Scalable, Green, Flexible Photochromic Bacterial Cellulose for Multicolor Switching, Photo-patterning, and Daily Sunlight UV Monitoring.

Sustainable, durable, and diverse photochromic smart textiles based on bacterial cellulose (BC) have emerged as attractive candidates in UV-sensing applications due to the green and easy functionalization of BC. However, existing BC-based photochromic textiles lack photochromic efficiency and combining fastness. In this study, a green strategy for in situ fermentation is developed to achieve the directional distribution of functional particles and remarkable photochromism in photochromic bacterial cellulose (PBC). The unique functional design obtained by regulating the photochromic dye distribution in 3D nanonetworks of PBCs during in situ growth affords a more uniform distribution and high fastness. Benefiting from the uniform distribution of photochromic dyes and adequate utilization of the 3D network structure, more surface area is provided to receive and utilize the photon energy from the UV rays, making the photochromic process more effective. The as-prepared PBCs exhibited rapid (within 1 min) and stable (30 cycles) discoloration and multicolor selectivity. Their simple preparation process and exceptional wearability, e.g., their flexibility, lightweight, and air permeability, make them suitable for various applications, including tunable color switching systems, photopatterning, and daily sunlight UV monitoring. This study provides empirical value for the biofabrication of photochromic textiles and wearable flexible UV sensors.

Melt-electrowriting-enabled anisotropic scaffolds loaded with valve interstitial cells for heart valve tissue Engineering.

Tissue engineered heart valves (TEHVs) demonstrates the potential for tissue growth and remodel, offering particular benefit for pediatric patients. A significant challenge in designing functional TEHV lies in replicating the anisotropic mechanical properties of native valve leaflets. To establish a biomimetic TEHV model, we employed melt-electrowriting (MEW) technology to fabricate an anisotropic PCL scaffold. By integrating the anisotropic MEW-PCL scaffold with bioactive hydrogels (GelMA/ChsMA), we successfully crafted an elastic scaffold with tunable mechanical properties closely mirroring the structure and mechanical characteristics of natural heart valves. This scaffold not only supports the growth of valvular interstitial cells (VICs) within a 3D culture but also fosters the remodeling of extracellular matrix of VICs. The in vitro experiments demonstrated that the introduction of ChsMA improved the hemocompatibility and endothelialization of TEHV scaffold. The in vivo experiments revealed that, compared to their non-hydrogel counterparts, the PCL-GelMA/ChsMA scaffold, when implanted into SD rats, significantly suppressed immune reactions and calcification. In comparison with the PCL scaffold, the PCL-GelMA/ChsMA scaffold exhibited higher bioactivity and superior biocompatibility. The amalgamation of MEW technology and biomimetic design approaches provides a new paradigm for manufacturing scaffolds with highly controllable microstructures, biocompatibility, and anisotropic mechanical properties required for the fabrication of TEHVs.

Structural Analysis and Intrinsic Enzyme Mimicking Activities of Ligand-Free PtAg Nanoalloys.

Nanozymes are nanomaterials with biocatalytic properties under physiological conditions and are one class of artificial enzymes to overcome the high cost and low stability of natural enzymes. However, surface ligands on nanomaterials will decrease the catalytic activity of the nanozymes by blocking the active sites. To address this limitation, ligand-free PtAg nanoclusters (NCs) are synthesized and applied as nanozymes for various enzyme-mimicking reactions. By taking advantage of the mutual interaction of zeolitic imidazolate frameworks (ZIF-8) and Pt precursors, a good dispersion of PtAg bimetal NCs with a diameter of 1.78 ± 0.1 nm is achieved with ZIF-8 as a template. The incorporation of PtAgNCs in the voids of ZIF-8 is confirmed with structural analysis using the atomic pair-distribution function and powder X-ray diffraction. Importantly, the PtAgNCs present good catalytic activity for various enzyme-mimicking reactions, including peroxidase-/catalase- and oxidase-like reactions. Further, this work compares the catalytic activity between PtAg NCs and PtAg nanoparticles with different compositions and finds that these two nanozymes present a converse dependency of Ag-loading on their activity. This study contributes to the field of nanozymes and presents a potential option to prepare ligand-free bimetal biocatalysts with sizes in the nanocluster regime.

