prepared by grafting sodium alginate with β-carboxyethyl acrylate and acrylamide was described and characterized. 9-Aminoacridine (9-AA), and kanamycin sulfate (KS) were separately loaded into the hydrogel in situ during graft polymerization. The grafting efficiency for the resulting hydrogels was 70.01-78.08 %. The chemical structure of the hydrogels, thermogravimetric analysis, and morphological features were investigated. The swelling study revealed that the hydrogel without drugs achieved a superior swelling rate compared to drug-loaded hydrogels. The hydrogel tuned the drug-release rate in a pH-dependent manner. Furthermore, the antibacterial study suggested that the hydrogels encapsulating 9-AA (88.6 %) or KS (89.3 %) exhibited comparable antibacterial activity against Gram-positive and Gram-negative bacterial strains. Finally, the cytocompatibility study conducted on normal lung cell line (Vero cells) demonstrated neglectable to tolerable toxicity for the drug-loaded hydrogel. More interestingly, the cell viability for the blank hydrogel was 92.5 %, implying its suitability for biomedical applications., Competing Interests: Declaration of competing interest The authors declare no conflict of interest., (Copyright © 2023 Elsevier B.V. All rights reserved.)

The continuous supply of hydrogen sulfide (H 2 S) gas at high concentrations to tumors is considered a promising and safe strategy for tumor therapy. However, the absence of a durable and cost-effective H 2 S-producing donor hampers its extensive application. Sulfate-reducing bacteria (SRB) can serve as an excellent H 2 S factory due to their ability to metabolize sulfate into H 2 S. Herein, a novel injectable chondroitin sulfate (ChS) hydrogel loaded with SRB (SRB@ChS Gel) is proposed to sustainably produce H 2 S in tumor tissues to overcome the limitations of current H 2 S gas therapy. In vitro, the ChS Gel not only supports the growth of encapsulated SRB, but also supplies a sulfate source to the SRB to produce high concentrations of H 2 S for at least 7 days, resulting in mitochondrial damage and immunogenic cell death. Once injected into tumor tissue, the SRB@ChS Gel can constantly produce H 2 S for >5 days, significantly inhibiting tumor growth. Furthermore, such treatment activates systemic anti-tumor immune responses, suppresses the growth of distant and recurrent tumors, as well as lung metastases, meanwhile with negligible side effects. Therefore, the injectable SRB@ChS Gel, as a safe and long-term, self-sustained H 2 S-generating factory, provides a promising strategy for anti-tumor therapy., Competing Interests: Declaration of Competing Interest The authors declare no conflict of interest., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Self-healing hydrogels have received considerable attention as a promising material for flexible electronic devices given their mechanical durability and structurally tunable properties. In this study, a highly stretchable self-healing hydrogel with dual cross-linking network was developed via borate ester bonds generated by polyvinyl alcohol and borax, and acylhydrazone bonds formed by aldehyde nanocellulose with adipic acid dihydrazide-modified alginate. Compared with the single network hydrogel composed of polyvinyl alcohol and borax, the introduction of dynamic acylhydrazone bonds greatly increases the flexibility of the hydrogel. The elongation rate increased from 480 % to approximately 1440 %, and the self-healing efficiency increased from 84.6 % to 92.7 % after healing for 60 min at ambient temperature without any stimulus. Moreover, the longer the self-healing time, the more evident the self-healing effect of the acylhydrazone bonds. In addition, electrical measurements confirmed a wide working strain range (ca.1000 %), durability, and reliability. Once assembled as a strain sensor, the hydrogel is able to monitor both large and subtle human motions. Besides, this hydrogel exhibited desirable biocompatibility, as demonstrated by in vitro cytotoxicity towards NIH 3T3 cells. These integrated properties make this nanocomposite hydrogel a promising candidate for future applications as green, flexible, and smart sensors., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Ionic conductive hydrogels have been widely used for sensor, energy storage and human-machine interface. To address the problems of the traditional ionic conductive hydrogels fabricated with the soaking method, such as the lack of frost resistance, poor mechanical properties, time-consuming and chemical-wasting, herein, a multi-physics crosslinking reinforced strong, anti-freezing and ionic conductive hydrogel sensor is fabricated utilizing the tannin acid-Fe 2 (SO 4 ) 3 through the simple one-pot freezing-thawing process at low electrolyte concentration. The results show that the P 10 C 0.4 T 8 -Fe 2 (SO 4 ) 3 (PVA 10% CNF 0.4% TA 8% -Fe 2 (SO 4 ) 3 ) displayed better mechanical property and ionic conductivity due to hydrogen bonding and coordination interaction. The tensile stress reaches up to 0.980 MPa (570 % strain). Moreover, the hydrogel presents excellent ionic conductivity (0.220 S⋅m -1 at room temperature), anti-freezing performance (0.183 S⋅m -1 at -18 °C), large gauge factor (1.75), excellent sensing stability, repeatability, durability and reliability. This work paves a way for preparing mechanical strong and anti-freezing hydrogel based on multi-physics crosslinking with one-pot freezing-thawing process., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Hydrogel with 3D networks have shown great potential for ion transportation and energy conversion. However, the micron size pores of hydrogel greatly limit the ion selectivity and energy conversion performance. Here, we report a bacterial cellulose (BC) derived hydrogel membrane with double-network (DN) and tailored ion transport channels by rationally filling acrylic acid (AAc)-co-acrylamide (AAm)-co-methyl methacrylate (MMA) polymers into BC hydrogel micropores. Fabricated AAM/BC DN hydrogel membrane displays a unique hierarchical interconnected porous structure and 3D cation transport channels. From the results, the maximum power density reached up to 7.63 W·m -2 at 50-fold salinity gradient under alkaline conditions (pH 11). Interestingly, the power density of 45.5 W·m -2 was achieved through acid-base neutralization reaction. Furthermore, hydrogel successfully obtained a power density of 28.4 W·m -2 from a mixed system of paper black liquor wastewater/seawater. The results of this investigation suggested the enormous potential of BC-based nanofluidic membrane in sustainable osmotic energy conversion., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

