Multicompartment Nanoparticles by Crystallization-Driven Self-Assembly of Star Polymers: Combining High Stability and Loading Capacity.

Herein novel multicompartment nanoparticles (MCNs) that combine high stability and cargo loading capacity are developed. The MCNs are fabricated by crystallization-driven self-assembly (CDSA) of a tailor-made 21 arm star polymer, poly(L-lactide)[poly(tert-butyl acrylate)-block-poly(ethylene glycol)]20 [PLLA(PtBA-b-PEG)20 ]. Platelet-like or spherical MCNs containing a crystalline PLLA core and hydrophobic PtBA subdomains are formed and stabilized by PEG. Hydrophobic cargos, such as Nile Red and chemotherapeutic drug doxorubicin, can be successfully encapsulated into the collapsed PtBA subdomains with loading capacity two orders of magnitude higher than traditional CDSA nanoparticles. Depolarized fluorescence measurements of the Nile Red loaded MCNs suggest that the free volume of the hydrophobic chains in the nanoparticles may be the key for regulating their drug loading capacity. In vitro study of the MCNs suggests excellent cytocompatibility of the blank nanoparticles as well as a dose-dependent cellular uptake and cytotoxicity of the drug-loaded MCNs.

Highly Transparent, Strong, and Flexible Films with Modified Cellulose Nanofiber Bearing UV Shielding Property.

This work investigates multifunctional composite films synthesized with cellulose nanofibers (CNFs) and poly(vinyl alcohol) (PVA). First, TEMPO-oxidized CNFs were modified in the heterogeneous phase with benzophenone, diisocyanate, and epoxidized soybean oil via esterification reactions. A thorough characterization was carried out via elemental analysis as well as FT-IR and X-ray photoelectron spectroscopies and solid-state NMR. Following, the surface-modified CNFs were combined with PVA to endow composite films with UV-absorbing capabilities while increasing their thermomechanical strength and maintaining a high light transmittance. Compared to neat PVF films, the tensile strength, Young modulus, and elongation of the films underwent dramatic increases upon addition of the reinforcing phase (maximum values of ∼96 MPa, ∼ 714 MPa, and ∼350%, respectively). A high UV blocking performance, especially in the UVB region, was observed for the introduced multifunctional PVA films at CNF loadings below 5 wt %. The trade-off between modified nanofibril function as interfacial reinforcement and aggregation leads to an optimum loading. The results indicate promising applications, for example, in active packaging.

Xylan derived fluorescence carbon dots composite with cotton cellulose paper as 'turn-off' fluorescence platform for sensitive and selective detection Cu2+ in real samples.

The pollution of heavy metals such as Cu2+ is still serious and the discharge of sewage of Cu2+ will cause damage to soil environment and human health. Herein, a biomass-based solid-state fluorescence detection platform (CPU-CDs) was developed as fluorescent sensor for detection Cu2+ via fluorescence and colorimetric dual-model methods in real time. CPU-CDs was composed of xylan-derived CDs (U-CDs) and cotton cellulose paper, which exhibiting good reusability, non-toxicity, excellent fluorescence characteristics and high biocompatibility. Further, CPU-CDs displayed high effectiveness and sensitivity for Cu2+ with the detection limit as low as 0.14 µM, which was well below U.S. EPA safety levels (20 µM). Practical application indicated that CPU-CDs could achieve precision response of Cu2+ change in real environment water samples with good recovery range of 90 %-119 %. This strategy demonstrated a promising biomass solid-state fluorescence sensor for Cu2+ detection for water treatment research, which is of great significance in dealing with water pollution caused by heavy metal ions.

Tribo-charge enhanced and cellulose based biodegradable nanofibrous membranes with highly fluffy structure for air filtration and self-powered respiration monitoring systems.

Recently, the demand for healthcare products especially wearable smart masks is increasing. The biosafety and degradability of smart masks are crucial for human health and environmental protection. However, the development of biodegradable and biocompatible fibrous membranes with high filtration efficiency and low pressure drop is still a challenge. How to realize the collaborative improvement between air filtration efficiency and pressure drop of the nanofibrous membrane is still a challenge. Here, a tribo-charge enhanced and biodegradable nanofibrous membranes (TCB NFMs) with highly fluffy structure for air filtration and self-powered respiration monitoring systems is reported for the first time. The filtration efficiency and pressure drop of the prepared membranes for 0.3 µm NaCl particulates is 99.971% and 41.67 Pa. The TCB NFMs based smart mask possesses a series of satisfactory and excellent characteristics, such as self-powered, biodegradable, biocompatible, high filtration efficiency, and low pressure drop, which is highly promising for application in air filtration systems and intelligent wearable respiration monitoring systems.