Redox-active NiS@bacterial cellulose nanofiber composite separators with superior rate capability for lithium-ion batteries.

Separator is an essential component of lithium-ion batteries (LIBs), which is placed between the electrodes to impede their electrical contact and provide the transport channels for lithium ions. Traditionally, the separator contributes the overall mass of LIBs, thereby reducing the gravimetric capacity of the devices. Herein, a dual-layer redox-active cellulose separator is designed and fabricated to enhance the electrochemical performances of LIBs by introducing NiS. The presented separator is composed of an insulating bacterial cellulose (BC) nanofiber layer and a conductive, and redox-active NiS@BC/carbon nanotubes layer. By using the NiS@BC separator, the discharge capacity of the LiFePO4//Li half battery is enhanced to 117 mAh g-1 at a current of 2C owing to the redox-activity of NiS. Moreover, the functional separator-electrode interface can facilitate the homogenous Li stripping/plating and depress the polarization upon the repeated stripping/plating process. Consequently, the battery containing the redox-active separator exhibits outstanding cycle stability and rate capability. The present study contributes a novel strategy for the developments of functional separators to improve the electrochemical properties of LIBs.

Bifunctional Smart Textiles with Simultaneous Motion Monitoring and Thermotherapy for Human Joint Injuries.

The motion detection and thermotherapy provides a convenient strategy for the diagnosis and rehabilitation assessment of joint injuries. However, it is still challenging to simultaneously achieve accurate joint motion monitoring and on-demand thermotherapy. Herein, core-sheath sensing yarns (CSSYs) is proposed and fabricated for excellent electrical and photothermal heating, which consists of carbon black (CB)-coated nylon (sheath layer), silver-plated nylon and elastic spandex yarns (core layer). The CSSYs demonstrates great joule heating performance, which reaches 75 °C at 2 V applied voltage. The good thermal management performance can be well maintained when weaving these yarns into bifunctional smart textile. Further, the optimized double-ply CSSYs (DPCSSYs) with helically twisted structure possess several appealing sensing performance, including preferable strain sensitivity (0.854), excellent linearity (0.962), and superior durability (over 5000 cycles). The as-woven bifunctional smart textile can provide instant and convenient thermotherapy to the injured joints, and simultaneously monitor the injury and recovery conditions of the joint. Therefore, the designed bifunctional smart textile can provide a promising route for developing next-generation healthcare smart textile.

Superb Silk Hydrogels with High Adaptability, Bioactivity, and Versatility Enabled by Photo-Cross-Linking.

The exceptional biocompatibility and adaptability of hydrogels have garnered significant interest in the biomedical field for the fabrication of biomedical devices. However, conventional synthetic hydrogels still exhibit relatively weak and fragile properties. Drawing inspiration from the photosynthesis process, we developed a facile approach to achieve a harmonious combination of superior mechanical properties and efficient preparation of silk fibroin hydrogel through photo-cross-linking technology, accomplished within 60 s. The utilization of riboflavin and H2O2 enabled a sustainable cyclic photo-cross-linking reaction, facilitating the transformation from tyrosine to dityrosine and ultimately contributing to the formation of highly cross-linked hydrogels. These photo-cross-linking hydrogels exhibited excellent elasticity and restorability even after undergoing 1000 cycles of compression. Importantly, our findings presented that hydrogel-encapsulated adipose stem cells possess the ability to stimulate cell proliferation along with stem cell stemness. This was evidenced by the continuous high expression levels of OCT4 and SOX2 over 21 days. Additionally, the utilization of photo-cross-linking hydrogels can be extended to various material molding platforms, including microneedles, microcarriers, and bone screws. Consequently, this study offered a significant approach to fabricating biomedical hydrogels capable of facilitating real-time cell delivery, thereby introducing an innovative avenue for designing silk devices with exceptional machinability and adaptability in biomedical applications.

Preparation of chitin twisted fiber and its functional applications.