In this study, the dielectric behavior of polyanionic electrically conductive superabsorbent hydrogel based on sodium alginate-g-poly(AM-co-ECA-co-AMPS) was investigated by broadband dielectric spectroscopy (BDS). The dielectric spectra obtained from -70 to 70 °C showed a superposition of three distinctive processes, electrode polarization, charge carrier's transport, and a molecular relaxation process. These dynamic processes were further analyzed along with the effect of both temperature and reduced graphene oxide (rGO) content. The development of a clear electrochemical double layer (ECDL) at the electrode/hydrogel interface strongly supports its possible application in supercapacitors' forms of energy storage. TGA, DSC, rheology, and electrochemical properties were studied. Furthermore, when the composite hydrogel with rGO content of 2.5 % was assembled into a symmetric supercapacitor, it displayed a specific capacitance of 756 F.g -1 at 1 A.g -1 and 704 F.g -1 after 5000 cycles with high capacitance retention of 93.2 %. The superior conductivity and porous structure of the rGO composite hydrogel are credited with the hydrogel's excellent electrochemical capabilities., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Liquid metal (LM) nanodroplets and MXene nanosheets are integrated with sulfonated bacterial nanocellulose (BNC) and acrylic acid (AA). Upon fast sonication, AA polymerization leads to a crosslinked composite hydrogel in which BNC exfoliates Mxene, forming organized conductive pathways. Soft conducting properties are achieved in the presence of colloidally stable core-shell LM nanodroplets. Due to the unique gelation mechanism and the effect of Mxene, the hydrogels spontaneously undergo surface wrinkling, which improves their electrical sensitivity (GF = 8.09). The hydrogels are further shown to display interfacial adhesion to a variety of surfaces, ultra-elasticity (tailorable elongation, from 1000 % to 3200 %), indentation resistance and self-healing capabilities. Such properties are demonstrated in wearable, force mapping, multi-sensing and patternable electroluminescence devices., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier Ltd.)

