Immobilization of laccase on magnetic PEGDA-CS inverse opal hydrogel for enhancement of bisphenol A degradation in aqueous solution.

Endocrine disruptors such as bisphenol A (BPA) adversely affect the environment and human health. Laccases are used for the efficient biodegradation of various persistent organic pollutants in an environmentally safe manner. However, the direct application of free laccases is generally hindered by short enzyme lifetimes, non-reusability, and the high cost of a single use. In this study, laccases were immobilized on a novel magnetic three-dimensional poly(ethylene glycol) diacrylate (PEGDA)-chitosan (CS) inverse opal hydrogel (LAC@MPEGDA@CS@IOH). The immobilized laccase showed significant improvement in the BPA degradation performance and superior storage stability compared with the free laccase. 91.1% of 100 mg/L BPA was removed by the LAC@MPEGDA@CS@IOH in 3 hr, whereas only 50.6% of BPA was removed by the same amount of the free laccase. Compared with the laccase, the outstanding BPA degradation efficiency of the LAC@MPEGDA@CS@IOH was maintained over a wider range of pH values and temperatures. Moreover, its relative activity of was maintained at 70.4% after 10 cycles, and the system performed well in actual water matrices. This efficient method for preparing immobilized laccases is simple and green, and it can be used to further develop ecofriendly biocatalysts to remove organic pollutants from wastewater.

Enhancing miR-19a/b induced cardiomyocyte proliferation in infarcted hearts by alleviating oxidant stress and controlling miR-19 release.

Fully restoring the lost population of cardiomyocytes and heart function remains the greatest challenge in cardiac repair post myocardial infarction. In this study, a pioneered highly ROS-eliminating hydrogel was designed to enhance miR-19a/b induced cardiomyocyte proliferation by lowering the oxidative stress and continuously releasing miR-19a/b in infarcted myocardium in situ. In vivo lineage tracing revealed that ∼20.47 % of adult cardiomyocytes at the injected sites underwent cell division in MI mice. In MI pig the infarcted size was significantly reduced from 40 % to 18 %, and thereby marked improvement of cardiac function and increased muscle mass. Most importantly, our treatment solved the challenge of animal death--all the treated pigs managed to live until their hearts were harvested at day 50. Therefore, our strategy provides clinical conversion advantages and safety for healing damaged hearts and restoring heart function post MI, which will be a powerful tool to battle cardiovascular diseases in patients.

Copper nanoparticles incorporated visible light-curing chitosan-based hydrogel membrane for enhancement of bone repair.

Alveolar bone defects caused by tumor, trauma and inflammation can lead to the loss of oral function and complicate denture restoration. Currently, guided bone regeneration (GBR) barrier membranes for repairing bone defect cannot effectively promote bone regeneration due to their unstable degradation rate and poor antibacterial properties. Furthermore, they require additional tailoring before implantation. Therefore, this study developed a visible light-curing hydrogel membrane (CF-Cu) comprising methacrylated carboxymethyl chitosan (CMCS-MA), silk fibroin (SF), and copper nanoparticles (Cu NPs) to address these shortcomings of commercial membranes. The CF-Cu hydrogel, characterized by scanning electron microscopy (SEM), a universal testing machine, and swelling and degradation tests, demonstrated a smooth porous network structure, suitable swelling ratio, biodegradability, and enhanced mechanical strength. Cytotoxicity and hemolysis tests in vitro demonstrated excellent cyto- and hemo-compatibility of the CF-Cu hydrogel extracts. Additionally, evaluation of antibacterial properties in vitro, including colony forming unit (CFU) counts, MTT assays, and live/dead fluorescence staining, showed that the CF-Cu hydrogel exhibited excellent antibacterial properties, inhibiting over 80% of S. aureus, S. mutans, and P. gingivalis with CF-1Cu hydrogel compared to the control group. Moreover, evaluation of osteogenic differentiation of rBMSCs in vitro suggested that the CF-1Cu hydrogel significantly improved alkaline phosphatase (ALP) activity and the mineralization of extracellular matrix, up-regulating the expressions of osteogenesis-related genes (Runx2, ALP, Col-1, OPN and BSP). In summary, these results indicated that CF-1Cu hydrogel exhibited excellent cytocompatibility, antibacterial and osteogenic properties in vitro. Therefore, the CF-1Cu hydrogel holds potential as a viable material for application in GBR procedures aimed at addressing bone defects.