Chitin has garnered significant attention due to its renewable, biocompatibility and biodegradability, while its practical application seriously hindered as the functionality of chitin itself can no longer meet people's increasing requirements for materials. Here, an effective method is successfully built for high-performance chitin fibers fabrication through a multi-step strategy that involved chemical pre-crosslinking, followed by wet-twisting and wet-stretching techniques, combined with physical cross-linking. The as-prepared chitin fiber exhibited a smooth surface, adjustable diameter, and mechanical strong properties (144.6 MPa). More importantly, functional chitin fiber with magnetic or conductive abilities can be easily obtained by spraying Fe3O4 particles or Ag nanowire on the chemical pre-crosslinking chitin gel film before stretching and twisting. The doped functional inorganic particles exist in a continuous ribbon structure in the fiber reduced the decrease in material strength caused by uneven particles dispersion, resulting 88.4 % of stress and 91.6 % of strain retention. This work not only bestow invaluable insights into the fabrication of functional chitin fibers but also provide a novel approach to solve the problem of poor compatibility between organic and inorganic composite materials.

A triple-crosslinking strategy for high-performance regenerated cellulose fibers derived from waste cotton textiles.

Regenerated cellulose fibers has attracted increasing attention for high-grade textile raw materials and industrial textiles, but the low mechanical property caused by differences in regenerated raw materials and production levels limits its commercial application in the product diversity. Herein, we proposed a novel triple-crosslinking strategy by coupling with hydrogen bonds, chemical crosslinking, and internal mineralization from multiple pulsed vapor phase infiltration (MPI) to improve the mechanical performance of regenerated cellulose fibers. A binary solvent composed of ionic liquid (IL) and dimethyl sulfoxide (DMSO) is used to dissolve waste cotton textile and then wet spinning. Dual-crosslinking is firstly achieved by coupling glutaraldehyde (GA) and cellulose reaction. Subsequently, a metal oxide is intentionally infiltrated into inner cellulosic through MPI technology to form a third form of crosslinking, accompanied by the ultra-thin metal oxide nano-layer onto the surface of regenerated cellulose fibers. Results showed that the triple-crosslinking strategy has increased the tensile stress of the fiber by 43.57 % to 287.03 MPa. In all, triple-crosslinking strategy provides a theoretical basis and technical approach for the reinforcement of weak fibers in waste cotton recycling, which is expected to accelerate the development of the waste textile recycling industry and promote of the added-value of regenerated products.

Advances in regenerated cellulosic aerogel from waste cotton textile for emerging multidimensional applications.

Rapid development of society and the improvement of people's living standards have stimulated people's keen interest in fashion clothing. This trend has led to the acceleration of new product innovation and the shortening of the lifespan for cotton fabrics, which has resulting in the accumulation of waste cotton textiles. Although cotton fibers can be degraded naturally, direct disposal not only causes a serious resource waste, but also brings serious environmental problems. Hence, it is significant to explore a cleaner and greener waste textile treatment method in the context of green and sustainable development. To realize the high-value utilization of cellulose II aerogel derived from waste cotton products, great efforts have been made and considerable progress has been achieved in the past few decades. However, few reviews systematically summarize the research progress and future challenges of preparing high-value-added regenerated cellulose aerogels via dissolving cotton and other cellulose wastes. Therefore, this article reviews the regenerated cellulose aerogels obtained through solvent methods, summarizes their structure, preparation strategies and application, aimed to promote the development of the waste textile industry and contributed to the realization of carbon neutrality.

Preparation and properties of chitin/silk fibroin biocompatible composite fibers.

In the present world chitin is used enormously in various fields, such as biopharmaceuticals, medical and clinical bioproducts, food packaging, etc. However, its development has been curbed by the impaired performance and cumbersome dissolution process when chitin materials are dissolved and regenerated by physical or chemical methods. To further obtain the regenerated chitin fiber material with improved performance, silk fibroin was introduced into the chitin matrix material, and chitin/silk fibroin biocompatible composite fibers were obtained by formic acid/calcium chloride/ethanol ternary system and top-down wet spinning technology. The produced composite fibers outperformed previously reported chitin-silk composites in terms of the tensile strength (160 MPa) and failure strain (25%). The fibers also performed good cell compatibility and strong cellular affinity for non-toxicity. The cell viabilities of the fibers were about 20% greater than those of silk fiber after three days of co-culture with NIH-3T3. Furthermore, no hemolysis occurs in the presence of chitin/silk fibers, demonstrating their superior hemocompatibility. The fibers had a hemolysis index as low as 1%, which is far lower than the acceptable level of 5%. The material offers prospective opportunities for biomaterial applications in anticoagulation, absorbable surgical sutures, etc.