As the typical bio-macromolecules, cellulose and its derivates are widely studied due to the fact that they are green and renewable resources in nature. In this work, intelligent temperature-pH sensitive nanohydrogels consisting of nanocellulose, thermal responsive monomer (N-isopropylacrylamide, NIPAM), and pH responsive monomer (acrylic acid, AA; acrylamide, AM) were prepared [NFC-g-(AA/AM)]-g-NIPAM, the [NFC-g-(AA/AM)]-g-NIPAM was characterized by FTIR, scanning electron microscope (SEM), thermogravimetric analysis (TGA) and automatic gas adsorption analysis (BET). The results showed that the copolymerization of AA, AM and NIPAM were carried out successfully. The specific surface area, total pore volume, average pore diameter and thermal stability of the modified nano-cellulose were increased. In addition, the as-prepared nanohydrogels with 5-fluorouracil (5-FU) released more 5-FU at 40 °C and acidic condition compared to the room temperature and neutral pH, showing the characteristics of the temperature-PH dual response functionalization. The [NFC-g-(AA/AM)]-g-NIPAM have been proved to be the promising drug release nanohydrogels towards 5-FU, and the valuable findings might provide an idea for maximizing the potential of the nanocellulose-based nanohydrogels for the application of environmental pollution control., Competing Interests: Declaration of competing interest The authors declare that they have no conflict of interest., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Hydrogels with fascinating adhesion have been demonstrated great potential in various applications. However, most hydrogels lose their adhesion in wet or underwater environments due to the influence of interfacial water. Inspired by mussel, an underwater adhesive hydrogel was facilely fabricated by introducing electrostatic interactions, which consisted of poly (acrylic acid) (PAA), quaternized xylan (QAX) and tannic acid (TA). In this hydrogel, -COO - from PAA, -N + (CH 3 ) 3 from QAX and catechol group from TA resembled amino acids with negative and positive charges and 3,4-dihydroxyphenylalanine units in mussel, which endowed the hydrogels with great underwater adhesion through multiple interactions. Notably, acrylic acid (AA) played a key role in the dispersion of the system. QAX, a biomass derived from plants with excellent properties, worked with PAA to construct hydrogel networks. The resultant hydrogels exhibited excellent mechanical properties including remarkable stretchability (>4000 %) and compressibility. Moreover, the hydrogels had superior UV-blocking (~99.96 %), and showed good adhesion both in air and underwater. The hydrogels can be exploited as a wearable sensor to monitor human motions and even subtle motions, which have the potential to be explored in human health monitoring., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Recent advances in the area of hydrogel synthesis have been directed to enhance the mechanical properties and biocompatibility, which are critical in their use as functional biomaterials. In this work, a green and facile method is introduced to produce a hydrogel based on xylan, a plant-based heteropolysaccharide, that is shown to successfully form hydrogen-bonded, semi-interpenetrating polymer networks with polyvinyl alcohol. Upon crosslinking with sodium trimetaphosphate, the obtained hydrogels achieved an exceptional compressive strength (up to 84.2 MPa at a fracture strain of 90 %), which surpasses any polysaccharide-based hydrogels reported so far. The hydrogels were further shown to have high degradation temperature (350-370 °C), to be mechanically resilient with a form and creep recovery of 95 % (78 % stress after 1000 cycles under 30 % strain) and 98 % in height, respectively. All materials used in the preparation of the hydrogels were non-toxic and biocompatible, which makes the synthesized hydrogels suitable potential candidates for soft-tissue engineering and biomedical applications., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

In this study, the anti-freezing conductive hydrogel electrolytes with outstanding mechanical properties were synthesized by a facile and feasible method. The mechanical and anti-freezing properties of the synthesized polyacrylamide/lithium lhloride/water soluble cellulose acetate (PAM/LiCl/WSCA) hydrogels are significantly enhanced with the addition of WSCA and LiCl. The tensile strength and toughness of the gels were gradually increased to 341 KPa and 1.2 MJ/m 3 , respectively. The hydrogel electrolyte can remain soft and flexible at -80 °C, displaying certain elasticity and electrical conductivity. In addition, the super-capacitor assembled with PAM/LiCl/WSCA hydrogel as electrolyte showed excellent stability in capacitance retention after 500 times of folding cycles and 10,000 times of charge and discharge tests. The capacitor still maintains 64.64 % of its capacity at -40 °C. This facile strategy to fabricate anti-freezing conductive hydrogel electrolyte provides a new idea and way to the application of hydrogels as electrolytes in extreme cold environments., (Copyright © 2021. Published by Elsevier Ltd.)

Electrochemical conductive hydrogels are being extensively explored in the fabrication of portable batteries and high-performance supercapacitors. Herein, the rational design of a new polyanionic electrically conductive hydrogels based on sodium alginate-g-poly(AM-co-ECA-co-AMPS) are described. rGO was incorporated into the hydrogel during the polymerization process generating rGO@ sodium alginate-g-poly(AM-co-ECA-co-AMPS) composite hydrogels to study the impact of rGO on the performance of the hydrogels. FT-IR, XRD, and SEM-EDX characterized the chemical composition, crystalline, and morphological structure of the new synthesized hydrogels. The electrochemical performance of as-synthesized hydrogels was investigated by cyclic voltammetry, galvanostatic, charge-discharge rate, and electrochemical impedance spectroscopy. The supercapacitor performance for ECH2.5 composite hydrogel showed a capacitance of 753 F. g -1 at 1 A. g -1 with good rate capability and cycling stability up to 5000 cycles. Thus, ECH2.5 hydrogel is a good candidate as electrode material in supercapacitor applications., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

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.)

With the rapid development of flexible wearable devices, various polymer hydrogels have gained immense progress due to their adjustable mechanical properties, high conductivity, super sensitivity, good biocompatibility and adaptable wearability. Lignosulfonate (LS), generating from the sulfite pulping industry, was emerged as a promising filler in polymer hydrogels with great potential for multifunctional wearable electronics. Herein, we comprehensively review the latest research progress associated with LS-based hydrogels. Firstly, the function mechanism of lignosulfonate in diverse polymer hydrogels was introduced in detail. Then, the rational design strategies of LS filled multifunctional hydrogels was summarized as toughening filler, adhesive agent, conductive filler dispersant, UV protectant and catalysts. Finally, the future development of LS filled hydrogel for flexible wearable electronics was proposed., (Copyright © 2022. Published by Elsevier B.V.)