Biomass-based indole derived fluorescence sensor composited with cellulose paper: Detection of picric acid in food and environment samples.

Picric acid (PA) is highly water-soluble, the fact makes it stand out as the most hazardous environment pollutant. Therefore, accurate determination of PA is of great significance for human health and environmental protection. Herein, a novel indole-based fluorescent sensor (H1) with good water solubility and fluorescence stability was reported. H1 exhibited 'turn-off' fluorescence response for PA with fast reaction rate (<30 s), unique specificity and excellent selectivity and high sensitivity (limit of detection = 34 nM). Further, H1 was successfully applied to detect PA in real samples (tap water, Yangtze River, Xuanwu Lake, soil, food, fish and shrimp) with satisfactory recoveries at three spiking levels ranging from 98.0 to 112.0 %. In addition, H1 displayed high biocompatibility in mung beans and fresh blood. Moreover, aiming to attain portable analysis, H1 was composited with biomass cellulose paper (H1-FP) and integrated with smartphone for construction as a solid-state fluorescence platform to achieve fast and visual detection of PA in suit with significant stability, high sensitively and selectivity. The establishment of this sensing approach is expected to offer new insight into rapid, selective, and sensitive detection of major pollutants for food and environmental safety.

Biomaterials based on hyaluronic acid, collagen and peptides for three-dimensional cell culture and their application in stem cell differentiation.

In recent decades, three-dimensional (3D) cell culture technologies have been developed rapidly in the field of tissue engineering and regeneration, and have shown unique advantages and great prospects in the differentiation of stem cells. Herein, the article reviews the progress and advantages of 3D cell culture technologies in the field of stem cell differentiation. Firstly, 3D cell culture technologies are divided into two main categories: scaffoldless and scaffolds. Secondly, the effects of hydrogels scaffolds and porous scaffolds on stem cell differentiation in the scaffold category were mainly reviewed. Among them, hydrogels scaffolds are divided into natural hydrogels and synthetic hydrogels. Natural materials include polysaccharides, proteins, and their derivatives, focusing on hyaluronic acid, collagen and polypeptides. Synthetic materials mainly include polyethylene glycol (PEG), polyacrylic acid (PAA), polyvinyl alcohol (PVA), etc. In addition, since the preparation techniques have a large impact on the properties of porous scaffolds, several techniques for preparing porous scaffolds based on different macromolecular materials are reviewed. Finally, the future prospects and challenges of 3D cell culture in the field of stem cell differentiation are reviewed. This review will provide a useful guideline for the selection of materials and techniques for 3D cell culture in stem cell differentiation.

Preparation of a thermosensitive nanofibre membrane for blackberry preservation.

Blackberries provide multiple health benefits. However, they deteriorate easily during harvesting, storage, and transportation (temperature-changing). Therefore, to extend their shelf-life under variable temperature conditions, a temperature-sensitive nanofibre-based material with good preservation attributes was developed, composed of polylactic acid (PLA) electrospun fibres, loaded with lemon essential oil (LEO) and covered with poly (N-isopropylacrylamide) (PNIPAAm). Compared with PLA and PLA/LEO nanofibres, PLA/LEO/PNIPAAm exhibited good mechanical properties, oxidation resistance, antibacterial ability, and controlled release of LEO. The PNIPAAm layer prevented rapid LEO release below the low critical solution temperature (32 °C). When the temperature exceeded 32 °C, the PNIPAAm layer underwent a chain-to-globule transition and accelerated LEO release (slower than PLA/LEO). The temperature-controlled release of LEO via PLA/LEO/PNIPAAm membrane prolongs its action time. Therefore, PLA/LEO/PNIPAAm effectively maintained the appearance and nutritive quality of blackberries during variable storage temperatures. Our research demonstrated that active fibre membranes have great potential applications in preserving fresh products.

