Layer-by-layer Films Research Articles

Layer-by-layer films containing emodin or emodin encapsulated in liposomes for transdermal applications

Dermal drug release systems are an important area of research because they can be applied to the skin in a non-invasive procedure using a lower concentration of drugs. In this study, we have developed two types of Layer-by-Layer (LbL) films for releasing emodin (EM). In one system, EM was intercalated with poly(ethylenimine) PEI and poly(vinyl sufonate) (PVS) polyelectrolytes, forming (PEI/PVS)2(PEI/EM)7; in another, EM was incorporated in liposomes obtained by mixing dipalmitoyl phosphatidyl glycerol (DPPG) and palmitoyl oleoyl phosphatidyl glycerol (POPG) lipids, forming (PEI/PVS)2(PEI/DPPG-POPG-EM)7. UV–vis and FTIR spectroscopies were used to characterize the LbL films. These showed that the depositions of material by LbL were efficient, with increases in the absorbance of each bilayer evidencing the presence of EM in the film. The (PEI/PVS)2(PEI/EM)7 and (PEI/PVS)2(PEI/DPPG-POPG-EM)7 films released EM in three and five days, respectively. The cyclic voltammetry (CV) assay of the (PEI/PVS)2(PEI/EM)7 results are in agreement with UV–vis measurements, which suggest that EM was protonated in acid environments, while the CV of (PEI/PVS)2(PEI/DPPG-POPG-EM)7 demonstrated distinct protonation behaviour for EM within the inner liposome structure, even in acid solutions. Therefore, this study presents two systems based on LbL films and provides additional details about the release of EM from these films to create a viable alternative for transdermal applications.

Synthetic Lift-off Polymer beneath Layer-by-Layer Films for Surface-Mediated Drug Delivery.

A broad range of biomaterials coatings and thin film drug delivery systems require a strategy for the immobilization, retention, and release of coatings from surfaces such as patches, inserts, and microneedles under physiological conditions. Here we report a polymer designed to provide a dynamic surface, one that first functions as a platform for electrostatic thin film assembly and releases the film once in an in vivo environment. Atom transfer radical polymerization (ATRP) was used to synthesize this polymer poly(o-nitrobenzyl-methacrylate-co-hydroxyethyl-methacrylate-co-poly(ethylene-glycol)-methacrylate) (PNHP), embedded beneath multilayered polyelectrolyte films. Such a base layer is designed to photochemically pattern negative charge onto a solid substrate, assist deposition of smooth layer-by-layer (LbL) polyelectrolyte in mildly acidic buffers and rapidly dissolve at physiological pH, thus lifting off the LbL films. To explore potential uses in the biomedical field, a lysozyme (Lys)/poly(acrylic acid) (PAA) multilayer film was developed on PNHP-coated silicon wafers to construct prototype antimicrobial shunts. Film thickness was shown to grow exponentially with increasing deposition cycles, and effective drug loading and in vitro release was confirmed by the dose-dependent inhibition of Escherichia coli (E. coli) growth. The efficacy of this approach is further demonstrated in LbL-coated microscale needle arrays ultimately of interest for vaccine applications. Using PNHP as a photoresist, LbL films were confined to the tips of the microneedles, which circumvented drug waste at the patch base. Subsequent confocal images confirmed rapid LbL film implantation of PNHP at microneedle penetration sites on mouse skin. Furthermore, in human skin biopsies, we achieved efficient immune activation demonstrated by a rapid uptake of vaccine adjuvant from microneedle-delivered PNHP LbL film in up to 37% of antigen-presenting cells (APC), providing an unprecedented LbL microneedle platform for human vaccination.

Controllable nanoporous fibril-like morphology by layer-by- layer self-assembled films of bioelectronics poly(pyrrole-co-formyl pyrrole)/polystyrene sulfonate for biocompatible electrode

We demonstrate a new class of nanocoating materials for biocompatible electrode based on poly (pyrrole-co-formyl pyrrole) (P(Py-co-Fpy)) multilayered with polystyrene sulfonate (PSS) using layer by layer (LBL) self-assembly technique. By modulating the number layer of deposition, the unique surface properties of P(Py-co-Fpy) are evaluated for bioaffinity. Atomic force microscopy (AFM) demonstrates the controllable morphology of the degree fibril network structure of P(Py-co-Fpy)/PSS surface. The direct adsorption of bovine serum albumin (BSA) onto the top surface of P(Py-co-Fpy)/PSS film by AFM analysis reveals the forming of BSA multilayer at high degree of fibril structure P(Py-co-Fpy). In addition, the adsorbed fibrinogen (Fgn) reveals the reversible conformation change on surface of P(Py-co-Fpy)/PSS. The effect of P(Py-co-Fpy)/PSS morphology on primary mouse embryonic fibroblasts (MEF) is investigated. Cell morphology and proliferation on P(Py-co-Fpy)/PSS LBL film at different number of layer deposition are evaluated, demonstrating that P(Py-co-Fpy)/PSS LBL nanocoating surface is non-cytotoxic as morphology-dependent.