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.)

The human digestive and absorption system has a specific pH environment, which makes it difficult to for accurate drug-release. Zwitterionic hydrogel, as a kind of drug carrier, is a feasible response strategy. In this work, a facile method was employed to prepare a series zwitterionic hydrogels composed of BC and chitosan. The composite gels could in-situ formed via Schiff's base reaction between partially oxidated bacterial cellulose and chitosan which exhibited relatively well mechanical properties. Besides, the rich amino and carboxyl groups endowed the hydrogels with excellent pH responsive performance. The minimum swelling rate of the hydrogels appeared at pH 3.5-pH 5.0. In lower or higher pH solutions, the swelling rate was greatly increased. The drug (naproxen) loading of the hydrogels was above 110 mg/g. The release amount of naproxen in the simulated gastric juice was less than intestinal fluid with the sustained release time exceeded 24 h. Through kinetic simulation analysis, the drug release behavior is in accordance with zero-order release model. Such kind of composite hydrogel is suggested to be a potential drug carrier for clinical therapy., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Conductive hydrogel flexible sensors have attracted considerable research interest because of their good conductivity, flexibility, and biocompatibility. However, conventional hydrogels suffer from dehydration under ambient environments and freezing at low temperatures. Herein, we prepared a chitin/polyacrylamide organohydrogel with highly stretchable, anti-freezing, and anti-drying properties. This organohydrogel was creatively prepared by one-step radical polymerization in the chitin and calcium chloride/methanol (Ca solvent) aqueous solution. Benefiting from the chitin/Ca solvent system, the organohydrogel shows relatively high stretchability (improve ~5 times), excellent anti-freezing (up to -80 °C) upon long-term storage, and anti-drying (67 days under normal environment) performance. What's more, the reversible noncovalent bonds in the organohydrogel endow it with repeatable multi-purpose adhesion and rapid self-healing, while the abundant free ions grant it good conductivity to be a flexible sensor. Therefore, it is promising that this chitin-based conductive organohydrogel with multifunctionality would provide wide application scopes of flexible electronic devices., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Conductive hydrogels have emerged as promising material candidates for multifunctional strain sensors, attributed to their similarity to biological tissues, good wearability, and high accuracy of information acquisition. However, it is difficult to simultaneously manufacture conductive hydrogel-based multifunctional strain sensors with the synergistic properties of reliable healability for long-term usage and environmental degradability/recyclability for decreasing the electronic waste. This work reports a facile strategy to engineer a self-healing, recyclable and conductive strain sensor by virtue of molecular-level multi-dynamic interactions (MMDIs) including Schiff base complexes, hydrogen bonds, and coordination bonds, which were fabricated using a dialdehyde TEMPO (2,2,6,6-tetramethylpiperidine-1-oxyl)-oxidized nanofibrillated cellulose (DATNFC) pre-reinforced gelatin nanocomposite hydrogel (gelatin/DATNFC hydrogel, GDH) followed by dipping in an Fe 3+ aqueous solution. The MMDI strategy allows synchronous regulation of both bulk and interfacial interactions to obtain exciting properties that outperform those of conventional hydrogels, including extraordinary compressive stress (1310 kPa), intriguing self-healing abilities, and remarkable electrical conductivity. With these outstanding merits, the as-prepared gelatin/DATNFC/Fe 3+ hydrogel (GDIH) is developed to be a multifunctional strain sensor with appealing strain sensitivity (GF = 2.24 under 6% strain) and compressive sensitivity ( S = 1.14 kPa -1 under 15 kPa), which can be utilized to manufacture electronic skin and accurately discern subtle bodily motions, handwriting and personal signatures. Notably, this GDIH-based sensor also exhibited reliable self-healing properties for long-term usage, environmental degradability and complete recyclability for decreasing the electronic waste. In consideration of the extremely facile preparation process, biocompatibility, satisfactory functionalities, remarkable self-healing properties and recyclability, the emergence of the GDIH-based sensor is believed to propose a new strategy for the development of sustainable-multifunctional strain sensors and healthcare monitoring.

