Mussel-inspired Strategy Research Articles

Mussel-inspired ionic hydrogel for tactile perception: Toward versatility, robustness and sustainability

The ever-growing wearable and implantable medical devices have spawned an urgent demand for integrating tactile sensors and portable power sources into a single device. However, identifying a suitable material that balances electronic and mechanical performance to simultaneously meet the requirements of high biocompatibility, elasticity, conductivity, and versatility for such soft electronic applications remains a challenge. Here, highly conductive and robust ionic hydrogel is synthesized via a mussel-inspired strategy, where cellulose nanofibers (CNFs) and ZIF-8 particles are introduced into poly(acrylic acid-co-2-(methacryloyloxy)ethyl trimethylammonium chloride) (PADH) matrix for achieving mechanical reinforcement. Besides adhesive strengths of 30.26 kPa, strong hydrogen-bonding central to the embedded CNFs/ZIF-8 joint induces densely cross-linked tough panel points and soft-hard layered network structure that provide tensile strength of 110 kPa, elongation at break up to 697 % (increased by ∼2.2 times and ∼1.9 times, respectively) and compressive strength of 984 kPa. Excellent self-healing (89 % within 12 h) and self-adhesion capabilities (adhesion strength of about 30.26 kPa) are also witnessed, which can be attributed to the reversibility of the abundant hydrogen bonds. Meanwhile, the ion-rich tunnels promoted by the migration of IL/Gly/H2O ternary solvent system (EgHTS) not only significantly enhance the ionic conductivity, but also improve temperature tolerance and provide prolonged resistance to dehydration. The dynamical balance of the electric double layers at the CNF-ZIF-PADH interface leads to highly stable and durable hybrid triboelectric-piezoresistive sensors that are capable identifying both the physical characteristic of dynamic objects and static forces while harvesting mechanical energy, thus enabling versatile, robust, temperature-tolerant conductive hydrogels for self-powered soft electronics.

Preparation strategies of mussel-inspired chitosan-based biomaterials for hemostasis.

Chitosan (CS) has been extensively studied in wound care for its intrinsic hemostatic and antibacterial properties. However, CS has limiting hemostasis applications on account of its drawbacks such as poor adhesion in humid environments and water solubility at neutral pH. CS-based biomaterials, inspired by mussel-adhesive proteins, serve as a suggested platform by biomedical science. The reports show that the mussel-inspired CS-based hemostatic structure has negligible toxicity and excellent adhesiveness. Biomedicine has witnessed significant progress in the development of these hemostatic materials. This review summarizes the methods for the modification of CS by mussel-inspired chemistry. Moreover, the general method for preparation of mussel-inspired CS-based biomaterials is briefly discussed in this review. This work is expected to give a better understanding of opportunities and challenges of the mussel-inspired strategy for the functionalization of CS-based biomaterials in hemostasis and wound healing. This review is hoped to provide an important perspective on the preparation of mussel-inspired CS-based hemostatic materials.

Polydopamine-functionalized natural cellulosic Juncus effusus fiber for efficient and eco-friendly Cr (VI) removal from wastewater

Biomass adsorbents have received extensive attention for the removal of heavy metals, but most of them had very limited adsorption capacity or needed to be modified with environmentally unfriendly chemicals to achieve acceptable performance. In this study, a green biomass adsorbent was fabricated using an abundant natural cellulosic Juncus effusus (JE) fiber and natural melanin polydopamine (PDA) through a simple mussel-inspired polymerization strategy. JE's unique hollow three-dimensional network structure provided an ideal scaffold substrate with abundant sites for dopamine polymerization deposition. This enabled the modified PDA@JE fibers to be rich in amino, hydroxyl, and other active adsorption sites, thereby endowing the PDA@JE fiber adsorbent with a promising Cr (VI) adsorption capacity of up to 145.8 mg / g. This capacity was significantly higher than that of most previously reported biomass-based adsorbents. Furthermore, 10–20 times the concentration of common interfering ions such as Ca2+, Cd2+, Cu2+, NO3-, Cl-, SO42- and PO43- had little effect on the adsorption efficiency. This study provided a green and general mussel-inspired strategy for preparing effective biomass adsorbent, offering a promising approach for utilizing natural cellulosic fibers in eco-friendly applications.

