Polymerizable deep eutectic solvent treated lignocellulose: Green strategy for synergetic production of tough strain sensing elastomers and nanocellulose.

Liquid free ion-conductive elastomers (ICEs) have demonstrated promising potential in various advanced application scenarios including sensor, artificial skin, and human-machine interface. However, ICEs that synchronously possess toughness, adhesiveness, stability, and anti-bacterial capability are still difficult to achieve yet highly demanded. Here, a one-pot green and sustainable strategy was proposed to fabricate multifunctional ICEs by extracting non-cellulose components (mainly lignin and hemicellulose) from lignocellulose with polymerizable deep eutectic solvents (PDES) and the subsequent in-situ photo-polymerization process. Ascribing to the uniform dispersion of non-cellulose components in PDES, the resultant ICEs demonstrated promising mechanical strength (a tensile strength of ~1200 kPa), high toughness (~9.1 MJ m-3), favorable adhesion (a lap-shear strength up to ~61.5 kPa toward metal), conducive stabilities, and anti-bacterial capabilities. With the help of such advantages, the ICEs exhibited sensitive (a gauge factor of ~23.5) and stable (~4000 cycles) performances in human motion and physiological signal detection even under sub-zero temperatures (e.g., -20 °C). Besides, the residue cellulose can be mechanically isolated into nanoscale fibers, which matched the idea of green chemistry.

Lignin reinforced tough, adhesive, and recoverable protein organohydrogels for wearable strain sensing under sub-zero temperatures.

Protein-based hydrogels with promising biocompatibility and biodegradability have attracted considerable interest in areas of epidermal sensing, whereas, which are still difficult to synchronously possess high mechanical strength, self-adhesion, and recoverability. Hence, the bio-polymer lignosulfonate-reinforced gluten organohydrogels (GOHLx) are fabricated through green and simple food-making processes and the following solvent exchange with glycerol/water binary solution. Ascribing to the uniform distribution of lignosulfonate in gluten networks, as well as the noncovalent interactions (e.g., H-bond) between them, the resultant GOHLx exhibit favorable conductivity (∼14.3 × 10-4 S m-1), toughness (∼711.0 kJ m-3), self-adhesion (a maximal lap-shear strength of ∼33.5 kPa), high sensitivity (GF up to ∼3.04), and durability (∼3000 cycles) toward shape deformation, which are suitable for the detection of both drastic (e.g., elbow and wrist bending) and subtle (e.g., swallowing and speaking) human movements even under -20 °C. Furthermore, the GOHLx is also biocompatible, degradable, and recoverable (by a simple kneading process). Thus, this work may pave a simple, green, and cheap way to prepare all-biomass-based, tough, sticky, and recoverable protein-based organohydrogels for epidermal strain sensing even in harsh environments.

Green conversion of delignified sorghum straw and polyethylene glycol into form-stable phase change materials with promising solar energy capture, transition, and storage capabilities.

Phase change materials (PCMs) have attracted considerable attention as a thermal energy management technology for thermal storage. However, achieving high energy-storing abilities, low leakage rates, and solar absorption abilities simultaneously in PCMs remains greatly challenging. This research proposed a green strategy for preparing sorghum straw-based PCMs. By facile delignification and solvothermal process, delignified sorghum straw (DSS) and carbon quantum dots (CQDs) derived from removal lignin are prepared. The obtained PEG@CQDs/DSS possessed considerable reusable stabilities, excellent photo-thermal conversion properties, and thermal energy management capacities due to the delicate micropores and intrinsic noncovalent interactions among components. Especially, the PEG@CQDs-7.5/DSS exhibited superior solar-thermal conversion capabilities (with conducive photo-thermal conversion efficiency ~90.84%), and kept stable after 100 cycles of heating and cooling, in which the melting enthalpy value is ~168.1 J/g (enthalpy efficiency of ~91.11%). In conclusion, the synthesized PCMs showed potential for application in energy-saving and building thermal management.

Amino-grafted Biochar as a Novel Photocatalyst for degradation of high concentration dye.

Photocatalytic degradation of organic pollution by biochar was a sustainable strategy for waste water remediation, nevertheless, it still suffers drawbacks like low efficiency due to the poor photocatalytic properties of pristine biochar. Herein, amino groups were grafted on the edge sites/defects of biochar by Friedel-Crafts acylation to enhance the degradation of high concentration dye solutions. The results suggested that the amino groups played an important role in imparting photocatalytic properties to biochar. Owing to the strong Lewis basicity and electron-donating ability of amino groups, their interaction with oxygen-containing functional groups/aromatic structures in biochar was improved, which enhanced the electron exchange ability of biochar under visible light irradiation, resulting in excellent degradation performances of high concentration RhB (∼10 times faster than ungrafted biochar). In this work, amino-grafted garlic peel biochar delivered a new idea for the future direction of biochar-based photocatalysis in wastewater remediation.

