Photopolymerizable and Antibacterial Hydrogels Loaded with Metabolites from Lacticaseibacillus rhamnosus GG for Infected Wound Healing.

In response to increasing antibiotic resistance and the pressing demand for safer infected wound care, probiotics have emerged as promising bioactive agents. To address the challenges associated with the safe and efficient application of probiotics, this study successfully loaded metabolites from Lacticaseibacillus rhamnosus GG (LGG) into a gelatin cross-linked macromolecular network by an in situ blending and photopolymerization method. The obtained LM-GelMA possesses injectability and autonomous healing capabilities. Importantly, the incorporation of LGG metabolites endows LM-GelMA with excellent antibacterial properties against Staphylococcus aureus and Escherichia coli, while maintaining good biocompatibility. In vivo assessments revealed that LM-GelMA can accelerate wound healing by mitigating infections induced by pathogenic bacteria. This is accompanied by a reduction in the expression of key proinflammatory cytokines such as TNF-α, IL-6, VEGFR2, and TGF-ß, leading to increased re-epithelialization and collagen formation. Moreover, microbiological analysis confirmed that LM-GelMA can modulate the abundance of beneficial wound microbiota at family and genus levels. This study provides a facile strategy and insights into the functional design of hydrogels from the perspective of wound microenvironment regulation.

Green preparation of antibacterial shape memory foam based on bamboo cellulose nanofibril and waterborne polyurethane for adaptive relief of plantar pressure.

This study developed an aqueous solution blending and freeze-drying method to prepare an antibacterial shape memory foam (WPPU/CNF) based on waterborne PHMG-polyurethane and cellulose nanofibers derived from bamboo in response to the increasing demand for environmentally friendly, energy conserving, and multifunctional foams. The obtained WPPU/CNF composite foam has a highly porous network structure with well-dispersed CNFs forming hydrogen bonds with the WPPU matrix, which results in a stable and rigid cell skeleton with enhanced mechanical properties (80 KPa) and anti-abrasion ability. The presence of guanidine in the polyurethane chain endowed the WPPU/CNF composite foam with an instinctive and sustained antibacterial ability against Escherichia coli and Staphylococcus aureus. The WPPU/CNF composite foam exhibited a water-sensitive shape memory function in a cyclic shape memory program because of the chemomechanical adaptability of the hydrogen-bonded network of CNFs in the elastomer matrix. The shape-fixation ratio for local compression reached 95 %, and the shape-recovery rate reached 100 %. This allows the WPPU/CNF pad prototype to reversibly adjust the undulation height to adapt to plantar ulcers, which can reduce the local plantar pressure by 60 %. This study provides an environmentally friendly strategy for cellulose-based composite fabrication and enriches the design and application of intelligent foam devices.

Photocuring and Gelatin-Based Antibacterial Hydrogel for Skin Care.

The development of moisturizing, antibacterial, and biocompatible multifunctional hydrogels is essential to protect skin and promote skin defects recovery. Gelatin has admired potential to be applied for skin care as a hydrogel in virtue of its hydrophilic biocompatible and biodegradable properties. In this study, triclosan-grafted gelatin and photo-cross-linkable methacrylated gelatin were synthesized and then combined to construct the semi-interpenetrating network and antibacterial hydrogels with the aid of a visible blue light. The antimicrobial test demonstrated that the resulting hydrogel obtained excellent inactivation capacity against E. coli, S. aureus, T. rubrum, and C. albicans with sterilizing rates of 99.998%, 99.998%, 99.19%, and 99.64%, respectively. In addition, the cytotoxicity, hemolysis, skin irritation, and rat skin wound healing experiments proved the good biocompatibility of the hydrogel. Therefore, this investigation sheds light on the development of multifunctional hydrogels in skin care.

Development of an antibacterial polypropylene/polyurethane composite membrane for invisible orthodontics application.

In virtue of the advantages, such as aesthetics, designability, convenient removal, and comfortable experience, invisible orthodontics (IO) have been widely recognized and accepted by the public. However, most of the membranes currently used for IO only meet the requirement of shape retention. Other vital functions, like antibacterial and antifouling activities, are neglected. Herein, antibacterial composite membranes (ACMs) containing polypropylene (PP), thermoplastic polyurethane (TPU) and poly (hexamethylene guanidine) hydrochloride-sodium stearate (PHMG-SS) were facilely manufactured through the hot-pressing membrane forming technology. ACMs were conferred with favorable transparency (∼70% in the visible light range) and excellent antibacterial ability. Experiment results demonstrated that bactericidal rates of ACMs against Staphylococcus aureus, Escherichia coli and Streptococcus mutans were larger than 99.99%. Noticeably, the amount of protein adhered on the surface of ACMs was only 28.1 µg/cm2, showing ideal antifouling performance. Collectively, the mutifunctional ACMs in the study are expected to be prominent alternatives for existing IO.