Electroactive Hydrogels with Photothermal/Photodynamic Effects for Effective Wound Healing Assisted by Polydopamine-Modified Graphene Oxide.

Antibacterial hydrogel wound dressings have attracted considerable attention in recent years. However, bacterial infections can occur at any point during the wound-healing process. There is a demand for hydrogels that possess on-demand antibacterial and excellent wound repair properties. Herein, we report a near-infrared (NIR)-light-responsive indocyanine green (ICG)-loaded polydopamine (PDA)-mediated graphene oxide (PGO) and amorphous calcium phosphate (CaP)-incorporated poly(vinyl alcohol) (PVA) hydrogel using a mussel-inspired approach. PGO was reduced by PDA, which endowed the hydrogel with electroactivity and provided abundant sites for loading ICG. Amorphous CaP was formed in situ in the PVA hydrogel to enhance its mechanical properties and biocompatibility. Taking advantage of the high photothermal and photodynamic efficiency of ICG-PGO, the ICG-PGO-CaP-PVA hydrogel exhibited fascinating on-demand antibacterial activity through NIR light irradiation. Moreover, the thermally induced gel-sol conversion of PVA accelerated the release of Ca ions and allowed the hydrogel to adapt to irregular wounds. Meanwhile, PGO endows the hydrogel with conductivity and cell affinity, which facilitate endogenous electrical signal transfer to control cell behavior. In vitro and in vivo studies demonstrated that the ICG-PGO-CaP-PVA hydrogel exhibited a strong tissue repair activity under NIR light irradiation. This mussel-inspired strategy offers a novel way to design hydrogel dressings for wound healing.

A hyaluronic acid/silk fibroin/poly-dopamine-coated biomimetic hydrogel scaffold with incorporated neurotrophin-3 for spinal cord injury repair

Bio-factor stimulation is essential for axonal regeneration in the central nervous system. Thus, persistent and efficient factor delivery in the local microenvironment is an ideal strategy for spinal cord injury repair. We developed a biomimetic hydrogel scaffold to load biofactors in situ and release them in a controlled way as a promising therapeutic modality. Hyaluronic acid and silk fibroin were cross-linked as the basement of the scaffolds, and poly-dopamine coating was used to further increase the loading of factors and endow the hydrogel scaffolds with ideal physical and chemical properties and proper biocompatibility. Notably, neurotrophin-3 release from the hydrogel scaffolds was prolonged to 28 days. A spinal cord injury model was constructed for hydrogel scaffold transplantation. After eight weeks, significant NF200-positive nerve fibers were observed extending across the glial scar to the center of the injured area. Due to the release of neurotrophin-3, spinal cord regeneration was enhanced, and the cavity area of the injury graft site and inflammation associated with CD68 positive cells were reduced, which led to a significant improvement in hind limb motor function. The results show that the hyaluronic acid/silk fibroin/poly-dopamine-coated biomimetic hydrogel scaffold achieved locally slow release of neurotrophin-3, thus facilitating the regeneration of injured spinal cord. Statement of significanceHydrogels have received great attention in spinal cord regeneration. Current research has focused on more efficient and controlled release of bio-factors. Here, we adopted a mussel-inspired strategy to functionalize the hyaluronic acid/silk fibroin hydrogel scaffold to increase the load of neurotrophin-3 and extend the release time. The hydrogel scaffolds have ideal physiochemical properties, proper release rate, and biocompatibility. Owing to the continuous neurotrophin-3 release from implanted scaffolds, cavity formation is reduced, inflammation alleviated, and spinal cord regeneration enhanced, indicating great potential for bio-factor delivery in soft tissue regeneration applications.