Advancements in the Transdermal Drug Delivery Systems Utilizing Microemulsion-based Gels.

Microemulsion gel, as a promising transdermal nanoparticle delivery system, addresses the limitations of microemulsions and enhances their performance in drug delivery and release. This article aims to discuss the advantages of microemulsion gel, including improved drug bioavailability, reduced drug irritation, enhanced drug penetration and skin adhesion, and increased antimicrobial properties. It explores the methods for selecting microemulsion formulations and the general processes of microemulsion preparation, as well as commonly used oil phases, surfactants, and co-surfactants. Additionally, the biomedical applications of microemulsion gel in treating conditions, such as acne and psoriasis, are also discussed. Overall, this article elucidates the significant potential of microemulsion gel in topical drug delivery, providing insights into future development and clinical applications.

Aided Porous Medium Emulsification for Functional Hydrogel Microparticles Synthesis.

Despite the substantial advancement in developing various hydrogel microparticle (HMP) synthesis methods, emulsification through porous medium to synthesize functional hybrid protein-polymer HMPs has yet to be addressed. Here, the aided porous medium emulsification for hydrogel microparticle synthesis (APME-HMS) system, an innovative approach drawing inspiration from porous medium emulsification is introduced. This method capitalizes on emulsifying immiscible phases within a 3D porous structure for optimal HMP production. Using the APME-HMS system, synthesized responsive bovine serum albumin (BSA) and polyethylene glycol diacrylate (PEGDA) HMPs of various sizes are successfully synthesized. Preserving protein structural integrity and functionality enable the formation of cytochrome c (cyt c) - PEGDA HMPs for hydrogen peroxide (H2O2) detection at various concentrations. The flexibility of the APME-HMS system is demonstrated by its ability to efficiently synthesize HMPs using low volumes (≈50 µL) and concentrations (100 µm) of proteins within minutes while preserving proteins' structural and functional properties. Additionally, the capability of the APME-HMS method to produce a diverse array of HMP types enriches the palette of HMP fabrication techniques, presenting it as a cost-effective, biocompatible, and scalable alternative for various biomedical applications, such as controlled drug delivery, 3D printing bio-inks, biosensing devices, with potential implications even in culinary applications.

Optimization of Vascularized Intestinal Organoid Model.

Vasculature is crucial for maintaining organ homeostasis and metabolism. Although 3D organoids can mimic organ structures and patterns, they still lack vascular systems, limiting the recapitulation of physiological complexities. Although vascularization of organoids has been demonstrated by mixing Matrigel in fibrin, how the mixed gel niche affects endothelial cells (ECs) and organoids remains unclear. Existing protocols rely on fibroblasts to promote vascular network formation. This study explores how varying the ratio of Matrigel in fibrin-Matrigel co-gel affects vascular network formation and intestinal organoid growth. A fine-tuned hydrogel is developed by adding aprotinin and 15% Matrigel in fibrin. Medium for co-culturing ECs and organoids is modified with basic fibroblast growth factor (bFGF) and heparin. In combination with fine-tuned hydrogel and modified medium, vascular network formation and organoid vascularization are successfully generated in the absence of fibroblast. Furthermore, structural cues and pore architectures are critical for angiogenesis and vascularization. By incorporating engineered thick collagen fiber bundles into the system, vascular network formation is guided by bundle architectures, enhancing interactions between vascular networks and organoids. The results demonstrate an optimized system that advances tissue and organoid vascularization by combining fiber bundles with fine-tuned hydrogel and modified medium.

Rhein-chitosan in situ hydrogel promotes wound healing in diabetic mice.

Chronic inflammation and infection often lead to delayed healing in skin wounds of patients with diabetes, presenting a significant challenge in clinical wound repair. In an effort to tackle this issue, we explored the utilization of the natural compounds Rhein and chitosan in the creation of a crosslinked in situ gel. Developed as Rhein-chitosan in situ hydrogel (CS-Rh gel), this formulation has the ability to gel at body temperature, making it suitable for irregular wounds of varying shapes. Our experimental investigations have demonstrated its excellent biocompatibility, controlled release of Rhein, biodegradability, anti-inflammatory properties, antibacterial effect, as well as its ability to enhance keratinocyte proliferation and migration. Furthermore, in vivo studies have confirmed that CS-Rh gel can effectively mitigate tissue inflammation, promote collagen deposition, and significantly accelerate wound healing in diabetic mice within a short timeframe of two weeks. Consequently, this innovative approach holds promise as a viable therapeutic strategy for supporting the healing of diabetic wounds in a clinical setting.