Lotus Leaf-Inspired Breathable Membrane with Structured Microbeads and Nanofibers.

Electrospinning is a feasible technology to fabricate nanomaterials. However, the preparation of nanomaterials with controllable structures of microbeads and fine nanofibers is still a challenge, which hinders widespread applications of electrospun products. Herein, inspired by the micro/nanostructures of lotus leaves, we constructed a structured electrospun membrane with excellent comprehensive properties. First, micro/nanostructures of membranes with adjustable microbeads and nanofibers were fabricated on a large scale and quantitatively analyzed based on the controlling preparation, and their performances were systematically evaluated. The deformation of diverse polymeric solution droplets in the electrospinning process under varying electric fields was then simulated by molecular dynamic simulation. Finally, novel fibrous membranes with structured sublayers and controllable morphologies were designed, prepared, and compared. The achieved structured membranes demonstrate a high water vapor transmission rate (WVTR) > 17.5 kg/(m2 day), a good air permeability (AP) > 5 mL/s, a high water contact angle (WCA) up to 151°, and a high hydrostatic pressure of 623 mbar. The disclosed science and technology in this article can provide a feasible method to not only adjust micro/nanostructure fibers but also to design secondary multilayer structures. This research is believed to assist in promoting the diversified development of advanced fibrous membranes and intelligent protection.

Improvement of Antibacterial and Antifouling Properties of a Cellulose Acetate Membrane by Surface Grafting Quaternary Ammonium Salt.

Through etherification reaction, epoxy propyl dimethyl dodecyl ammonium chloride (EPDMDAC) was grafted onto the surface of a cellulose acetate (CA) membrane to prepare a stable nonleaching antibacterial antifouling membrane (QCA-X). The results showed that with the extension of grafting reaction time, the quaternary ammonium salt groups on the membrane surface increased and the hydrophilicity was enhanced. Compared with those of the CA membrane, the filtration capacity and antifouling performance of the QCA-X membrane are improved. When the grafting time is 4 h, the water permeability and flux recovery rate of the QCA-4 membrane are increased by 139 and 21.5%, respectively. The QCA-X membrane showed excellent antibacterial performance, and the sterilization rate against S. aureus and E. coli was more than 99.99%. After four repeated antibacterial cycles, the bactericidal rates against S. aureus and E. coli were maintained at about 99.69 ± 0.02 and 99.98 ± 0.02%, respectively, with good antibacterial persistence. Moreover, the QCA-X membrane can effectively inhibit bacterial adhesion. Mild and simple EPDMDAC grafting modifications improve the antibacterial, antifouling, and antibioadhesion properties of the CA membrane, showing its application potential in long-term water treatment, especially in biofouling water treatment.

Cadmium-Rich Plant Powder/PAN/PU Foams with Low Thermal Conductivity.

Treating and utilizing heavy metal enriched plants have become growing problems. In this work, a series of composite foams were made from the powder of Cadmium-rich plant, polyacrylonitrile (PAN) and polyurethane (PU). Test results indicated that the addition of plant powder can not only increase the specific surface area, but also improve the apparent density and thermal stability of the foams. Besides, compared with the foam without plant powder, the powder-added foams exhibited a decreasing trend for thermal conductivity, and the minimum was 0.048 w/(m·k), which indicated that the addition of plant powder can help to enhance the thermal insulation of composite foam. More importantly, the results of leaching experiment showed that the leaching rate of heavy metal cadmium in the composite foam with 50% plant powder content was as low as 0.14% after being immersed in the acidic (pH = 3) solution for 5 days, which implies that the foam materials are very safe. This study provides a new way to realize high value-added resource utilization of heavy metal-enriched plants.

Positively-charged microcrystalline cellulose microparticles: Rapid killing effect on bacteria, trapping behavior and excellent elimination efficiency of biofilm matrix from water environment.

Pathogen and biofilm contamination in aqueous systems leave millions of people at risk of waterborne diseases. Herein, to address this issue, a green and highly efficient strategy is developed to concurrently trap and kill bacteria, eliminate the debris and the existing biofilm matrix in water environment via magnetic microparticles. The particles (TPFPs) were prepared from the in-situ deposition of Fe3O4 nanoparticles onto the surface of antibacterial functionalized microcrystalline cellulose (MCC). Noticeably, TPFPs can completely inactivate both S. aureus and E. coli once contacting for 30 min by disrupting the bacterial membrane. Meanwhile, the MCC-based magnetic particles retained 100% biocidal efficiency against E. coli (5 * 104E. coli/mg particles) during ten recycling procedures without any treatment. More importantly, according to the results of trapping behavior and antibiofilm assays, not only bacteria could be captured by the particles (trapping rate was over 85%), but also the residual debris from dead bacteria and fragmented biofilm was together removed based on the special structure and functions of the antibacterial particles (~ 80%), including extremely rough surfaces, surficial positive charge and magneto-responsive property. This study presents an efficient approach for microorganism management in water system which can be expectantly applied to improve the water safety.