Sustainable Biochar Nanosheets Derived from Sweet Sorghum Residues via Superbase Pretreatment.

Two-dimensional (2D) sheet-like biochar as promising alternatives to graphene nanosheets has gained significant attention in materials science while being highly restricted by its complicated synthetic steps. In this study, the dimethyl sulfoxide/potassium hydroxide (DMSO/KOH) superbase system was first used to pretreat sweet sorghum residues (SS) and then carbonized to prepare sheet-like biochar. Ascribing to the strong nucleophilicity of DMSO/KOH, a synergistic effect was achieved by partially removing non-cellulosic components in SS and swelling the amorphous region of cellulose, leaving more layered cellulose behind (∼46.5 wt %), which was favorable for the formation of 2D biochar nanosheets with high graphitization degrees (∼93.1%). This strategy was also suitable for other biomass fibers (e.g., straw, wood powders, and nuclear shells) to obtain sheet-like biochar. The resulting sheet-like biochar could be compounded with cellulose nanofibers to achieve the structural design of composites and solve the molding problem of biochar, which was beneficial for dyeing wastewater treatment. Thus, this work provides insight into a simple strategy for developing 2D ultrathin sheet-like biochar from sustainable biomass wastes.

Aramid Nanofibers-Reinforced Rhein Fibrous Hydrogels as Antibacterial and Anti-Inflammatory Burn Wound Dressings.

Burn injuries are one of the most devastating traumas. The development of polymer-based hydrogel dressings to prevent bacterial infection and accelerate burn wound healing is continuously desired. Mechanical strong hydrogels that encapsulated antibacterial drugs have gained increasing attention. Herein, aramid nanofibers (ANFs)-reinforced rhein fibrous hydrogels (ANFs/Rhein) were fabricated through a one-pot procedure to serve as a possible treatment for the Staphylococcus aureus-infected burn wound. ANFs preserved the highly aligned backbones and the mechanical properties of Kevlar, and its combination with an antibacterial drug rhein produced a composite hydrogel that possesses favorable physicochemical properties including appropriate mechanical strength, high water holding capacity, satisfactory antibacterial efficiency, and excellent biocompatibility. As wound dressings, ANFs/Rhein hydrogels provided a moist environment for the wound site and released antibacterial drugs continuously to improve the wound healing rate by efficiently restraining bacterial infection, reducing inflammation, enhancing collagen deposition, and promoting the formation of blood vessels, in this way to offer a potential treatment strategy for bacteria-associated burn wound healing.

Silk sericin stabilized proanthocyanidins for synergetic alleviation of ulcerative colitis.

Silk sericin (SS) has become a noticeable drug nanocarrier due to its excellent biocompatibility and bioactivity. To further extend the application of SS, a facile one-step process was constructed to fabricate SS-stabilized-drug composites. Various insoluble drugs can be encapsulated into SS with high loading amount, and showed good dispersity in aqueous solution. For example, proanthocyanidins (PAC), a natural polyphenol with initial antioxidant and anti-inflammatory effects, can be loaded on SS to form SS/PAC composites. The SS/PAC can disperse uniformly in aqueous solution with an average particle diameter of ~136 nm, and showed high drug loading amount of 1767 mg/g. The SS/PAC exhibited high antioxidant efficiency and excellent biocompatibility (non-irritant, non-hemolysis, and non-cytotoxicity), could remarkably alleviate the symptoms of dextran sulfate sodium-induced ulcerative colitis by decreasing the disease activity index scores, inhibiting the shortening of colon length, regulating oxidative stress, suppressing inflammation, and reversing the histopathological injuries. This work provides a simple method to fabricate SS-stabilized-drug composites, promises high potential in therapeutic and pharmaceutical applications.

Rhein incorporated silk fibroin hydrogels with antibacterial and anti-inflammatory efficacy to promote healing of bacteria-infected burn wounds.

Advanced dressings that can simultaneously prevent bacterial colonization/infection and reduce inflammation are highly desired. A simple strategy was developed to incorporate an anti-inflammatory and antibacterial drug rhein into the structure of silk fibroin (SF) matrix to fabricate a hydrogel dressing. The SF/Rhein hydrogels showed fibrous network nanostructure, high water content (~90%), high water adsorption ability (>2 folds of its own weight), acceptable mechanical strength, biocompatibility and antibacterial properties, suitable as dressings for the treatment of bacterial infected wounds. The SF/Rhein hydrogels enhanced the healing rate of burn wounds by reducing inflammation, expediting angiogenesis, and promoting skin appendages formation, being a promising candidate as wound dressings.