Hydrogels are functional materials that are similar to human skin and have received much attention in recent years for biomedical applications. However, the preparation of nontoxic, highly adhesive, and antimicrobial hydrogels in an efficient way remains a great challenge. Inspired by adhesive mussel foot proteins (mfps) which consist of abundant catecholic amino acids and lysine (Lys) residues, gallic acid-modified ε-poly-L-lysine (EPL/GA) was synthesized, and an active functional monomer (AA-EPL/GA) was then created through a reaction with acrylic acid (AA). The polymerization of AA-EPL/GA occurred rapidly (30-160 s) under blue light (λ = 405 nm) irradiation to produce a biomimetic PAA-EPL/GA hydrogel under mild conditions. The biomimetic pyrogallol-Lys distribution endowed the PAA-EPL/GA hydrogels with superior adhesion in humid environments (with an adhesive strength of 50.02 kPa toward wet porcine skin) and tunable mechanical and self-healing properties. Additionally, the PAA-EPL/GA hydrogels exhibited outstanding antibacterial ability due to the inherent characteristics of GA and EPL. In a mouse model, PAA-EPL/GA adhered firmly around the wound tissues. Photographs of the wound and the histological results demonstrated the ability of the hydrogel to promote wound healing, control wound infection, and suppress scar formation. Moreover, the hydrogel had a good hemostatic effect on liver bleeding. Our results highlighted the promising application potential of GA-based hydrogels, which were easily, harmlessly, and efficiently fabricated by blue light irradiation., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Herein, we innovatively synthesized an ionic conductive PVA/LNP hydrogel with integrated excellent mechanical, anti-freezing, moisturizing, transparent and UV-shielding performances via incorporating nanolignin (also called lignin nanoparticle, LNP) and aluminum chloride (AlCl 3 ) into polyvinyl alcohol (PVA) matrix containing ethylene glycol/water (EG/H 2 O) binary solvent. The rigid porous network structure was well constructed by the hydrogen bond interactions among the evenly distributed LNP and PVA chains, thus providing abundant ion transport channels, which attributed to the outstanding ionic conductivity (up to 1.35 × 10 -2  S/m, at -24 °C) with improved mechanical strength and flexibility. The tensile strength and elongation at break of PVA/LNP hydrogel were greatly increased from 574.6 kPa and 363.7% to 1241.4 kPa and 589% at the addition of 0.35% LNP, respectively. In addition, the UV-resistance ability was 95% at 365 nm, while the transparency was 74% at 550 nm. The binary solvent of EG and H 2 O ensured long-term moisturizing capability (10 days) of the hydrogel at 35 °C and 60 RH%, as well as possessing superior anti-freezing performance over the temperature range of -62.6 to 24 °C. As a result, the fabricated PVA/LNP hydrogel was successfully used as strain sensor for detecting diverse human motions and electrophysiological signals., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Flexible hydrogels with integration of excellent mechanical and electrical properties are well suited for applications as wearable electronic sensors, and others. Self-adhesion is an important feature of wearable sensors. However, the usual isotropic- adhesion hydrogels have the drawback of poor anti-interference, which negatively affects their applications. In this study, we developed asymmetric-adhesion and tough lignin reinforced hydrogels in a facile two-step process: 1) PAA hydrogels, with lignin as the binder and conductive filler, were first prepared; 2) the asymmetric-adhesion property was imparted to lignin reinforced hydrogel by simple soaking of the top portion of the hydrogel in CaCl 2 solution. The as-obtained asymmetric-adhesion lignin reinforced hydrogel was assembled into a wearable sensor, which shows excellent anti-interference and accurate and stable collections of sensing signals, with its gauge factor (GF) of 2.51 (in the strain range of 0-51.5%). In addition, the tough hydrogel is capable of generating electricity upon moist air sweeping through it, showing excellent energy conversion capabilities, with open-circuit voltage of as high as 306.6 mV. These results provided new prospects for the application of polyelectrolyte hydrogel materials in the fields of wet-to-electric conversion and wearable electronic sensors., (Copyright © 2021. Published by Elsevier B.V.)

Hydrogels have found applications in many different fields. However, poor mechanical properties, such as low elasticity and lack of rapid recovery under large deformation, can severely limit their applications. In this study, we developed lignin reinforced hydrogels made of calcium ion containing ternary polymers (lignosulfonate (LS), alginate (Alg), and polyacrylic acid (PAA)). The resultant hydrogel has excellent elasticity, rapid self-recovery, and multi-functionalities. The covalent PAA network acts as the elastic scaffold of hydrogel, while calcium bridging networks of LS, Alg, and PAA, as well as the strong hydrogen bonding network in the system, function as sacrifice bonds to dissipate energy and transfer stress. The PAA/LS/Alg/Ca hydrogels exhibit rapid and durable elastic recovery ability under large deformation with the highest compressive stress of 835 kPa (95% strain), highest tensile fracture stress of 357 kPa, and highest tensile strain of 1144%. In addition, these tough hydrogels show UV resistance, self-healing, antifreeze, and excellent electro-conductivity. When assembled into a strain sensor, stable and reliable electrical responses with 375 ms response time are demonstrated. The PAA/LS/Alg/Ca hydrogel strain sensors can monitor human movements with responsive and accurate physiological signals. These results support the conclusion that the PAA/LS/Alg/Ca hydrogel strain sensors have great application potential in flexible wearable electronics and smart devices., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Recently, versatile hydrogels with multifunctionality have been widely developed with emerging applications as wearable and implantable devices. In this work, we reported novel versatile hydrogels by self-catalyzing the gelation of an interpenetrating polymer network consisting of acrylic acid (AA) monomers and GA-modified collagen (GCOL) in situ decorated silver nanoparticles (AgNPs). The resultant hydrogel, namely AgNP@GCOL/PAA, has many desirable features, including good mechanical properties (such as 123 kPa, 916%, and 1961 J m -2 for the fracture stress, strain and tearing energy) that match with those of animal skin, excellent self-healing performance, favorable conductivity and strain sensitivity as a flexible biosensor, and excellent antibacterial and anti-UV properties, as well as the strong adhesiveness on skin. Moreover, AgNP@GCOL/PAA showed excellent biocompatibility via in vitro cell culture. Remarkably, AgNP@GCOL/PAA displayed superior hemostatic properties with sharply decreasing blood loss for a mouse liver incision, closely related to its strong self-adhesion which produced anchoring strength to the bleeding site and thus formed a network barrier with liver tissue. This study provides new opportunities for the facile preparation of widely used multifunctional collagen-based hydrogels based on a simple pyrogallol-Ag system.