Photosensitive Layer-by-Layer Assemblies Containing Azobenzene Groups: Synthesis and Biomedical Applications.

This review provides an overview of the syntheses of photosensitive layer-by-layer (LbL) films and microcapsules modified with azobenzene derivatives and their biomedical applications. Photosensitive LbL films and microcapsules can be prepared by alternate deposition of azobenzene-bearing polymers and counter polymers on the surface of flat substrates and microparticles, respectively. Azobenzene residues in the films and microcapsules exhibit trans-to-cis photoisomerization under UV light, which causes changes in the physical or chemical properties of the LbL assemblies. Therefore, azobenzene-functionalized LbL films and microcapsules have been used for the construction of photosensitive biomedical devices. For instance, cell adhesion on the surface of a solid can be controlled by UV light irradiation by coating the surface with azobenzene-containing LbL films. In another example, the ion permeability of porous materials coated with LbL films can be regulated by UV light irradiation. Furthermore, azobenzene-containing LbL films and microcapsules have been used as carriers for drug delivery systems sensitive to light. UV light irradiation triggers permeability changes in the LbL films and/or decomposition of the microcapsules, which results in the release of encapsulated drugs and proteins.

Porous titanium scaffolds with self-assembled micro/nano-hierarchical structure for dual functions of bone regeneration and anti-infection.

Porous titanium (Ti) scaffolds are widely used for bone repair because of their good biocompatibility, mechanical properties, and corrosion resistance. However, pristine Ti scaffolds are bioinert and unable to induce bone regeneration. In this study, chitosan coated bovine serum albumin nanoparticles (CBSA NPs) and oxidized alginate (OSA) were in a layer-by-layer (LbL) manner on Ti scaffolds. The LbL film possessed micro/nano-hierarchical architectures, has the features of nanostructures, and possesses abundant functional groups from CBSA NPs and OSA to improve the surface biocompatibility and biofunctionality of Ti scaffolds. These groups provide active sites for stable and efficient immobilization of bone morphogenic protein-2 (BMP2) through chemical and physical interactions without compromising its bioactivity. The synergistic effect of the hierarchical structure of assembled films and immobilized BMP2 on the scaffold improves cell adhesion, proliferation, and induces osteogenic differentiation of bone marrow stromal cells in vitro. Moreover, this modification also enhances ectopic bone formation bone. Furthermore, grafting of vancomycin on OSA resulted in good antibacterial activity of Ti scaffolds for prevention of infection during the bone healing process. In summary, this NPs-assembling method is convenient and effective to produce nanostructures and to load growth factors and antibacterial agents into Ti scaffolds for bone tissue engineering. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 105A: 3482-3492, 2017.

UV and NIR-Responsive Layer-by-Layer Films Containing 6-Bromo-7-hydroxycoumarin Photolabile Groups.

This paper describes polyelectrolyte multilayer films prepared by the layer-by-layer (LbL) technique capable of undergoing dissolution upon exposure to either ultraviolet or near-infrared light. Film dissolution is driven by photochemical deprotection of a random methacrylic copolymer with two types of side chains: (i) 6-bromo-7-hydroxycoumarinyl esters, photocleavable groups that are known to have substantial two-photon photolysis cross sections, and (ii) cationic residues from the commercially available monomer N,N-dimethylaminoethyl methacrylate (DMAEMA). In addition, the dependence of stability of both unirradiated and irradiated films on pH provides experimental evidence for the necessity of disrupting both ion-pairing and hydrophobic interactions between polyelectrolytes to realize film dissolution. This work therefore provides both new fundamental insight regarding photolabile LbL films and expands their applied capabilities to nonlinear photochemical processes.

Development of Functional Thin Polymer Films Using a Layer-by-Layer Deposition Technique.