Development of chitosan/konjac glucomannan/tragacanth gum tri-layer food packaging films incorporated with tannic acid and ε-polylysine based on mussel-inspired strategy

Constructing biodegradable food packaging with good mechanics, gas barrier and antibacterial properties to maintain food quality is still challenge. In this work, mussel-inspired bio-interface emerged as a tool for constructing functional multilayer films. Konjac glucomannan (KGM) and tragacanth gum (TG) with physical entangled network are introduced in the core layer. Cationic polypeptide ε-polylysine (ε-PLL) and chitosan (CS) producing cationic-π interaction with adjacent aromatic residues in tannic acid (TA) are introduced in the two-sided outer layer. The triple-layer film mimics the mussel adhesive bio-interface, where cationic residues in outer layers interact with negatively charged TG in the core layer. Furthermore, a series of physical tests showed excellent performance of triple-layer film with great mechanical properties (tensile strength (TS): 21.4 MPa, elongation at break (EAB): 7.9 %), UV-shielding (almost 0 % UV transmittance), thermal stability, water, and oxygen barrier (oxygen permeability (OP): 1.14 × 10−3 g/m s Pa and water vapor permeability (WVP): 2.15 g mm/m2 day kPa). In addition, the triple-layer film demonstrated advanced degradability, antimicrobial functions, and presented good moisture-proof performance for crackers, which can be potentially applied as dry food packaging.

Mussel-inspired cationic chitosan-based flocculants with floc enlarging capacity for efficient removal of anionic dye

Biomass-based flocculants have been widely studied and applied to wastewater treatment due to their environmental friendliness. However, these flocculants tend to generate flocs with small size and lead to difficult solid-liquid separation after the flocculation. The key to solving the floc size problem is enhancing intermolecular or intramolecular interaction forces by changing the molecular structure and functional groups of flocculants. Herein, we developed a mussel-inspired cationic biomass flocculant by functionalizing chitosan (CS) with cation component acryloyloxyethyltrimethyl ammonium chloride (DAC) and mussel-inspired monomer N-2-(3, 4-dihydroxyphenethyl) acrylamide (DAA) through free radical polymerization. The prepared flocculant could provide multiple interaction forces such as electrostatic interaction, cation-π interaction, π −π stacking, and hydrogen bonding to pollutants. As a result, the spent CS-g-p (DAC-co-DAA) flocculant generate dye-containing flocs with dramatically increased size when compared with its counterpart CS-g-pDAC without catechol groups and are capable to realize more than 95% removal efficiency towards organic dyes such as MB and CR over a broad pH range from 3 to 9. This study provides some insights in how to apply this mussel-inspired strategy to develop environmentally friendly biomass-derived flocculants with floc enlarging capacity to treat organic wastewaters in wide pH range.

Multi-crosslinked hydrogels with strong wet adhesion, self-healing, antibacterial property, reactive oxygen species scavenging activity, and on-demand removability for seawater-immersed wound healing.