Polydopamine (PDA)-based self-adhesive hydrogel sensors are extensively explored but it is still a challenge to construct PDA-based hydrogels by free radical polymerization. Herein, a new approach to construct self-adhesive hydrogels by conducting free radical polymerization in both aqueous phase and micelle phase is developed. The following two-phase polymerization processes account for the formation of the self-adhesive hydrogels. The first one is the polymerization of acrylamide (AM) and dopamine (DA) in aqueous phase to form adhesive component PAM-PDA (PAM, polyacrylamide; PDA, polydopamine). The second one is the polymerization of hydrophobic monomer 2-methoxyethyl acrylate (MEA) in micelles of an amphiphilic block copolymer Pluronic F127 diacrylate (F127DA). The poly(2-methoxyethyl acrylate) (PMEA) networks help to maintain the high robustness of the hydrogel. Because PMEA and PDA form in relatively separated phases, the inhibition effect of PDA on the free radical polymerization process of PMEA is weakened. Based on this mechanism, mechanically strong and adhesive hydrogels are achieved. The introduced ions during preparation process, such as Na + , OH - and K + , endow the resulting hydrogels ionic conductivity. Resistive strain sensor of the hydrogel achieves a high gauge factor (GF) of 5.26, a response time of 0.25 s and high sensing stability. Because of the adhesiveness, such hydrogel sensor can be applied as wearable sensors in monitoring various human motions. To further address the freezing and drying problems of the hydrogels, organohydrogels are constructed in glycerol-water mixed solvent. The organohydrogels exhibit outstanding anti-freezing property and moisture retention ability, and their adhesiveness is well maintained in subzero conditions. Capacitive pressure sensors of the organohydrogels possessing a GF of 2.05 kPa -1 , high sensing stability and reversibility, are demonstrated and explored in monitoring diverse human motions., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier Inc. All rights reserved.)

Recently, great efforts have been devoted to developing conductive adhesive hydrogels to meet the needs of various applications. However, grand challenges remain in achieving anisotropic hydrogels simultaneously featuring multiple properties using natural polymers and renewable resources. Here, a cellulose-based conductive hydrogel with strong, ultrastretchable, and adhesive properties is prepared via a simple magnetic field-induced strategy. This strategy involves the formation of a suspension mixture with well-oriented cellulose-polydopamine nanocomposites under magnetic fields, followed by rapid orientation via covalent crosslinking. The tensile strength of the oriented hydrogel in longitudinal direction is ~0.22 MPa, which is ~1.4 times higher than that in radial direction. Moreover, the hydrogel shows good cyclic loading-unloading ability, high conductivity (6.9 ± 0.6 S m -1 ), and strong adhesion (71 kPa). The hydrogel also shows significant anisotropic properties and made it a versatile platform for wearable sensors to monitor large and subtle human motion in the foreseeable future., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