Functional thin films containing insulin were prepared using layer-by-layer (LbL) deposition of insulin and negatively- or positively-charged polymers on the surface of solid substrates. LbL films composed of insulin and negatively-charged polymers such as poly(acrylic acid) (PAA), poly(vinylsulfate) (PVS), and dextran sulfate (DS) were prepared through electrostatic affinity between the materials. The insulin/PAA, insulin/PVS, and insulin/DS films were stable in acidic solutions, whereas they decomposed under physiological conditions as a result of a change in the net electric charge of insulin from positive to negative. Interestingly, the insulin-containing LbL films were stable even in the presence of a digestive-enzyme (pepcin) at pH 1.4 (stomach pH). In contrast, LbL films consisting of insulin and positively-charged polymers such as poly(allylamine hydrochloride) (PAH) decomposed in acidic solutions due to the positive charges of insulin generated in acidic media. The insulin-containing LbL films can be prepared not only on the surface of flat substrates, such as quartz slides, but also on the surface of microparticles, such as poly(lactic acid) (PLA) microbeads. Thus, insulin-containing LbL film-coated PLA microbeads can be handled as a powder. In addition, insulin-containing microcapsules were prepared by coating LbL films on the surface of insulin-doped calcium carbonate (CaCO3) microparticles, followed by dissolution of the CaCO3 core. The release of insulin from the microcapsules was accelerated at pH 7.4, whereas it was suppressed in acidic solutions. These results suggest the potential use of insulin-containing microcapsules in the development of oral formulations of insulin.

Improved glucose label-free biosensor with layer-by-layer architecture and conducting polymer poly(3,4-ethylenedioxythiophene)

Abstract Layer-by-layer (LbL) self-assembly has been used for the development of a new glucose label-free biosensor. Glucose oxidase (GOx) was incorporated in a multilayer film on a gold electrode, previously modified with a film of the conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT), by electropolymerization, for better conductivity. Multilayer films, containing the enzyme and nitrogen doped graphene (NG) dispersed in the biocompatible positively-charged polymer chitosan {chit + (NG + GOx)}, together with the negatively charged polymer poly(styrene sulfonate), PSS − , were assembled. Cyclic voltammetry and electrochemical impedance spectroscopy were used for characterization of the biosensor architectures. The LbL film growth was monitored by Surface Plasmon Resonance Spectroscopy in order to evaluate the interactions involved in the biomolecule immobilization. Atomic force microscopy and scanning electron microscopy imaging show the morphological structure of the multilayer film modified electrode. The analytical properties of the glucose biosensor were determined by fixed potential amperometry and showed a substantial improvement in biosensor sensitivity in the presence of PEDOT. The biosensor operates at a low potential of −0.2 V vs. Ag/AgCl, with a sensitivity of 237 μA cm −2 mM −1 and a detection limit of 41 μM. The biosensor applicability was evaluated by measuring glucose content in wines obtained from Romanian grapes ( Vitis vinifera ).

Layer-by-layer films of block copolymer micelles with cores exhibiting upper critical solution temperature behaviour

We report on preparation of block copolymer micelles with cores exhibiting upper critical solution temperature (UCST) behavior in the range of 40–45°C at pH 7.5 and incorporation of such micelles into layer-by-layer (LbL) films to obtain UCST-type multilayer films. Pyridine units of poly(2-vinylpyridine-b-ethylene oxide) (P2VP-b-PEO) were partially quaternized and its self-assembly into micellar aggregates was achieved in the presence of potassium hexacyanoferrate (K3Fe(CN)6) at pH 7.5 at either 25°C or 37.5°C. The cores of the resulting (QP2VP+[Fe(CN)6]3−)-b-PEO micelles exhibited UCST-type behavior at pH 7.5 and the critical temperature varied in the range of 40–45°C depending on the micellization temperature and amount of K3Fe(CN)6. Our results showed that micellization temperature and K3Fe(CN)6 concentration were highly critical on the UCST of the micellar cores. In case of (QP2VP+[Fe(CN)6]3−)-b-PEO micelles prepared at 25°C, increasing K3Fe(CN)6 concentration during micellization suppressed UCST behavior within a temperature range of 25-50°C. In contrast, increasing K3Fe(CN)6 concentration induced only small shifts in UCST when (QP2VP+[Fe(CN)6]3−)-b-PEO micelles were produced at 37.5°C. Moreover, we showed that (QP2VP+[Fe(CN)6]3−)-b-PEO micelles could be incorporated into LbL films using Tannic Acid (TA) at pH 7.5. Multilayers which partially disintegrate near above 40°C could be assembled by controlling micellization temperature and film deposition temperature. This study contributes to fundamental understanding of salt-induced micellization and structure–property relationship in hydrogen-bonded LbL films.