In general, seawater-immersed wounds are associated with tissue necrosis, infection, prolonged healing period, and high mortality because of high salinity, hyperosmosis, and the presence of various pathogenic bacteria in seawater. However, current wound dressings can hardly achieve strong and stable wet adhesion and antibacterial properties, thus limiting their application to seawater-immersed wounds. Here a multifunctional hydrogel (OD/EPL@Fe) comprising catechol-modified oxidized hyaluronic acid (OD), ε-poly-L-lysine (EPL), and Fe3+ was prepared primarily through Schiff-base reaction, metal chelation, cation-π, and electrostatic interaction. The hydrogel with high wet adhesion (about 78 kPa) was achieved by combining the mussel-inspired strategy, dehydration effect, and cohesion enhancement, which is higher than that of commercial fibrin glues and cyanoacrylate glues. Meanwhile, the hydrogel can eliminate Marine bacteria (V. vulnificus and P. aeruginosa) and inhibit their biofilm formation. In addition, the hydrogel demonstrated injectability, self-healing, reactive oxygen species scavenging activity, photothermal effect, seawater isolation, on-demand removal, and hemostatic properties. In vivo results showed that the hydrogel had good adhesion to dynamic wounds in a rat neck full-thickness skin wound model. In particular, the hydrogel exhibited antibacterial, anti-inflammatory, and antioxidant properties in a rat seawater-immersed infected wound model and accelerated the reconstruction of skin structure and functions. The results demonstrated that the OD/EPL@Fe would be a potential wound dressing for seawater-immersed wound healing. STATEMENT OF SIGNIFICANCE: A multifunctional OD/EPL@Fe hydrogel has been prepared for the treatment of seawater-immersed wounds. The hydrogel with high wet adhesion was achieved by combining the mussel-inspired strategy, dehydration effect, and cohesion enhancement. The results revealed that the wet adhesion value of hydrogel was about eight times greater than commercial fibrin glues and 1.5 times greater than commercial cyanoacrylate glues. The hydrogel can be easily removed after being sprayed with deferoxamine mesylate. Notably, the inherent antimicrobial material of the hydrogel combined with the photothermal effect can eliminate marine bacteria and inhibit their biofilm formation. Moreover, the hydrogel can accelerate the healing of seawater-immersed infected wound on mice.

Carboxymethyl chitosan/sodium alginate hydrogels with polydopamine coatings as promising dressings for eliminating biofilm and multidrug-resistant bacteria induced wound healing

Microorganisms induced wound infection and the accompanying excessive inflammatory response is the daunting problems in wound treatment. Due to the lack of corresponding biological functions, traditional wound dressings cannot effectively protect the wound and are prone to induce local infection, excessive inflammation, and vascular damage, resulting in prolonged unhealing. Here, a mussel-inspired strategy was adopted to prepare a multifunctional hydrogel created by H2O2/CuSO4-induced rapid polydopamine (PDA) deposition on carboxymethyl chitosan (CMC)/sodium alginate (Alg) based hydrogel, termed as CAC/PDA/Cu(H2O2). The prepared CAC/PDA/Cu(H2O2) hydrogel features excellent biocompatibility, adequate mechanical properties, and good degradability. Moreover, the CAC/PDA/Cu(H2O2) hydrogel can not only realize antibacterial, and anti-inflammatory effects, but also promote angiogenesis to accelerate wound healing in vitro thanks to the composite PDA/Cu(H2O2) coatings. Significantly, CAC/PDA/Cu(H2O2) hydrogel illustrates excellent therapeutic effects in Methicillin-resistant Staphylococcus aureus (MRSA) induced-rat infection models, which can efficiently eliminate MRSA, dramatically reduce inflammatory expression, promote angiogenesis, and ultimately shorten the wound healing time. CAC/PDA/Cu(H2O2) hydrogel exhibited the best wound healing rate on days 7 (80.63 ± 2.44 %), 11 (92.45 ± 2.26 %), and 14 (97.86 ± 0.66 %). Thus, the multifunctional hydrogel provides a facile and efficient approach to wound management and represents promising potential in the therapy for wound healing.

Mussel-Inspired Surface Modification of α-Zirconium Phosphate Nanosheets for Anchoring Efficient and Reusable Ultrasmall Au Nanocatalysts

The shortage of powerful functionalities on scalable α-zirconium phosphate (ZrP) materials blocks the facile preparation of highly dispersed and immobilized metal nanocatalysts. We herein present a mild and facile mussel-inspired strategy based on polydopamine (PDA) for the surface modification of ZrP, and hence, the generation of powerful functionalities at a high density for the straightforward reduction of chloroauric acid to Au nanoparticles (AuNPs) and the immobilization of AuNPs. The resulting ternary ZrP@PDA/Au exhibited ultra-small AuNPs with a particle size of around 6.5 nm, as estimated based on TEM images. Consequently, the ZrP@PDA/Au catalyst showed significant activity in the catalytic conversion of 4-nitrophenol (4NP) to 4-aminophenol (4AP), a critical transformation reaction in turning the hazard into valuable intermediates for drug synthesis. The PDA was demonstrated to play a critical role in the fabrication of the highly efficient ZrP@PDA/Au catalyst, far outperforming the ZrP/Au counterpart. The turnover frequency (TOF) achieved by the ZrP@PDA/Au reached as high as 38.10 min−1, much higher than some reported noble metal-based catalysts. In addition, the ZrP@PDA/Au showed high stability and reusability, of which the catalytic efficiency was not significantly degraded after prolonged storage in solution.