Stimuli-responsive electrospun fibers and their applications.

Stimuli-responsive electrospun nanofibers are gaining considerable attention as highly versatile tools which offer great potential in the biomedical field. In this critical review, an overview is given on recent advances made in the development and application of stimuli-responsive fibers. The specific features of these electrospun fibers are highlighted and discussed in view of the properties required for the diverse applications. Furthermore, several novel biomedical applications are discussed and the respective advantages and shortcomings inherent to stimuli-responsive electrospun fibers are addressed (136 references).

Quaternized chitin/tannic acid bilayers layer-by-layer deposited poly(lactic acid)/polyurethane nanofibrous mats decorated with photoresponsive complex and silver nanoparticles for antibacterial activity.

Chronic wounding treatment based on bacterially infected diabetes suffers an essential limitation in persistent skin injuries due to the resistance of progressive antibiotics, which inhibits the process of healing with wound tissue. Therefore, biologically friendly and nontoxic bio-based mats without antibiotics are taken for granted as a versatile platform for biomedical dressing, but urgently necessitates further functional diversification. Herein, a novel tannic acid (TA)/silver (Ag)-modified poly(lactic acid) (PLA)/Polyurethane (PU) antibacterial hybrid nanofibers were successfully constructed by electrospinning technology. Layer-by-layer (LBL) self-assembly technique was utilized to produce membranes via deposited biocompatible quaternized chitin (QC) and TA. The mats are enabled with outstanding flexibility, antibacterial activity, great hemocompatibility, and good ROS-scavenger in a wounding environment. Consequently, the basis of morphology and structure of electrospun membranes was verified by SEM and FT-IR. Besides, the LBL-structured surface was proved to impart improved wettability and hydrophilic via the test of water contact angle. Additionally, antimicrobial experiments demonstrate the effective broad-spectrum antibacterial ability of as-prepared hybrids, inhibiting infection of gram-positive microbial (S. aureus) as well as gram-negative microbial. Finally, the anti-oxidation performance holds great promise in conducive to the formation favorable physiological environment for wound healing. In conclusion, this work establishes a feasible but effective pathway to construct a multifunctional antibacterial dressing for the skin infection.

Toxic reactive oxygen species enhanced chemodynamic therapy by copper metal-nanocellulose based nanocatalysts.

When compared with traditional petroleum-based materials, bio-based materials show greater application potential in the field of biomedicine owing to the good biocompatibility, in specifical, the application of natural macromolecular polymers in chemotherapeutics has become a hot topic in anticancer treatment. In this study, cellulose nanocrystals (CNCs) were selected as carriers, and Au nanoparticles (NPs) were directly conjugated on their surface, with the highly reactive Cu2+ ions serving as an ion-ligand bridge, to construct a multifunctional nanocatalyst. These findings suggest that the nanosystem delivers a large amount of highly reactive Cu2+ ions (3.75 wt%) and DOX (7.71 wt%) by the surface loading of cellulose nanocrystals, which greatly improves ROS yield and promotes the application of the Fenton reaction system in cancer therapy.

A biomass-derived Schiff base material composited with polylactic acid nanofiber membrane as selective fluorescent 'turn off/on' platform for Pb2+ quantitative detection and characterization.

Herein, a biomass-derived compound Z1 is synthesized via 'one pot' method for detection Pb2+ using fluorescence and visual dual-mode in aqueous solution. Z1 shows good response to Pb2+ with a limit of detection (LOD) of 13.4 nM. Importantly, the coordination mode of Z1 with Pb2+ is further evaluated by UV-vis and NMR spectroscopy and a 1:1 stoichiometry is identified. Furthermore, Z1 can be applied to detection Pb2+ in practical samples with satisfactory recoveries in range of 96.0 %-112.0 % in real samples. Besides, Z1 is added into polylactic acid (PLA) solution and made as portable fluorescence nanofiber membrane for Pb2+ detection. Further, Z1 responds to Pb2+ with high selectivity and sensitivity and has been applied for tracking Pb2+ changes in soil samples, zebrafish, and plant tissues. These results indicated that Z1 had great application potential in accurate detection Pb2+.