Ligand-selective turn-off sensing, harvesting and post-adsorptive use of Dy(III) and Yb(III) by intrinsically fluorescent flower-shaped Gum Acacia-grafted hydrogels.

Rare earth metals (REMs), such as Dysprosium (Dy) and Ytterbium (Yb), have experienced unprecedented demand in recent times due to their applications in high-end technologies. REMs are found only in select geographic locations placing tremendous economic constraints on their use. In this work, we have developed Gum Acacia-grafted hydrogels (GmAc-FluoroTerPs) that are capable of selective detection and capture of Dy and Yb. The intrinsically blue fluorescent polymer hydrogel GmAc-FluoroTerP has been optimized for Dy(III) and Yb(III) specific quenching, enabling limit of detection of the REMs at 0.13 nM and 60.8 pM, respectively. A comprehensive structural characterization of the fluorescent hydrogel has been performed via NMR, FTIR, XPS, EPR, TGA, XRD, TEM, SEM, EDX, TCSPC, and DLS. In addition to an in situ generated fluorophore, GmAc-FluoroTerP displays a distinctive aggregation induced emission enhancement in mixed solvents. The complexation of Dy(III)/Yb(III) with GmAc-FluoroTerP hydrogel has been characterized by XPS, TCSPC, and logic gate analyses, and the adsorptive capacity for Dy(III) and Yb(III) are found to be best reported till date as 125.57 mg g-1 and 102.27 mg g-1, respectively. Desorption at acidic pH allows recovery of the REMs. We also report semiconducting behaviour of the native fluorescent hydrogel, that is enhanced upon adsorptive capture of Dy(III) and Yb(III), with calculated band gaps at 1.37, 0.77, and 0.49 eV, respectively. The convergent sensing, capture, and reuse of Dy(III) and Yb(III) presented in this work promises a hitherto unreported template for application on other REMs.

Fabrication and characterization of biodegradable hydrogel beads of guar gum for the removal of chlorpyrifos pesticide from water.

A new guar gum hydrogel beads were fabricated by dropping method from an aqueous solution of guar gum (GG) using ammonium persulphate and polyethylene glycol as initiator and crosslinker respectively, for the adsorption of chlorpyrifos (CP) from water. The semi-crystalline nature of the synthesized beads was confirmed by FESEM analysis. The TGA studies implied that the beads were thermally stable up to 600 °C. The maximum swelling ratio of 1400 gg-1 was attained at pH 9.2 and 80 min. The evidence of a strong absorption band was found in FTIR spectrum at 584 cm-1 due to -P=S of the adsorbed pesticide CP. The maximum adsorption of CP was found to be 220.97 mgg-1. The adsorption followed pseudo second-order kinetics and Langmuir adsorption isotherm with regression coefficients 0.9998 and 0.9938 which followed the chemisorption process. It is due to the hydrolysis of CP at pH 9.2 to yield 3,5,6-trichloropyridinol which in turn reacts with the carboxylic group present in GG giving -N-C=O linkage. A -ΔG indicates that the process is spontaneous and involves chemisorption which is thermodynamically and kinetically favorable and a -ΔH value (-10.37 kJ/mol) suggests that the adsorption is exothermic.

Enhanced specific surface area and mechanical property of silk nanofibers aerogel for potential hemostasis applications.

Biopolymer aerogel is a new type of material with potential applications in the biomedical field. Silk fibroin is of particular interest as a raw material with good biocompatibility and degradable. However, the low mechanical strength and small specific surface area of silk fibroin aerogels limit its further development. Herein, a fast water absorption, highly specific surface area and mechanically strong of aerogels were prepared using low crystal silk fibroin nanofibers (SNF), sol-gel process, solvent exchange and supercritical carbon dioxide (CO2) drying method. The resulting Aero-Sc displayed highly specific surface area (251 m2/g), porosity (97.6 %) and water absorption capacity (1200 %). Furthermore, with rapid water absorption and stronger erythrocyte adhesion, the Aero-Sc showed highly effective hemostasis in vitro. In vivo, animal experiments on rat liver hemorrhage model confirmed that SNF aerogels have a less blood loss (312 ± 29 mg) and faster hemostatic time (92 ± 13 s) than commercially gelatin sponge (p < 0.05). The unique properties of silk fibroin nanofibers aerogel developed in this study has great potential to be a safe and effective hemostatic medical device.