Mussel-inspired nanocomposite hydrogel based on alginate and antimicrobial peptide for infected wound repair

Timely hemostasis, antibacterial activity, and good adhesion are essential for wound healing. Here, we report about a novel nanocomposite hydrogel with hemostatic, antibacterial, and adhesive properties constructed with a mussel-inspired strategy. Oxidized alginic acid, dopamine, and antimicrobial peptide ε-polylysine were used to prepare a nanocomposite (ODP), and then further cross-linked with acrylamide to fabricate a nanocomposite hydrogel (ODPA). ODPA hydrogel can adhere to the surface of bleeding organs and arrest bleeding within 30 s. It can also be stretched to 12 times its original length and withstand a compression strain of 40 %, and shows effective inhibition on gram-positive and gram-negative bacteria. Compared with commercial alginate sponge, ODPA hydrogel can accelerate the healing of infected full-thickness wound by reducing inflammation, promoting angiogenesis, and collagen deposition. Therefore, the nanocomposite hydrogel is expected to be a multifunctional dressing for promoting healing of infected wounds.

Mussel-Inspired Surface Coating to Stabilize and Functionalize Supramolecular J-Aggregate Nanotubes Composed of Amphiphilic Cyanine Dyes.

We report a mussel-inspired strategy of polydopamine (PDA) coating to stabilize and functionalize J-aggregate nanotubes (NTs) formed by supramolecular self-assembly of an amphiphilic cyanine dye called C8S3 in aqueous media. Optimization of the coating condition by changing the incubation time in a slightly basic media of dopamine with different concentrations leads to conformal wrapping of the PDA layer with controllable thickness on the surface of the NTs. Compared to noncoated pristine C8S3 NTs, these PDA-coated NTs show enhanced stability against dilution, heating, and photobleaching. Moreover, the PDA layer wrapping around the NTs serves as an adhesive for the adsorption of a variety of metal ions and electroless deposition of the metal nanoparticles. Such stabilized and functionalized NT composites may offer a robust synthetic J-aggregate system to mimic the structure and function of light-harvesting complexes and reaction centers in photosynthetic systems.

Mussel-inspired strategy to construct 3D silver nanoparticle network in flexible phase change composites with excellent thermal energy management and electromagnetic interference shielding capabilities

Nowadays, efficient thermal management and electromagnetic interference shielding as effective measures for maintaining the normal operation of electronic devices are extremely significant. However, composites with both thermal management and electromagnetic interference shielding performance are rarely reported. In this study, a kind of flexible polydopamine (PDA) and silver nanoparticles (AgNPs) wrapped melamine foam (MF) constructed by adopting the mussel-inspired strategy was used to fabricate MPAχ-PEG phase change materials (PCMs) via encapsulating polyethylene glycol (PEG). PDA was selected to enhance the interface bonding between MF and AgNPs due to its strong adhesion based on mussel-inspired surface chemistry. Continuous AgNPs wrapped on skeleton of MF construct the three-dimensional (3D) thermal/electrical-conductive porous network. MPAχ-PEG PCMs exhibit a relatively high phase change enthalpy of 148.9 J/g and a high thermal conductivity enhancement of 1400% in comparison with that of MF-PEG. Moreover, MPAχ-PEG PCMs are provided with electromagnetic interference (EMI) shielding performance with the mean SET of 82.02 dB and electro-to-thermal energy conversion efficiency (86.3% under the voltage of 1.2 V) due to the 3D conductive AgNPs network. Combining the elasticity of MPAχ foams and the phase change feature of PEG, the MPAχ-PEG PCMs show good solar-induced shape memory performance. The flexible PCMs could avoid the sharp temperature increase of smartphone by the solid-liquid phase change process of PEG. Therefore, this study provides a promising strategy to prepare flexible PCMs, which can achieve various forms of energy conversion, as well as thermal management and EMI shielding performance, can definitely broaden their application prospect in electronic devices.