Flexible dual-functionalized hyaluronic acid hydrogel adhesives formed in situ for rapid hemostasis.

Hydrogel adhesives integrating both rapid and strong adhesion to blooding tissues and biocompatibility are highly desired for fast hemostasis. Herein, a flexible hyaluronic acid hydrogel adhesive is fabricated via photocrosslinking of the solution originating from dopamine-conjugated maleic hyaluronic acid (DMHA) in situ. The introduction of acrylate groups with high substitutions into the hydrogel matrix endows the adhesive with rapid gelation and strong tissue adhesion properties through photopolymerization. Moreover, the high substitution of catechol groups with unoxidized state can not only induce red blood cell aggregation and platelets adhesion but also adhere to wound tissue to further enhance hemostasis. Based on its bio-adhesion and procoagulant activity, the DMHA hydrogel formed in situ reveals superior hemostatic performance in the rat liver injury model and noncompressible hemorrhage model, and rabbit femoral artery puncture model, compared to commercial products (gauze, absorbable gelatin sponge) and oxidized DMHA (SMHA) hydrogel. Besides, the hydrogel exhibited good adaptability, biodegradability, and superior cytocompatibility as well as negligible inflammation. This hydrogel adhesive is a promising biological adhesive for hemorrhage control.

Substituent effect on the π linkers in triphenylamine dyes for sensitized solar cells: a DFT/TDDFT study.

A series of metal-free organic donor-π bridge-acceptor dyes are studied computationally using density functional theory (DFT) and time-dependent DFT (TDDFT) approaches to explore their potential performances in dye-sensitized solar cells (DSSCs). Taking triphenylamine (TPA) and cyanoacrylic acid moieties as donor and acceptor units, respectively, the effects of different substituents of the π linkers in the TPA-based dyes on the energy conversion efficiency of the DSSCs are theoretically evaluated through optimized geometries, charge distributions, electronic structures, simulated absorption spectra, and free energies of injection. The results show that the molecular orbital energy levels and electron-injection driving forces of the TPA dyes can be tuned by the introduction of substituents with different electron-withdrawing or -donating abilities. The electron-withdrawing substituent always lowers the energies of both frontier orbitals, while the electron-donating one heightens them simultaneously. The efficiency trend of these TPA derivatives as sensitizers in DSSCs is also predicted by analyzing the light-harvesting efficiencies and the free energies of injection. The following substituents are shown to increase the efficiency of the dye: OMe, OEt, OHe, and OH.

Self-Healing Hyaluronic Acid Nanocomposite Hydrogels with Platelet-Rich Plasma Impregnated for Skin Regeneration.

The development of natural hydrogels with sufficient strength and self-healing capacity to accelerate skin wound healing is still challenging. Herein, a hyaluronic acid nanocomposite hydrogel was developed based on aldehyde-modified sodium hyaluronate (AHA), hydrazide-modified sodium hyaluronate (ADA), and aldehyde-modified cellulose nanocrystals (oxi-CNC). This hydrogel was formed in situ using dynamic acylhydrazone bonds via a double-barreled syringe. This hydrogel exhibited improved strength and excellent self-healing ability. Furthermore, platelet-rich plasma (PRP) can be loaded in the hyaluronic acid nanocomposite hydrogels (ADAC) via imine bonds formed between amino groups on PRP (e.g., fibrinogen) and aldehyde groups on AHA or oxi-CNC to promote skin wound healing synergistically. As expected, ADAC hydrogel could protect and release PRP sustainably. In animal experiments, ADAC@PRP hydrogel significantly promoted full-thickness skin wound healing through enhancing the formation of granulation tissue, facilitating collagen deposition, and accelerating re-epithelialization and neovascularization. This self-healing nanocomposite hydrogel with PRP loading appears to be a promising candidate for wound therapy.