Engineering bi-layered skin-like nanopads with electrospun nanofibers and chitosan films for promoting fibroblast infiltration in tissue regeneration and wound healing.

This study presents an innovative bi-layered three-dimensional skin-like nanopad (SLN) engineered for skin tissue regeneration. The SLN integrates a mechanically supportive polycaprolactone nanofibrous layer with a functional chitosan hydrogel film, mimicking natural skin. Our SLN exhibits superior flexibility, with a maximum elongation of 751.71 ± 125 % and exceptional porosity of 95 ± 4.5 %, ensuring effective exudate management due to its high water uptake capacity (4393 ± 72 %). FTIR analysis confirmed a distinctive fiber-hydrogel network within the SLN, which serves as a barrier against Staphylococcus aureus and Pseudomonas aeruginosa infiltration. In vitro cell viability assays with the human fibroblast have consistently demonstrated that 3D bi-layered SLN enhances fibroblast attachment, infiltration, and proliferation by 150 ± 20 %. In vivo studies in a rat model demonstrated significantly faster wound closure, with 60 % on day 7 and 87 % on day 10, compared to the 30 % and 60 % in controls, highlighting the efficacy of SLN. By mimicking the architecture of native skin, this biomimetic bi-layered SLN scaffold provides flexibility and support while accelerating in vivo wound closure by promoting fibroblast proliferation and infiltration. Customizable in size, depth, and shape, the engineered SLN has emerged as a promising platform for advanced wound care and tissue engineering.

Synthesis and characterization of injectable thermosensitive hydrogel based on Pluronic-grafted silk fibroin copolymer containing hydroxyapatite nanoparticles as potential for bone tissue engineering.

Injectable hydrogels are promising for bone tissue engineering due to their minimally invasive application and adaptability to irregular defects. This study presents the development of pluronic grafted silk fibroin (PF-127-g-SF), a temperature-sensitive graft copolymer synthesized from SF and modified PF-127 via a carbodiimide coupling reaction. The PF-127-g-SF copolymer exhibited a higher sol-gel transition temperature (34 °C at 16 % w/v) compared to PF-127 (23 °C), making it suitable for injectable applications. It also showed improved flexibility and strength, with a yielding point increase from <10 % to nearly 30 %. Unlike PF-127 gel, which degrades within 72 h in aqueous media, the PF-127-g-SF copolymer maintained a stable gel structure for over two weeks due to its robust crosslinked hydrogel network. Incorporating hydroxyapatite nanoparticles (n-HA) into the hydrogel reduced pore size and decreased swelling and degradation rates, extending structural stability to four weeks. Increasing n-HA concentration from 0 % to 20 % reduced porosity from 80 % to 66 %. Rheological studies indicated that n-HA enhanced the scaffold's strength and mechanical properties without altering gelation temperature. Cellular studies with MG-63 cells showed that n-HA concentration influenced cell viability and mineralization, highlighting the scaffold's potential in bone tissue engineering.

Biomimetic mineralization of hydrated magnesium carbonate for hydrogel reinforcement and heavy metal adsorption.