Mussel-inspired extracellular matrix-mimicking hydrogel scaffold with high cell affinity and immunomodulation ability for growth factor-free cartilage regeneration.

BackgroundInjury to articular cartilage cause certain degree of disability due to poor self-repair ability of cartilage tissue. To promote cartilage regeneration, it is essential to develop a scaffold that properly mimics the native cartilage extracellular matrix (ECM) in the aspect of compositions and functions.MethodsA mussel-inspired strategy was developed to construct an ECM-mimicking hydrogel scaffold by incorporating polydopamine-modified hyaluronic acid (PDA/HA) complex into a dual-crosslinked collagen (Col) matrix for growth factor-free cartilage regeneration. The adhesion, proliferation, and chondrogenic differentiation of cells on the scaffold were examined. A well-established full-thickness cartilage defect model of the knee in rabbits was used to evaluated the efficacy and functionality of the engineered Col/PDA/HA hydrogel scaffold.ResultsThe PDA/HA complex incorporated-hydrogel scaffold with catechol moieties exhibited better cell affinity than bare negatively-charged HA incorporated hydrogel scaffold. In addition, the PDA/HA complex endowed the scaffold with immunomodulation ability, which suppressed the expression of inflammatory cytokines and effectively activated the polarization of macrophages toward M2 phenotypes. The in vivo results revealed that the mussel-inspired Col/PDA/HA hydrogel scaffold showed strong cartilage inducing ability to promote cartilage regeneration.ConclusionsThe PDA/HA complex-incorporated hydrogel scaffold overcame the cell repellency of negatively-charged polysaccharide-based scaffolds, which facilitated the adhesion and clustering of cells on the scaffold, and therefore enhanced cell-HA interactions for efficient chondrogenic differentiation. Moreover, the hydrogel scaffold modulated immune microenvironment, and created a regenerative microenvironment to enhance cartilage regeneration.The translational potential of this articleThis study gives insight into the mussel-inspired approach to construct the tissue-inducing hydrogel scaffold in a growth-factor-free manner, which show great advantage in the clinical treatment. The hydrogel scaffold composed of collagen and hyaluronic acid as the major component, providing cartilage ECM-mimicking environment, is promising for cartilage defect repair.

A mussel-inspired strategy for CNT/carbon fiber reinforced epoxy composite by hierarchical surface modification

The mechanical properties of carbon fiber-reinforced polymer (CFRP) composites are strongly affected by the fiber-matrix interface performance. Here, we report a mussel-inspired nondestructive method to introduce carbon nanotube (CNT) onto carbon fiber (CF) surface using polydopamine (PDA) via π-π interaction and covalent bonding. The analysis of the surface morphologies, chemical properties, and the wettability of CF reveal that the functionalized CF exhibit an increased roughness and better wettability with epoxy matrix. Mechanically, the modification improves the tensile strength of CF by 14.73%, while the interfacial shear strength and interlaminar shear strength of modified CF/epoxy composite are enhanced by 89.72% and 55.44%, respectively. The enhancement mechanism could be attributed to the interpenetrating ultra-adhesive PDA molecules and CNTs network, which provide the synergistic effects of π-π interaction, hydrogen bonding, covalent bonding, and mechanical interlocking at the interface. As a result, the applied load can be effectively transferred from resin to CFs. This study provides a convenient and environment-friendly surface treatment approach to improve the interfacial and mechanical properties of CFRP composites.