Biomass-based indole derived composited with cotton cellulose fiber integrated as sensitive fluorescence platform for NH3 detection and monitoring of seafood spoilage.

Herein, an indole-derived water-soluble fluorescence nanomaterial and biomass-based cellulose filter paper integrated as solid-state fluorescence platform (H2-FP) for seafood spoilage detection was prepared. H2 exhibits high fluorescence stability and good biocompatibility with green beans, onion tissues, blood and zebrafish, which proving that H2 has a wide range of application scenarios. Further, H2-FP with effective, solid-state fluorescence, portable, and reusable characteristics is nanoengineered for NH3 quantitative and qualitative detection (DOL = 2.6 ppm). Then, H2-FP has been successfully used to monitor NH3 release in the seafood spoilage process at various storage time (4 °C and 25 °C). More importantly, fluorescence color of H2-FP is integrated smartphone are converted to digital values through RGB channels and successfully used to visualize semi-quantitative recognition of NH3. This sensing fluorescence platform integrated with smartphone furnishes an effective fabrication strategy and broad prospects for explore various biomass-based materials for sensing NH3 change in biological and environmental samples.

A biocompatible and pH-responsive nanohydrogel based on cellulose nanocrystal for enhanced toxic reactive oxygen species generation.

Traditional therapeutic regimens are currently far from satisfactory, and the integration of biocompatible carbohydrate polymers and nanotechnologies with conventional therapeutics has become a focus of research in cancer therapy. Herein, A novel biocompatible and pH-responsive nanohydrogel composed of two functional polymeric chains was developed from cellulose nanocrystals (CNCs) and 5-aminolevulinic acid (ALA), or dopamine (DPA). The biological molecules PDA and ALA were respectively conjugated to CNC through the coordination of iron ions to form two functional polymeric chains (PDA/Fe@CNC and ALA/Fe@CNC). The PDA/Fe@CNC chain increased the adhesion of the nanohydrogels to cells, while the ALA/Fe@CNC chain significantly increased reactive oxygen species (ROS) production. Furthermore, PTX molecules loaded into the nanohydrogels combined with ROS to efficiently kill tumor cells. The nanohydrogels displayed excellent cell affinity, high ROS yield (8.0-fold greater than that in control), and strong cytotoxicity (2.7 % of cell viability). The present study highlights the great potential of biocompatible natural polysaccharide-based materials for biomedical applications, and provides a new strategy for reducing the toxicity and side effects associated with traditional chemotherapy, demonstrating a novel antitumor treatment paradigm with high-efficiency but with only minor side effects.

Healable, Adhesive, and Conductive Nanocomposite Hydrogels with Ultrastretchability for Flexible Sensors.

In recent years, conductive hydrogels have generated tremendous attention in biomedicals and bioelectronics fields due to their excellent physiochemical properties. In this study, a physically cross-linked conducting hydrogel has been designed in combination with cellulose nanocrystalline (CNC), polyacrylic acid (PAA) chains, laurel methacrylate, and sodium dodecyl sulfate. The obtained result shows that the hydrogel prepared is ultrastretchable, mechanically robust, transparent, biocompatible, conductive, and self-healing. The mechanical property of the prepared hydrogel is optimized through variation of the CNC content. The optimal hydrogel (CNC-1/PAA) exhibits an impressive mechanics, including high stretchability (∼1800%) and compressibility, good elasticity, and fatigue resistance. Furthermore, the conductivity of the hydrogel enables tensile strain- and pressure-sensing capabilities. The CNC/PAA-based flexible sensors are successfully designed, which shows high sensitivity, fast response (290 ms), and excellent cycle stability as well as the pressure sensing capability. As a result, the designed hydrogel has the ability to sense and detect diverse human motion, including elbow/finger/wrist bending and speaking, which demonstrates that the designed self-healing conductive hydrogels have significant potential for applications in flexible electronics.

Dual-Functional Surfaces Based on an Antifouling Polymer and a Natural Antibiofilm Molecule: Prevention of Biofilm Formation without Using Biocides.