A Flexible and Weavable Lignocellulose-Based Photocatalyst Supported by Natural Three-Dimensional Porous Juncus effusus for Highly Efficient Degradation of Environmental Contaminants.

Lignocellulosic biomass is a potential biotemplate for disposing the burden of the uncontrollable accumulation of environmental contaminants disrupting the hydrophytic ecosystems. Herein, an efficient solar-driven catalyst was prepared using a natural three-dimensional (3D) porous lignocellulose-based Juncus effusus (JE) fiber for wastewater treatment. Owing to the exquisite 3D microstructure and abundant hydroxyl groups, the two-dimensional lamellar graphitic carbon nitride/graphene oxide (g-C3N4/GO) nanocomposites were successfully synthesized and decorated on the carboxymethylated JE fiber via the electrostatic self-assembly method. The as-prepared g-C3N4/GO-JE (CNG-JE) photocatalyst exhibits excellent light absorption efficiency and a superior ability to accelerate photogenerated electron migration. The outstanding adsorption performance toward pollutants also contributes to the photodegradation property of CNG-JE, showing highly efficient degradation of C.I. Reactive Red 120 (99.8%), C.I. Acid Yellow 11 (99.8%), methylene blue (99.4%), Cr(VI) (98.8%), and tetracycline (87.2%). Most importantly, the lignocellulose-based CNG-JE fibers could be fabricated into a photocatalyst textile due to their flexible and weavable properties. In actual application, the CNG-JE textile can be reused for at least five cycles under the sun, demonstrating that the flexible CNG-JE textile is practical and recyclable. This study may provide a platform for constructing efficient, flexible, and weavable biomass-based porous materials for cost-effective and sustainable catalytic applications.

Polylactic acid scaffold with directional porous structure for large-segment bone repair.

Biodegradable porous scaffolds with different structure, porosity, and strength play a critical role in the repair and regeneration of defects in bone tissue engineering by changing the proliferation condition for cell. In this study, polylactic acid (PLA) scaffold with directional porous structure is designed and fabricated using the method of ice template and phase inversion for speeding up bone repair by promoting the growth and proliferation of bone cells. The morphology, mechanical properties, hydrophilicity, and wicking properties of PLA scaffolds were characterized by scanning electron microscope, universal testing machine, contact angle tester and wicking rate test, respectively. In vitro biocompatibility has been investigated through measuring cell adhesion, proliferation, and viability on PLA scaffold with directional porous structure. Prepared PLA scaffold was implanted into animals to observe the repair mechanism of large-sized bone defects. This study proposes a novel bioporous scaffold design to induce osteocyte growth at the rat calvaria with a directional pore structure, and the scaffold edges were integrated with the calvaria at week 12, effectively promoting the repair and regeneration of defective bone tissue.

Bacterial cellulose production from terylene ammonia hydrolysate by Taonella mepensis WT-6.

Hydrothermal degradation was used to pretreat terylene with an aim of noticeably improving the yield of fermentable monomers: terephthalic acid (TPA), mono (2- hydroxyethyl) terephthalic acid (MHET), bis-hydroxyethyl terephthalate (BHET), and ethylene glycol (EG). After 0.5 h of reaction time at 180 °C, hydrothermal degradation with ammonia led to almost complete conversion of the terylene to TPA, MHET, BHET and EG, which were then transformed by Taonella mepensis WT-6 to bacterial cellulose (BC). Furthermore, the optimum fermentation conditions with the maximum BC yield were 5.0 g/L yeast extract, 30.0 °C, pH 9.0, 8.0% inoculum, and hydrolysate TOC (5.02 g/L). Additionally, mechanical and thermal analysis revealed that the properties of BC produced from TAH medium were similar to those of BC produced with HS medium. Considering the substantial amount of global terylene waste being produced, this study provides an alternative solution for the biosynthesis of BC.

Bioinspired Cellulose Foam with Excellent Water Wicking and Flux Properties Prepared Using Ice Template.