With excessive Mn(Ⅱ) and Cu(Ⅱ) pollution in aquatic environments posing potential health risks to inhabitants, the emergence of carbon capture, utilization and storage (CCUS) technology has promoted the improvement of heavy metal remediation technologies. Using hydrothermal sediment as a crystal seed, rhamnolipid was used to mediate biomimetic mineralization to prepare hydrated magnesium carbonate (HMC) composites to enhance the Mn(Ⅱ)/Cu(Ⅱ) adsorption performance of alginate hydrogels. Hydrothermal sediment is beneficial for accelerating biomimetic mineralization, while rhamnolipid can induce a crystalline phase transformation from dypingite to nesquehonite. The addition of sediment significantly enhanced the compressive mechanical properties and thermal stability of the hydrogels. The adsorption performances of the nesquehonite and dypingite hydrogels were better for Mn(II) and Cu(II), respectively. An increase in the amount of sediment improved the adsorption of Cu(II) by the hydrogels appropriately, resulting in stronger selectivity for Cu(II). The adsorption of Mn(II) and Cu(II) on the hydrogel beads was thermodynamically spontaneous. The inhibitory effects of sodium dodecyl benzene sulfonate (SDBS), fulvic acid (FA) and alginate on Cu(II) adsorption were more obvious than those of bovine serum albumin (BSA). Both the complexation of functional groups on alginate and mineralization by HMC participated in the adsorption of Mn(II) and Cu(II).

Effects of Enteromorpha prolifera sulfated polysaccharide and aluminium ion addition on the multifunctional property of conductive hydrogel for wearable strain sensing.

Although introducing Enteromorpha prolifera sulfated polysaccharide (SPEP) enhances the mechanical properties of hydrogels significantly, little is known about the effects of polysaccharide and ion addition on morphological and physicochemical properties of conductive hydrogel. Therefore, the Poly (acrylic acid)/SPEPn/Al3+m (PAA/SPEPn/Al3+m) hydrogels with different SPEP and Al3+ addition were synthesized by simple one-pot method. The porosity, tensile strength, and swelling ration increased, while compressive strength, elongation at break, self-healing, self-adhesion properties increased first and then decreased as SPEP addition increased from 0 % to 3.80 %. The Al3+ addition increased from 0.08 % to 0.30 %, both tensile and compressive strength increased first and then decreased, while elongation at break kept increasing. Unexpectedly, both increasing SPEP and Al3+ addition reduced the electrical conductivity, while SPEP increased the gauge factor of hydrogel. The hydrogel exhibited optimal comprehensive properties when SPEP and Al3+ addition were 2.31 % and 0.24 %, respectively. The PAA/SPEP2.31%/Al3+0.24% hydrogel showed high tensile strength (107.60 kPa), elongation at break (2426.67 %), strain self-healing rate (81.87 %), adhesion strength (21.61 kPa), and conductivity (3.60 S/m). Overall, the properties of PAA/SPEPn/Al3+m hydrogels can be regulated through tailoring SPEP and Al3+ addition, which can be used as on-demand strategy to improve the performance of PAA/SPEPn/Al3+m hydrogels for each application.

In Situ-Forming, Bioorthogonally Cross-linked, Nanocluster-Reinforced Hydrogel for the Regeneration of Corneal Defects.

Corneal defects can lead to stromal scarring and vision loss, which is currently only treatable with a cadaveric corneal transplant. Although in situ-forming hydrogels have been shown to foster regeneration of the cornea in the setting of stromal defects, the cross-linking, biomechanical, and compositional parameters that optimize healing have not yet been established. This, Corneal defects are also almost universally inflamed, and their rapid closure without fibrosis are critical to preserving vision. Here, an in situ forming, bioorthogonally cross-linked, nanocluster (NC)-reinforced collagen and hyaluronic acid hydrogel (NCColHA hydrogel) with enhanced structural integrity and both pro-regenerative and anti-inflammatory effects was developed and tested within a corneal defect model in vivo. The NCs serve as bioorthogonal nanocross-linkers, providing higher cross-linking density than polymer-based alternatives. The NCs also serve as delivery vehicles for prednisolone (PRD) and the hepatocyte growth factor (HGF). NCColHA hydrogels rapidly gel within a few minutes upon administration and exhibit robust rheological properties, excellent transparency, and negligible swelling/deswelling behavior. The hydrogel's biocompatibility and capacity to support cell growth were assessed using primary human corneal epithelial cells. Re-epithelialization on the NCColHA hydrogel was clearly observed in rabbit eyes, both ex vivo and in vivo, with expression of normal epithelial biomarkers, including CD44, CK12, CK14, α-SMA, Tuj-1, and ZO-1, and stratified, multilayered morphology. The applied hydrogel maintained its structural integrity for at least 14 days and remodeled into a transparent stroma by 56 days.

Antibiotic Nanoparticles-Loaded Wound Dressings Against Pseudomonas aeruginosa's Skin Infection: A Systematic Review.