Surface bioengineering of diverse orthopaedic implants with optional functions via bioinspired molecular adhesion and bioorthogonal conjugations

In this work, we reported an upgraded mussel-inspired strategy for surface bioengineering of osteoimplants by combination of mussel adhesion and bioorthogonal click chemistry. The main idea of this strategy is a mussel-inspired synthetic peptide containing multiple 3,4-dihydroxy-L-phenylalanine (DOPA) units and a dibenzocyclooctyne (DBCO) terminal (DOPA-DBCO). According to the mussel adhesion mechanism, the DOPA-DBCO peptide could stably adhere onto a variety of material surface, leaving the residual DBCO groups on the surface. Then, the DBCO residues could be employed for a second-step bioorthogonal conjugation with azide-capping biomolecules through bioorthogonal click chemistry, finally leading to the biomodified surfaces. To demonstrate the generality of our strategy for surface biomodification of diversified orthopaedic materials including metallic and polymeric substrates, we here conceptually conjugated some typical azide-capping biomolecules on both metal and polymeric surfaces. The results definitely verified the feasibility for engineering of functional surfaces with some essential requirements of osteoimplants, for example, the ability to facilitate cell adhesion, suppress bacterial infection, and promote osteogenesis. In a word, this study indicated that our novel surface strategy would show broad applicability for diverse osteoimplants and in different biological scenarios. We can also image that the molecular specificity of bioorthogonal conjugation and the universality of mussel adhesion mechanism may jointly provide a versatile surface bioengineering method for a wider range of biomedical implants.

Sprayable hydrogel dressing accelerates wound healing with combined reactive oxygen species-scavenging and antibacterial abilities

Wound management poses a considerable economic burden on the global healthcare system, considering the impacts of wound infection, delayed healing and scar formation. To this end, multifunctional dressings based on hydrogels have been developed to stimulate skin healing. Herein, we describe the design, fabrication, and characterization of a sprayable hydrogel-based wound dressing loaded with cerium oxide nanoparticles (CeONs) and an antimicrobial peptide (AMP), for combined reactive oxygen species (ROS)-scavenging and antibacterial properties. We adopted a mussel-inspired strategy to chemically conjugate gelatin with dopamine motifs and prepared a hydrogel dressing with improved binding affinity to wet skin surfaces. Additionally, the release of AMP from the hydrogel demonstrated rapid release ablation and contact ablation against four representative bacterial strains, confirming the desired antimicrobial activities. Moreover, the CeONs-loaded hydrogel dressing exhibited favorable ROS-scavenging abilities. The biocompatibility of the multifunctional hydrogel dressing was further proven in vitro by culturing with HaCaT cells. Overall, the benefits of the developed hydrogel wound dressing, including sprayability, adhesiveness, antimicrobial activity, as well as ROS-scavenging and skin-remodeling ability, highlight its promissing translational potentials in wound management. Statement of SignificanceVarious hydrogel-based wound-dressing materials have been developed to stimulate wound healing. However, from the clinical perspective, few of the current wound dressings meet all the intended multifunctional requirements of preventing infection, promoting rapid wound closure, and minimizing scar formation, while simultaneously offering the convenience of application. In the current study, we adopted a mussel-inspired strategy to functionalize the GelMA hydrogels with DOPA to fabricate GelMA-DOPA hydrogel which exhibited an enhanced binding affinity for wound surfaces, AMP HHC-36 and CeONs are further encapsulated into the GelMA-DOPA hydrogel to confer the hydrogel wound dressing with antimicrobial and ROS-scavenging abilities. The GelMA-DOPA-AMP-CeONs dressing offered the benefits of sprayability, adhesiveness, antimicrobial activity, as well as ROS-scavenging and skin-remodeling ability, which might address the therapeutic and economic burdens associated with chronic wound treatment and management.

PLGA Membranes Functionalized with Gelatin through Biomimetic Mussel-Inspired Strategy.