Tea-polyphenol treated skin collagen owns coalesced adaptive-hydration, tensile strength and shape-memory property.

Tea-polyphenol, as non-toxic skincare, even a therapeutic agent, was extensively studied from chemical, biological and physiological perspectives. This study reveals physical intelligences of a tea-polyphenol treated skin collagen (TP-treated SC) through a material-approach. Compared to untreated one, the TP-treated SC shows resistance to over-swelling and dehydration damage. There exists an inflection point in stress value of TP-treated SC below extension of 25%. Such promptly transformation from flexibility to stiffness is self-adaptive stretch behavior. Moreover, TP-treated SC owns water responsive shape-memory property. These effects are attributed to polyphenol as plasticizer with chains crosslinked to multi-sites on collagen-fibers as netpoints. The discovery, mechanism and method, which have not been reported before, may help to develop new shape memory device, skincare products, as well as provides insights into the physiological behavior of collagen contained tissue.

Scalable Spider-Silk-Like Supertough Fibers using a Pseudoprotein Polymer.

Spider silks are tougher than almost all other materials in the world and thus are considered ideal materials by scientists and the industry. Although there have been tremendous attempts to prepare fibers from genetically engineered spider-silk proteins, it is still a very large challenge to artificially produce materials with a very high fracture energy, not to mention the high scaling-up requirements because of the extremely low productivity and high cost levels. Here, a facile spider-silk-mimicking strategy is first reported for preparing scalable supertough fibers using the chemical synthesis route. Supertoughness (≈387 MJ m-3 ), more than twice the reported value of common spider dragline silk and comparable to the value of the toughest spider silk, the aciniform silk of Argiope trifasciata, is achieved by introducing ß-sheet crystals and α-helical peptides simultaneously in a pseudoprotein polymer. The process opens up a very promising avenue for obtaining excellent spider fibers.

Conformational manipulation of scale-up prepared single-chain polymeric nanogels for multiscale regulation of cells.

Folded single chain polymeric nano-objects are the molecular level soft material with ultra-small size. Here, we report an easy and scalable method for preparing single-chain nanogels (SCNGs) with improved efficiency. We further investigate the impact of the dynamic molecular conformational change of SCNGs on cellular interactions from molecular to bulk scale. First, the supramolecular unfoldable SCNGs efficiently deliver siRNAs into stem cells as a molecular drug carrier in a conformation-dependent manner. Furthermore, the conformation changes of SCNGs enable dynamic and precise manipulation of ligand tether structure on 2D biomaterial interfaces to regulate the ligand-receptor ligation and mechanosensing of cells. Lastly, the dynamic SCNGs as the building blocks provide effective energy dissipation to bulk biomaterials such as hydrogels, thereby protecting the encapsulated stem cells from deleterious mechanical shocks in 3D matrix. Such a bottom-up molecular tailoring strategy will inspire further applications of single-chain nano-objects in the biomedical area.

Facile Preparation of Highly Stretchable and Recovery Peptide-Polyurethane/Ureas.

In this work, a new class of highly stretchable peptide-polyurethane/ureas (PUUs) were synthesized containing short ß-sheet forming peptide blocks of poly(γ-benzyl-l-glutamate)-b-poly(propylene glycol)-b-poly(γ-benzyl-l-glutamate) (PBLG-b-PPG-b-PBLG), isophorone diisocyanate as the hard segment, and polytetramethylene ether glycol as the soft phase. PBLG-b-PPG-b-PBLG with short peptide segment length (<10 residues) was synthesized by amine-initiated ring opening polymerization of γ-benzyl-l-glutamate-N-carboxyanhydrides (BLG-NCA), which shows mixed α-helix and ß-sheet conformation, where the percent of ß-sheet structure was above 48%. Morphological studies indicate that the obtained PUUs show ß-sheet crystal and nanofibrous structure. Mechanical tests reveal the PUUs display medium tensile strength (0.25⁻4.6 MPa), high stretchability (>1600%), human-tissue-compatible Young's modulus (226⁻513 KPa). Furthermore, the shape recovery ratio could reach above 85% during successive cycles at high strain (500%). In this study, we report a facile synthetic method to obtain highly stretchable and recovery peptide-polyurethane/urea materials, which will have various potential applications such as wearable and implantable electronics, and biomedical devices.