In recent years, smart-responsive nanocellulose composite hydrogels have attracted extensive attention due to their unique porous substrate, hydrophilic properties, biocompatibility and stimulus responsiveness. At present, the research on smart response nanocellulose composite hydrogel mainly focuses on the selection of composite materials and the construction of internal chemical bonds. The common composite materials and connection methods used for preparation of smart response nanocellulose composite hydrogels are compared according to the different types of response sources such as temperature, pH and so on. The response mechanisms and the application prospects of different response types of nanocellulose composite hydrogels are summarized, and the transformation of internal ions, functional groups and chemical bonds, as well as the changes in mechanical properties such as modulus and strength are discussed. Finally, the shortcomings and application prospects of nanocellulose smart response composite hydrogels are summarized and prospected., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Smart hydrogels responsive to minimally invasive near-infrared (NIR) light have great potential in localized drug delivery for cancer treatment, but they still show some limitations such as low photothermal conversion, poor photothermal stability, and improper temperature range in biomedical applications. In this paper, the two-dimensional MXene nanosheets with high photothermal conversion efficiency as well as photothermal stability was firstly prepared, then the MXene nanosheets and the therapeutic drug were embedded in the low-melting-point agarose hydrogel network to fabricate the drug-loaded MXene/agarose hydrogel (MXene@Hydrogel). With the addition of low concentration of MXene (20 ppm), the MXene@Hydrogel could quickly rise to 60 °C under NIR irradiation and melt to release the encapsulated drugs. Importantly, the drug on/off release and the kinetics could be easily controlled with varied agarose concentration, MXene concentration, light intensity, and exposure time. In addition, the drug doxorubicin retained the anticancer activity after released from the MXene@Hydrogel network under NIR irradiation. With the excellent biocompatibility, the newly fabricated NIR-responsive MXene@Hydrogel offers a novel way for the development of smart hydrogel-based drug delivery system for localized cancer treatment., (Copyright © 2021. Published by Elsevier B.V.)

Hydrogels derived from natural polymers have received great attention, but their practical applications are severely hindered by the relatively poor mechanical properties. In this work, cellulose nanofibril (CNF) was used as a crosslinker to reinforce the sodium alginate (SA)/chitosan (CS) hydrogels for drug sustained release. The CNF was prepared via a combined process of ball milling and deep eutectic solvents (DESs) pretreatment and characterized using SEM, FT-IR, and XRD. Furthermore, the microstructure, mechanical/biological properties and swelling performance of SA/CS/CNF hydrogels were investigated. Results showed that 1.0 wt% CNF addition led to the increases of 23.6% in storage modulus and 54.4% in loss modulus for the SA/CS/CNF hydrogels, indicating that CNF addition was effective in reinforcing the three-dimensional entangled networks of the hydrogels. Moreover, the presence of CNF was found to weaken the swelling performance of SA/CS/CNF hydrogels. When the synthesized SA/CS/CNF hydrogel with 1.0 wt% CNF was applied as a carrier for drug release, 50.8% reduction in the release rate in simulated gastric juice was achieved, demonstrating its outstanding sustained release properties. This work suggested that CNF might be conducive to enhancing the properties of SA/CS hydrogels, which can serve as an ideal polymeric carrier for drug release., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Purpose: TEMPO-oxidized nanofibrillated cellulose (TONFC) originating from an agricultural waste (sugar cane) was utilized to prepare injectable in-situ forming hydrogel scaffolds (IHS) for regenerative medicine., Methods: TONFC was prepared and characterized for its morphology and chemical structure using TEM and FT-IR, respectively. The cold method was applied to prepare hydrogels. Various concentrations of poloxamer 407 were added to the prepared TONFC (0.5%w/w). Different sources of calcium, Fujicalin ® (DCP) or hydroxyapatite (TCP), were used to formulate the aimed calcium-enriched raloxifene hydrochloride-loaded IHS. Gelation temperature, drug content, injectability and in-vitro drug release were evaluated along with the morphological characters. Cytocompatibility studies and tissue regeneration properties were assessed on Saos-2 cells., Results: TEM photograph of TONFC showed fibrous nanostructure. The selected formulation "Ca-IHS4" composed of TONFC+15% P407+10% TCP showed the most prolonged release pattern for 12 days with the least burst effect (about 25% within 24 h). SEM micro-photographs of the in-situ formed scaffolds showed a highly porous 3D structure. Cytocompatibility studies of formulation "Ca-IHS4" revealed the biocompatibility as well as improved cell adhesion, alkaline phosphatase enzyme activity and calcium ion deposition., Conclusion: The outcomes suggest that Ca-IHS4 presents a simple, safe-line and non-invasive strategy for bone regeneration., Competing Interests: The authors report no conflicts of interest in this work., (© 2021 Kamel et al.)

Ionic conductive hydrogel with multifunctional properties have shown promising application potential in various fields, including electronic skin, wearable devices and sensors. Herein, a highly stretchable (up to 2800% strain), tough, adhesive ionic conductive hydrogel are prepared using cationic nanocellulose (CCNC) to disperse/stabilize graphitic carbon nitride (g-C 3 N 4 ), forming CCNC-g-C 3 N 4 complexes and in situ radical polymerization process. The ionic interactions between CNCC and g-C 3 N 4 acted as sacrificial bonds enabled highly stretchability of the hydrogel. The hydrogel showed high sensitivity (gauge factor≈5.6, 0-1.6% strain), enabling the detection of human body motion, speech and exhalation. Furthermore, the hydrogel based self-powered device can charge 2.2 μF capacitor up to 15 V from human motion. This multifunctional hydrogel presents potential applications in self-powered wearable electronics., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

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.)