Pseudomonas aeruginosa (P. aeruginosa) is a common nosocomial pathogen that can cause severe infections in critically ill patients. Due to its resistance to multiple drugs, it is challenging to treat, which can result in serious illness and death. Conventional treatments for infected wounds often involve the topical or systemic application of antibiotics, which can lead to systemic toxicity and the development of drug resistance. The combination of wound dressings that promote wound healing with nanoparticles (NPs) represents a revolutionary strategy for optimizing the safety and efficacy of antibiotics. This review assesses a systematic search to identify the latest approaches where the evaluation of wound dressings loaded with antibiotic NPs is conducted. The properties of NPs, the features of wound dressings, the antimicrobial activity and biocompatibility of the different strategies are analyzed. The results indicate that most research in this field is focused on dressings loaded with silver NPs (57.1%) or other inorganic materials (22.4%). Wound dressings loaded with polymeric NPs and carbon-based NPs represent 14.3% and 6.1% of the evaluated studies, respectively. Nevertheless, there are no clinical trials that have evaluated the efficacy of NPs-loaded wound dressings in patients. Further research is required to ensure the safety of these treatments and to translate the findings from the bench to the bedside.

Structurally decoupled hyaluronic acid hydrogels for studying matrix metalloproteinase-mediated invasion of metastatic breast cancer cells.

In recent years, polymeric hydrogels have been employed to investigate cancer cell-extracellular matrix (ECM) interactions in vitro. In the context of breast cancer, cancer cells are known to degrade the ECM using matrix-metalloproteinases (MMPs) to support invasion resulting in disease progression. Polymeric hydrogels incorporating MMP-cleavable peptides have been employed to study cancer cell invasion, however, the approaches employed to incorporate these peptides often change other hydrogel properties. This underscores the need for decoupling hydrogel properties while incorporating MMP-cleavable peptides. Herein, we report structurally decoupled hyaluronic acid (HA) hydrogels formulated using varying ratios of a biologically sensitive MMP-cleavable peptide and an insensitive counterpart (Dithiothreitol (DTT) or polyethylene glycol dithiol (PEGDT)) to study MMP-mediated metastatic breast cancer cell invasion. Rheological, swelling ratio, estimated mesh size, and permeability measurements showed similar mechanical and physical properties for hydrogels crosslinked with different DTT (or PEGDT)/MMP ratios. However, their degradation rate in the presence of collagenase correlated with the ratio of MMP-cleavable peptide. Encapsulated metastatic breast cancer spheroids in HA hydrogels with MMP sensitivity exhibited increased invasiveness compared to those without MMP sensitivity after 14 days of culture. Overall, such structurally decoupled HA hydrogels provide a platform to study MMP-mediated breast cancer cell invasion in vitro.

Accelerated, injectable, self-healing, scarless wound dressings using rGO reinforced dextran/chitosan hydrogels incorporated with PDA-loaded asiaticoside.

The process of wound healing is intricate and complex, necessitating the intricate coordination of various cell types and bioactive molecules. Despite significant advances, challenges persist in achieving accelerated healing and minimizing scar formation. Herein, a multifunctional hydrogel engineered via dynamic Schiff base crosslinking between oxidized dextran and quaternized chitosan, reinforced with reduced graphene oxide (rGO) is reported. The resulting OQG hydrogels demonstrated injectability to aid in conforming to irregular wound geometries, rapid self-healing to maintain structural integrity and strong adhesion for intimate integration with wound beds. Moreover, the developed hydrogels possessed intrinsic antioxidant and antibacterial activities, mitigating inflammation and preventing infection. The incorporation of conductive rGO further facilitated the transmission of endogenous electrical signals, stimulating cell migration and tissue regeneration. In addition, the polydopamine-encapsulated asiaticoside (AC@PDA) nanoparticles were encapsulated in OQG hydrogels to reduce scar formation during in vivo evaluations. In vitro results confirmed the histocompatibility of the hydrogels to promote cell migration. The recovery of the full-thickness rat wounds revealed that these designed OQG hydrogels with the incorporation of AC@PDA nanoparticles could accelerate wound healing, reduce inflammation, facilitate angiogenesis, and minimize scarring when implemented. This multifunctional hydrogel system offers a promising strategy for enhanced wound management and scarless tissue regeneration, addressing the multifaceted challenges in wound care.