Electrospun membranes have been widely used as scaffolds for soft tissue engineering due to their extracellular matrix-like structure. A mussel-inspired coating approach based on 3,4-dihydroxy-DL-phenylalanine (DOPA) polymerization was proposed to graft gelatin (G) onto poly(lactic-co-glycolic) acid (PLGA) electrospun membranes. PolyDOPA coating allowed grafting of gelatin to PLGA fibers without affecting their bulk characteristics, such as molecular weight and thermal properties. PLGA electrospun membranes were dipped in a DOPA solution (2 mg/mL, Tris/HCl 10 mM, pH 8.5) for 7 h and then incubated in G solution (2 mg/mL, Tris/HCl 10 mM, pH 8.5) for 16 h. PLGA fibers had an average diameter of 1.37 ± 0.23 µm. Quartz crystal microbalance with dissipation technique (QCM-D) analysis was performed to monitor DOPA polymerization over time: after 7 h the amount of deposited polyDOPA was 71 ng/cm2. After polyDOPA surface functionalization, which was, also revealed by Raman spectroscopy, PLGA membranes maintained their fibrous morphology, however the fiber size and junction number increased. Successful functionalization with G was demonstrated by FTIR-ATR spectra, which showed the presence of G adsorption bands at 1653 cm−1 (Amide I) and 1544 cm−1 (Amide II) after G grafting, and by the Kaiser Test, which revealed a higher amount of amino groups for G functionalized membranes. Finally, the biocompatibility of the developed substrates and their ability to induce cell growth was assessed using Neonatal Normal Human Dermal Fibroblasts.

Mussel-inspired synthesis of magnetic N-Halamine nanoparticles for antibacterial recycling

Antibacterial N-halamine coatings are successful in avoiding and eliminating bacterial infections caused by bacterial contamination and biofilms on the surfaces. However, the N-halamine coatings remain a long-standing challenge faced by our healthcare system. Herein we reported a new mussel-inspired surface modification strategy to achieve N-halamine copolymer coatings with adhesive effects. The phenolic hydroxyl groups from N-halamine copolymers are used for ligand exchange with oleic acid on the magnetic Fe3O4 nanoparticles for binding the N-halamine copolymer onto the surface of the nanoparticles. The as-synthesized N-halamine coatings endow the magnetic Fe3O4 nanoparticles antibacterial activity toward both Gram-negative bacteria (Escherichia coli) and Gram-positive bacteria (Staphylococcus aureus). Since the super-paramagnetism of Fe3O4 in core, the N-halamine coatings are separable magnetically and remain high inactivating efficiency toward bacteria even after five cycles. We believe that, with the advantage of mussel-inspired strategy, the N-halamine coatings should have great potential for use in antibacterial and biomedical fields.

Functionalized polyurethane sponge based on dopamine derivative for facile and instantaneous clean-up of cationic dyes in a large scale

Functionalized sponge adsorbent was prepared by a mussel-inspired strategy, which achieved successive modification of material and remained the properties of substrate. The dopamine derivative, DOPAm, was synthesized and adhered to polyurethane (PU) sponge before in situ polymerization with sodium p-styrenesulfonate. The adsorbent showed superior removal efficiency for cationic dyes (98.9 % for methylene blue (MB) at the concentration of 200 μmol/L); it took 1 s only for the adsorbent to adsorb the dyes by swelling and squeezing out the bulk solution simply. Meanwhile, the superior adsorption effect of the adsorbent could be maintained in a wide range of solution pH values from 1 to 13 at room temperature (293 K) in several repeat experiments, due to the slight influence of strong acid and alkali on polysulfonate. With unchanged other experimental conditions, the removal efficiency is still more than 90 % after reusing for 10 times at the different concentrations of MB dye solutions (50, 100, 200 μmol/L). For large-scale wastewater treatment, with the removal efficiency of 80.0 %, the adsorbent could purify 4.1 L wastewater containing MB dye (100 μmol/L) with the maximum flux of 22.2 L/(m3·s) without the assistance of any equipment except for a vacuum pump. Therefore, the adsorbent has great possibilities to be applied in high-efficient and convenient treatment of wastewater in a large scale.