It is still a challenge to integrate high sensitivity, mechanical adaptability, and self-powered properties for hydrogels. Herein, we report a conductive polyvinyl alcohol (PVA) hydrogel based on natural nanoclay and cellulose nanofibrils (CNFs). The CNFs and PVA chains could construct a double network structure, resulting in a high mechanical composite hydrogel. Meanwhile, the nanoclay could be well dispersed and immobilized in the network of the hydrogel, thus improving mechanical adaptability of the hydrogel for curved and dynamic surfaces. Moreover, the conductive ions (Al 3+ ) imparted the hydrogel with high conductivity (6.67 S m -1 ) and gauge factor (1.17). Therefore, the composite hydrogel exhibited high sensitivity to tiny pressure changes, enabling recognition of the complicated sounding and handwriting. More importantly, the composite hydrogel possessed self-powered property, which could generate an output voltage of up to 78 mV. In summary, the multi-functional composite hydrogel may have giant applications in artificial electronic skins or wearable devices., (Copyright © 2021 Elsevier Ltd. 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.)

Tissue engineering intends to create functionalized tissues/organs for regenerating the injured parts of the body using cells and scaffolds. A scaffold as a supporting substrate affects the cells' fate and behavior, including growth, proliferation, migration, and differentiation. Hydrogel as a biomimetic scaffold plays an important role in cellular behaviors and tissue repair, providing a microenvironment close to the extracellular matrix with adjustable mechanical and chemical features that can provide sufficient nutrients and oxygen. To enhance the hydrogel performance and compatibility with native niche, the cell-laden hydrogel is an attractive choice to mimic the function of the targeted tissue. Injectable hydrogels, due to the injectability, are ideal options for in vivo minimally invasive treatment. Cell-laden injectable hydrogels can be utilized for tissue regeneration in a noninvasive way. This article reviews the recent advances and future opportunities of cell-laden injectable hydrogels and their functions in tissue engineering. It is expected that this strategy allows medical scientists to develop a minimally invasive method for tissue regeneration in clinical settings. Impact statement Cell-laden hydrogels have been vastly utilized in biomedical application, especially tissue engineering. It is expected that this upcoming review article will be a motivation for the community. Although this strategy is still in its early stages, this concept is so alluring that it has attracted all scientists in the community and specialists at academic health centers. Certainly, this approach requires more development, and a bunch of crucial challenges have yet to be solved. In this review, we discuss this various aspects of this approach, the questions that must be answered, the expectations associated with it, and rational restrictions to develop injectable cell-laden hydrogels.

Long-active conductivity, adhesiveness, and environmental stability are essential in the applications of hydrogel electronics. Integrating different functional materials into one system suffers from compatibility and cost problems. Inspired by the unique o-methoxyl structure in polyphenol lignin and its binding role in plants, catechol lignin (DAL) is constructed by one-step demethylation, which endows the lignin with a mussel-like bioadhesion, good reducibility, as well as a high ultraviolet absorption. The DAL is then applied to reduced graphene oxide, and the products-the oxidized DAL and the reduced graphene oxide mixture (DAL/rGO) is added into a sodium alginate/polyacrylamide (SA/PAM) double network hydrogel. Based on the Schiff base reaction between the quinone of the oxidized DAL and the amino of the skin, the DAL/rGO incorporated hydrogels could stably adhere to the skin, and sensitively respond to physiological signals. In addition, the DAL could provide the hydrogels with long-active sunscreen property when applied to real skin. These DAL based hydrogels have potential for on-skin sensing and outdoor sport equipment., (© 2021 Wiley-VCH GmbH.)

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.)

Mimicking the locomotive abilities of living organisms on the microscale, where the downsizing of rigid parts and circuitry presents inherent problems, is a complex feat. In nature, many soft-bodied organisms (inchworm, leech) have evolved simple, yet efficient locomotion strategies in which reciprocal actuation cycles synchronize with spatiotemporal modulation of friction between their bodies and environment. We developed microscopic (∼100 μm) hydrogel crawlers that move in aqueous environment through spatiotemporal modulation of the friction between their bodies and the substrate. Thermo-responsive poly-n-isopropyl acrylamide hydrogels loaded with gold nanoparticles shrink locally and reversibly when heated photothermally with laser light. The out-of-equilibrium collapse and reswelling of the hydrogel is responsible for asymmetric changes in the friction between the actuating section of the crawler and the substrate. This friction hysteresis, together with off-centered irradiation, results in directional motion of the crawler. We developed a model that predicts the order of magnitude of the crawler motion (within 50%) and agrees with the observed experimental trends. Crawler trajectories can be controlled enabling applications of the crawler as micromanipulator that can push small cargo along a surface.