The application and functionalization of cellulose has been attracting increased attention in academic and industrial studies because of its wide range of sources, short renewable cycle, and low environmental impact. In order to enhance the application field of cellulose and decrease the environmental pollution for organic solvent associated with its preparation, cellulose foam with a vertically hierarchically porous structure similar to wood was designed and fabricated successfully from a cellulose aqueous solution using an ice templated in this study. The cellulose foam prepared using a 3 wt % concentration possessed a uniform vertical hierarchically porous structure, which could provide a pathway for the flow of water or air based on the capillary effect. The highest water wicking rate and flux were 7.8184 mm·s-1 and 29.49 mL·min-1·g-1, respectively, for the porous foam prepared using a 3 wt % concentration. The mechanical testing experiment showed that the porous structure did not reduce the amount of stress that the sample could endure before being damaged. The compression strength increased with increasing cellulose concentration in solution. Therefore, the hierarchical structure formed in the prepared cellulose foam effectively improved the water flux behavior and provided a structural basis for future applications of cellulose scaffolds.

Small-diameter polyurethane vascular graft with high strength and excellent compliance.

In this study, a polyurethane vascular graft with excellent strength and compliance for clinical application was designed and fabricated by preparing three small-diameter vascular graft layers via the textile techniques of wet spinning and knitting. The polyurethane filament that was fabricated by wet spinning formed the inner layer. The polyurethane tubular fabric was used as the middle layer. The outer layer was prepared by spraying polyurethane solution. The three layers of the polyurethane vascular graft have uniform wall thickness, high strength, excellent compliance, and good puncture resistance compared with clinical poly(ethylene terephthalate) (PET) and expanded polytetrafluoroethylene (ePTFE) vascular graft. Therefore, these layers can have potential clinical applications in the replacement of the conventional artificial vascular graft prepared from PET and ePTFE.

Effect of poly (lactic acid) porous membrane prepared via phase inversion induced by water droplets on 3T3 cell behavior.

Phase inversion induced by water droplets has garnered attention in the field of polymer science as a novel method for preparing porous membranes. This study investigates the effect of the porous structure of poly (lactic acid) (PLA) membranes prepared through phase inversion induced by water droplets at four different temperatures (25, 50, 75, and 100 °C) on the morphology and proliferation of 3T3 cells. The surface properties of the PLA porous membrane, including pore size, pore size distribution, surface roughness, surface hydrophilicity, and cytocompatibility with 3T3 cells, were evaluated. The results indicated that the synthesized PLA membrane had two surfaces with different structures. The upper surface in contact with the water droplets during preparation contained uniformly distributed micropores, whereas the bottom surface was smooth and composed of small particles in contacted with the mold. The upper surface showed high cytocompatibility with 3T3 cells, and the 3T3 cells migrated and grew within the pores at 25 °C. In contrast, the bottom surface exhibited low biocompatibility with the 3T3 cells. Our study has wide-ranging implications and will improve the fabrication and implementation of 3D cultured scaffolds with excellent cytocompatibility.

Photocrosslinking maleilated hyaluronate/methacrylated poly (vinyl alcohol) nanofibrous mats for hydrogel wound dressings.

Although electrospinning of nanofibrous scaffolds benefit to wound healing have been developed at a fast pace, achieving nanofibrous scaffolds with high absorptivity by green electrospinning and crosslinking techniques is still a great challenge. Here, we developed a maleilated hyaluronate/methacrylated poly (vinyl alcohol) (MHA) (MaPVA) composite nanofibers by electrospinning from pure water solvent and followed by photopolymerization to form crosslinking nanofibers network. Electrospinnability of MHA/MaPVA blend systems were investigated and the results shows that the morphology and diameter of the nanofibers were mainly affected by MHA/MaPVA weight ratios by changing viscosity and conductivity of the blend solutions. The crystalline microstructure of the electrospun fibers was not well developed due to intermolecular hydrogen bonding interaction between the molecules of MHA and MaPVA. The photocrosslinking MHA/MaPVA nanofibrous mats can swell to form fibrous hydrogels with high water absorption, meanwhile it is cytocompatible and capable of promoting the cell attachment, which render it great potential for wound dressings.