On-demand bactericidal and self-adaptive antifouling hydrogels for self-healing and lubricant coatings of catheters.

Catheter-related infections are one of the most common nosocomial infections with increasing morbidity and mortality, and robust antibacterial or antifouling catheter coatings remain great challenges for long-term implantation. Herein, multifunctional hydrogel coatings were developed to provide persistent and self-adaptive antifouling and antibacterial effects with self-healing and lubricant capabilities. Polyvinyl alcohol (PVA) with ß-cyclodextrin (ß-CD) grafts (PVA-Cd) and 4-arm polyethylene glycol (PEG) with adamantane and quaternary ammonium compound (QAC) terminals (QA-PEG-Ad) were crosslinked through host-guest recognitions between adamantane and ß-CD moieties to acquire PVEQ coatings. In response to bacterial infections, QACs exhibit reversible transformation between zwitterions (pH 7.4) and cationic lactones (pH 5.5) to generate on-demand bactericidal effect. Highly hydrophilic PEG/PVA backbones and zwitterionic QACs build a lubricate surface and decrease the friction coefficient 10 times compared with that of bare catheters. The antifouling hydrated layer significantly inhibits blood protein adsorption and platelet activation and reveals negligible hemolysis and cytotoxicity. The dynamic host-guest crosslinking achieves full self-healing of cracks in PVEQ hydrogels, and the mechanical profiles were recovered to over 90% after rejuvenating the broken hydrogels, exhibiting a long-term stability after mechanical stretching, twisting, knotting and compression. After subcutaneous implantation and local bacterial infection, the retrieved PVEQ-coated catheters display no tissue adhesion and 3 log folds lower bacterial number than that of bare catheters. PVEQ coatings effectively prevent the repeated bacterial infections and there are few inflammatory reactions in the surrounding tissue, while substantial lymphoid infiltration and inflammatory cell aggregation occur in muscle tissues around the bare catheter. Thus, this study demonstrates a catheter coating strategy by on-demand bactericidal, self-adaptive antifouling, self-healing and lubricant hydrogels to address medical devices-related infections. STATEMENT OF SIGNIFICANCE: It is estimated over two billion peripheral intravenous catheters are annually used in hospitals around the world, and catheter-associated infection has become a great clinical challenge with rapidly rising morbidity and mortality. Surface coating is considered a promising approach, but substantial challenges remain in the development of coatings that simultaneously satisfy both anti-fouling and antibacterial attributes. Even more, few attempts have been made to design mechanically robust coatings and reversible antibacterial or antifouling capabilities, which are critical for long-term medical implants. To address these challenges, we propose a concise strategy to develop hydrogel coatings from commercially available poly(ethylene glycol) and polyvinyl alcohol. In addition to self-healing and lubricant capabilities, the reversible conversion between zwitterionic and cationic lactones of quaternary ammonium compounds enables on-demand bactericidal and self-adaptive antifouling effects.

Bioinspired Self-Growing Layered Hydrogel Enabled by Catechol Chemistry-Mediated Interfacial Catalytic System.

Tissue-inspired layered structural hydrogel has attracted increasing attention in artificial muscle, wound healing, wearable electronics, and soft robots. Despite numerous efforts being devoted to developing various layered hydrogels, the rapid and efficient preparation of layered hydrogels remains challenging. Herein, inspired by the self-growth concept of living organisms, an interfacial catalytic self-growth strategy based on catechol chemistry-mediated self-catalytic system of preparing layered hydrogels is demonstrated. Typically, the tannic acid-metal ion (e.g., TA-Fe3+) complex embedded in the hydrogel substrate would catalytically trigger rapid solid-liquid interfacial polymerization to grow the hydrogel layer without bulk solution polymerization. The self-growth process can be finely controlled by changing the growth time, the molar ratio of Fe3+/TA, and so on. The strategy is applicable to prepare various layered hydrogels as well as complex layered hydrogel patterns, allowing the customization of the physicochemical properties of the hydrogel. In addition, the self-adhesive layered hydrogel was prepared and can be utilized as a wearable strain sensor to monitor physiological activities and human motions. The demonstrated interfacial catalytic self-growth strategy will provide a route to design and fabricate layered hydrogel materials.