Pathogenic biofilms formed on the surfaces of implantable medical devices and materials pose an urgent global healthcare problem. Although conventional antibacterial surfaces based on bacteria-repelling or bacteria-killing strategies can delay biofilm formation to some extent, they usually fail in long-term applications, and it remains challenging to eradicate recalcitrant biofilms once they are established and mature. From the viewpoint of microbiology, a promising strategy may be to target the middle stage of biofilm formation including the main biological processes involved in biofilm development. In this work, a dual-functional antibiofilm surface is developed based on copolymer brushes of 2-hydroxyethyl methacrylate (HEMA) and 3-(acrylamido)phenylboronic acid (APBA), with quercetin (Qe, a natural antibiofilm molecule) incorporated via acid-responsive boronate ester bonds. Due to the antifouling properties of the hydrophilic poly(HEMA) component, the resulting surface is able to suppress bacterial adhesion and aggregation in the early stages of contact. A few bacteria are eventually able to break through the protection of the anti-adhesion layer leading to bacterial colonization. In response to the resulting decrease in the pH of the microenvironment, the surface could then release Qe to interfere with the microbiological processes related to biofilm formation. Compared to bactericidal and anti-adhesive surfaces, this dual-functional surface showed significantly improved antibiofilm performance to prevent biofilm formation involving both Gram-negative Pseudomonas aeruginosa and Gram-positive Staphylococcus aureus for up to 3 days. In addition, both the copolymer and Qe are negligibly cytotoxic, thereby avoiding possible harmful effects on adjacent normal cells and the risk of bacterial resistance. This dual-functional design approach addresses the different stages of biofilm formation, and (in accordance with the growth process of the biofilm) allows sequential activation of the functions without compromising the viability of adjacent normal cells. A simple and reliable solution may thus be provided to the problems associated with biofilms on surfaces in various biomedical applications.

Universal Antifouling and Photothermal Antibacterial Surfaces Based on Multifunctional Metal-Phenolic Networks for Prevention of Biofilm Formation.

Biofilms formed from the pathogenic bacteria that attach to the surfaces of biomedical devices and implantable materials result in various persistent and chronic bacterial infections, posing serious threats to human health. Compared to the elimination of matured biofilms, prevention of the formation of biofilms is expected to be a more effective way for the treatment of biofilm-associated infections. Herein, we develop a facile method for endowing diverse substrates with long-term antibiofilm property by deposition of a hybrid film composed of tannic acid/Cu ion (TA/Cu) complex and poly(ethylene glycol) (PEG). In this system, the TA/Cu complex acts as a multifunctional building block with three different roles: (i) as a versatile "glue" with universal adherent property for substrate modification, (ii) as a photothermal biocidal agent for bacterial elimination under irradiation of near-infrared (NIR) laser, and (iii) as a potent linker for immobilization of PEG with inherent antifouling property to inhibit adhesion and accumulation of bacteria. The resulted hybrid film shows negligible cytotoxicity and good histocompatibility and could prevent biofilm formation for at least 15 days in vitro and suppress bacterial infection in vivo, showing great potential for practical applications to solve the biofilm-associated problems of biomedical materials and devices.

A novel xanthan gum-based conductive hydrogel with excellent mechanical, biocompatible, and self-healing performances.

Tough and conductive hydrogels are promising materials for various applications. However, it remains a great challenge to develop an integrated hydrogel combining outstanding mechanical, conductive, and self-healing performances. Herein, we prepared a conductive, self-healing, and tough hydrogel by constructing synergistic multiple interaction among montmorillonite (MMT), Poly (acrylamide-co-acrylonitrile) (P(AAm-co-AN)), xanthan gum (XG) and ferric ion (Fe3+). The obtained xanthan gum/montmorillonite/Poly (acrylamide-co-acrylonitrile) (XG/MMT/PAAm) hydrogels showed high strain stress (0.48 MPa) and compressive stress (5.9 MPa) as well as good shape recovery after multiple loading-unloading cycle tests. Moreover, the XG/MMT/PAAm hydrogels have distinctive features such as remarkable resistance to fatigue and harsh environments, insensitivity to notch, conductive, biocompatible, pH-dependent swelling behaviors and self-healing. Therefore, the as-fabricated hydrogel delivers a new prospect for its applications in various fields, such as flexible conductive device and tissue engineering.

Nature-inspired chemistry toward hierarchical superhydrophobic, antibacterial and biocompatible nanofibrous membranes for effective UV-shielding, self-cleaning and oil-water separation.