Fibrous aramid hydrogel supported antibacterial agents for accelerating bacterial-infected wound healing.

Bacterial infections severely retard the wound healing process. Antibacterial drugs were loaded onto aramid nanofibers (ANFs) hydrogels through a convenient strategy to fabricate dressings for bacterial infected wound healing. ANFs hydrogels owned good mechanical properties, high water content (>98%), high water adsorption property (>10,000%) and good water retention ability (a water retention of >5000% after incubating at RH 30% for 8 h), capable to absorb and retain the wound exudate to form a moist environment. The incorporation of antibacterial drugs promised the ANFs hydrogels with durable antibacterial properties. Furthermore, the drug loaded ANFs hydrogels had no cytotoxicity nor hemolytic potential. In vivo skin wound healing results confirmed that the composite hydrogels accelerated the healing rate of infection wounds on mice and were suitable as a potential anti-infective wound dressing.

Properties evaluation of biochar/high-density polyethylene composites: Emphasizing the porous structure of biochar by activation.

Activated biochars (AB-0.5, AB-1, AB-1.5, AB-2) prepared under different concentrations of an activating agent were used to manufacturing composites (ABHC-0.5, ABHC-1, ABHC-1.5, ABHC-2) based on high-density polyethylene (HDPE) by compounding and injection molding. Thermal and mechanical properties of the composites were characterized and analyzed. The addition of activated biochars improved the thermal properties of HDPE shown by Differential scanning calorimetry and Thermogravimetric analysis. Additionally, ABHC-0.5 exhibited the best flexural strength (38.66 MPa), flexural modulus (2.46 GPa), tensile strength (32.17 MPa), tensile modulus (1.95 GPa), rigidity, elasticity, creep resistance, and anti-stress relaxation ability due to the best porous structure of AB-0.5. A decrease of mechanical properties was observed in ABHC-1, ABHC-1.5, ABHC-2 compared to ABHC-0.5, which was due to the fact that the porous structure was damaged by an excessive activating agent. The results of this study provided a predictive insight in view of optimizing process parameters and establishing the meaningful relationship between biochar porous structure and its resulting composites.

The synthesis of high-aspect-ratio Au microwires with a biomolecule for electrochemical sensing.

Gold (Au) crystalline microwires with an unprecedented diameter of >500 nm and an aspect ratio >400 were synthesized using l-tyrosine as a reducing and capping agent. The Au microwires possessed high conductivity and electrocatalytic activities towards glucose and Hg(ii). Their large diameters and aspect ratios also offered maneuverability, and it was easy to produce Au microelectrodes.

Inhibiting and catalysing amyloid fibrillation at dynamic lipid interfaces.

Proteins are naturally exposed to diverse interfaces in living organisms, from static solid to dynamic fluid. Solid interfaces can enrich proteins as corona, and then catalyze, retard or hinder amyloid fibrillation. But fluid interfaces abundant in biology have rarely been studied for their correlation with protein fibrillation. Unsaturated fatty acids own growing essential roles in diet, whose fluid interfaces are found in vitro to catalyze amyloid fibrillation under certain physiologic conditions. It is determined by the location of double bonds within alkyl chains as well as the presence of physical shear. Docosahexaenoic acid (DHA) shows low catalysis because its unique alkyl chain does not favor to stabilize cross-ß nucleus. Mixtures of different fatty acids also decelerate their catalytic activity. High catalysis poses an unprecedented approach to synthesize biologic nanofibrils as one-dimensional (1D) building blocks of functional hybrids. Fibrillation inhibition implied that appropriate diet would be a preventive strategy for amyloid-related diseases. Thus these results may find their significances in diverse fields of science as chemistry, biotechnology, nanotechnology, nutrition, amyloid pathobiology and nanomedicine.

Sheet-like and tubular aggregates of protein nanofibril-phosphate hybrids.

Bovine serum albumin assembled into supramolecular fibrils and aligned into microtubes and nanosheets upon simply heating and cooling its solution in phosphate buffer under carefully-selected conditions. This unique "one-batch" synthesis was justified by the one-dimensional growth of phosphate crystals in combination with the strong affinity of phosphate ions to protein fibrils.

Conductive Core-Shell Aramid Nanofibrils: Compromising Conductivity with Mechanical Robustness for Organic Wearable Sensing.