Fabrication of environmental-friendly, low-cost, and free-standing superhydrophobic nanofibrous membranes with additional functionalities such as self-cleaning and UV-shielding properties is highly demanded for oil-water separation. Herein, we describe the preparation of multifunctional superhydrophobic nanofibrous membrane by using a facile and novel nature-inspired method, i.e., plant polyphenol (tannic acid) metal complex is introduced to generate rough hierarchical structures on the surface of an electrospun polyimide (PI) nanofibrous membrane, followed by modification of poly (dimethylsiloxane) (PDMS). Taking an as-prepared tannic acid - Al3+-based superhydrophobic membrane as an example, it not only exhibits anti-impact, low-adhesive and self-cleaning functions, but also presents excellent performance in the separation of various oil-water mixtures. A high flux up to 6935 l m-2 h-1 with a separation efficiency of over 99% and the oil contents in water below 5 ppm is obtained even after repeating use for twenty separation cycles. Additionally, the membrane exhibits excellent UV-shielding property, attributing to the inherent UV-absorbing ability of tannic acid. Furthermore, the membrane also possesses additional properties including antibacterial activity, good biocompatibility, robust mechanical strength, and excellent resistance to various harsh conditions. These attractive properties of the as-prepared membrane make it a promising candidate for potential applications in industrial oil-contaminated water treatments and oil-water separation.

Smart, Photothermally Activated, Antibacterial Surfaces with Thermally Triggered Bacteria-Releasing Properties.

The development of effective antibacterial surfaces to prevent the attachment of pathogenic bacteria and subsequent bacterial colonization and biofilm formation is critically important for medical devices and public hygiene products. In the work reported herein, a smart antibacterial hybrid film based on tannic acid/Fe3+ ion (TA/Fe) complex and poly(N-isopropylacrylamide) (PNIPAAm) is deposited on diverse substrates. This surface is shown to have bacteria-killing and bacteria-releasing properties based on, respectively, near-infrared photothermal activation and subsequent cooling. The TA/Fe complex has three roles in this system: (i) as a universal adhesive "anchor" for surface modification, (ii) as a high-efficiency photothermal agent for ablation of attached bacteria (including multidrug resistant bacteria), and (iii) as a robust linker for immobilization of NH2-terminated PNIPAAm via either Michael addition or Schiff base formation. Moreover, because of the thermoresponsive properties of the immobilized PNIPAAm, almost all of the killed bacteria and other debris can be removed from the surface simply by lowering the temperature. It is shown that this hybrid film can maintain good antibacterial performance after being used for multiple "kill-and-release" cycles and can be applied to various substrates regardless of surface chemistry or topography, thus providing a broadly applicable, simple, and reliable solution to the problems associated with surface-attached bacteria in various healthcare applications.

Ecofriendly Electrospun Membranes Loaded with Visible-Light-Responding Nanoparticles for Multifunctional Usages: Highly Efficient Air Filtration, Dye Scavenging, and Bactericidal Activity.

Ambient particulate matter pollution has posed serious threats to global environment and public health. However, highly efficient filtration of submicron particles, the so-named "secondary pollution" caused by, e.g., bacterial growth in filters and the use of nondegradable filter materials, remains a serious challenge. In this study, poly(vinyl alcohol) (PVA) and konjac glucomannan (KGM)-based nanofiber membranes, loaded with ZnO nanoparticles, were prepared through green electrospinning and ecofriendly thermal cross-linking. Thus obtained fibrous membranes not only show highly efficient air-filtration performance but also show superior photocatalytic activity and antibacterial activity. The filtration efficiency of the ZnO@PVA/KGM membranes for ultrafine particles (300 nm) was higher than 99.99%, being superior to that of commercial HEPA filters. By virtue of the high photocatalytic activity, methyl orange was efficiently decolorized with a removal efficiency of more than 98% at an initial concentration of 20 mg L-1 under 120 min of solar irradiation. A multifunctional membrane with high removal efficiency, low flow resistance, superior photocatalytic activity, and superior antibacterial activity was successfully achieved. It is conceivable that the combination of a biodegradable polymer and an active metal particle would form an unprecedented photocatalytic system, which will be quite promising for environmental remediation such as air filtration and water treatment.