One-dimensional organic nanomaterials with a combination of electric conductivity, flexibility, and mechanical robustness are highly in demand in a variety of flexible electronic devices. Herein, conducting polymers were combined with robust Kevlar nanofibrils (aramid nanofibrils, abbreviated as ANFs) via in situ polymerization. Owing to the strong interactions between ANFs and conjugated polymers, the resultant core-shell ANFs showed high electric conductivity in combination with flexibility, robustness, physical stability, and endurance to bending and solvents, in sharp contrast to many inorganic conductive nanomaterials. Due to their responsivity of conductivity to different stimuli (e.g., humidity and strain), their membranes were capable not only of sensing human motions and speech words, but also of showing high sensitivity to variation of environmental humidity. In such a way, these core-shell ANFs may pave the way for combining both conductivity and mechanical properties applicable for diverse wearable devices.

Supramolecular proteinaceous biofilms as trapping sponges for biologic water treatment and durable catalysis.

Inspired by the bacterial biofilms and chorions of living organisms which are made by proteinaceous assemblies and functional for multi-applications, various artificial protein fibrils-based nanoporous films are developed, and show their potential applications in multiple fields. Here, a simple and environmental friendly method was identified to produce bovine serum albumin (BSA) nanofibrils based biofilms, through a combination of protein fibrillation and reverse dialysis. BSA nanofibrils formed biofilms through intermolecular interactions, the resultant biofilms showed tunable thickness by altering the initial protein amount, good stability in organic and salty solvents, transparency and fluorescence properties, hold high capacity of trapping different substances (e.g. nanomaterials, organic dyes, heavy-metal ions and enzymes), and further enabled applications in biologic water treatment and enzyme stabilization. Taken o-phenylenediamine as substrate, the trapped horseradish peroxidase showed a catalytic activity 9-38 folds higher than free ones in organic phase, together with enhanced stability. These protein nanofibrils-based films offered an attractive biologic platform to hybridize diverse materials for on-demand functions and applications.

Activation of Actuating Hydrogels with WS2 Nanosheets for Biomimetic Cellular Structures and Steerable Prompt Deformation.

Macroscopic soft actuation is intrinsic to living organisms in nature, including slow deformation (e.g., contraction, bending, twisting, and curling) of plants motivated by microscopic swelling and shrinking of cells, and rapid motion of animals (e.g., deformation of jellyfish) motivated by cooperative nanoscale movement of motor proteins. These actuation behaviors, with an exceptional combination of tunable speed and programmable deformation direction, inspire us to design artificial soft actuators for broad applications in artificial muscles, nanofabrication, chemical valves, microlenses, soft robotics, etc. However, so far artificial soft actuators have been typically produced on the basis of poly(N-isopropylacrylamide) (PNiPAM), whose deformation is motived by volumetric shrinkage and swelling in analogue to plant cells, and exhibits sluggish actuation kinetics. In this study, alginate-exfoliated WS2 nanosheets were incorporated into ice-template-polymerized PNiPAM hydrogels with the cellular microstructures which mimic plant cells, yet the prompt steerable actuation of animals. Because of the nanosheet-reinforced pore walls formed in situ in freezing polymerization and reasonable hierarchical water channels, this cellular hybrid hydrogel achieves super deformation speed (on the order of magnitude of 10° s), controllable deformation direction, and high near-infrared light responsiveness, offering an unprecedented platform of artificial muscles for various soft robotics and devices (e.g., rotator, microvalve, aquatic swimmer, and water-lifting filter).

Biomimetic Hybridization of Kevlar into Silk Fibroin: Nanofibrous Strategy for Improved Mechanic Properties of Flexible Composites and Filtration Membranes.

Silk, one of the strongest natural biopolymers, was hybridized with Kevlar, one of the strongest synthetic polymers, through a biomimetic nanofibrous strategy. Regenerated silk materials have outstanding properties in transparency, biocompatibility, biodegradability and sustainability, and promising applications as diverse as in pharmaceutics, electronics, photonic devices and membranes. To compete with super mechanic properties of their natural counterpart, regenerated silk materials have been hybridized with inorganic fillers such as graphene and carbon nanotubes, but frequently lose essential mechanic flexibility. Inspired by the nanofibrous strategy of natural biomaterials (e.g., silk fibers, hemp and byssal threads of mussels) for fantastic mechanic properties, Kevlar was integrated in regenerated silk materials by combining nanometric fibrillation with proper hydrothermal treatments. The resultant hybrid films showed an ultimate stress and Young's modulus two times as high as those of pure regenerated SF films. This is not only because of the reinforcing effect of Kevlar nanofibrils, but also because of the increasing content of silk ß-sheets. When introducing Kevlar nanofibrils into the membranes of silk nanofibrils assembled by regenerated silk fibroin, the improved mechanic properties further enabled potential applications as pressure-driven nanofiltration membranes and flexible substrates of electronic devices.