Ultrastrong and flame-resistant freestanding films from nanocelluloses, self-assembled using a layer-by-layer approach

Nanosized cellulose nanofibrils (CNF) prepared from phosphorylated pulp fibers (P-CNF) are combined with CNF prepared from aminated fibers (cationic CNF) through a layer-by-layer (LbL) assembly to prepare a freestanding, transparent all-cellulose film. It is shown that the thermal stability and flame-retardant properties of the all CNF film are significantly improved when phosphorylated CNF is combined with cationic fibrils in an LbL assembled structure. The freestanding films also show a tensile strength of 160MPa and a Young's modulus of 9GPa, placing it among strongest freestanding LbL films fabricated so far, showing large promise for the use of these types of ultrathin films in advanced applications. The LbL build-up of the cationic CNF/P-CNF multilayer film is carefully studied by quartz crystal microbalance with dissipation (QCM-D) and atomic force microscopy (AFM). Hydrophobized silicon substrates are used for the LbL deposition and it is shown that the (cationic CNF/P-CNF)300 film, 2.3μm thick, can be easily detached from the substrate using tweezers. The thermal stability, combustion behavior and mechanical properties of the films are further studied by thermogravimetric analysis, combustion and tensile tests respectively.

Polyethylene imine/graphene oxide layer-by-layer surface functionalization for significantly improved limit of detection and binding kinetics of immunoassays on acrylate surfaces

Antibody immobilization on polymeric substrates is a key manufacturing step for microfluidic devices that implement sample-to-answer automation of immunoassays. In this work, a simple and versatile method to bio-functionalize poly(methylmethacrylate) (PMMA), a common material of such “Lab-on-a-Chip” systems, is proposed; using the Layer-by-Layer (LbL) technique, we assemble nanostructured thin films of poly(ethylene imine) (PEI) and graphene oxide (GO). The wettability of PMMA surfaces was significantly augmented by the surface treatment with (PEI/GO)5 film, with an 81% reduction of the contact angle, while the surface roughness increased by 600%, thus clearly enhancing wettability and antibody binding capacity. When applied to enzyme-linked immunosorbent assays (ELISAs), the limit of detection of PMMA surface was notably improved from 340pgmL−1 on commercial grade polystyrene (PS) and 230pgmL−1 on plain PMMA surfaces to 130pgmL−1 on (PEI/GO)5 treated PMMA. Furthermore, the accelerated antibody adsorption kinetics on the LbL films of GO allowed to substantially shorten incubation times, e.g. for anti-rat IgG adsorption from 2h down to 15min on conventional and treated surfaces, respectively.

Incorporation of triclosan and acridine orange into liposomes for evaluating the susceptibility of Candida albicans

Candida albicans is responsible for many of the infections affecting immunocompromised individuals. Although most C. albicans are susceptible to antifungal drugs, uncontrolled use of these drugs has promoted the development of resistance to current antifungals. The clinical implication of resistant strains has led to the search for safer and more effective drugs as well as alternative approaches, such as controlled drug release using liposomes and photodynamic inactivation (PDI), to eliminate pathogens by combining light and photosensitizers. In this study, we used layer-by-layer (LBL) assembly to immobilize triclosan and acridine orange encapsulated in liposomes and investigated the possibility of controlled release using light. Experiments were carried out to examine the susceptibility of C. albicans to PDI. The effects of laser irradiation were investigated by fluorescence microscopy, atomic force microscopy, and release kinetics. Liposomes were successfully prepared and immobilized using the self-assembly LBL technique. Triclosan was released more quickly when the LBL film was irradiated. The release rate was approximately 40% higher in irradiated films (fluence of 15J/cm2) than in non-irradiated films. The results of the susceptibility experiments and surface morphological analysis indicated that C. albicans cell death is caused by photodynamic inactivation. Liposomes containing triclosan and acridine orange may be useful for inactivating C. albicans using light. Our results lay the foundation for the development of new clinical strategies to control resistant strains.

Different coating on electrospun nanofiber via layer-by-layer self-assembly for their photocatalytic activities

The water-stable PAA/PVA/PW12 nanofiber was firstly prepared by electrospinning and thermal treatments. The negatively charged phosphotungstic acid (PW12), positively charged polyethylenimine (PEI) and silver nanoparticle (Ag NPs) were alternatively deposited onto the fibrous substrate by layer-by-layer (LBL) self-assembly technique. The photocatalytic activity of different coated LBL film was observed under visible light irradiation. The results indicated that the conversion rate of methylene blue (MB) was gradually decreased with increasing the number of bilayers pairs. The behavior might ascribe to the more polycation electrolyte PEI that prevented from permeating for the MB molecule. On the other hand, in terms of the effects of surface charges on the photocatalytic activity, negatively charged surface (PEI)n(PW12)n indicated higher photocatalytic activity than that of positively charged surface (PEI)n(PW12)n−1. For the Ag NPs deposited on the LBL film, Ag-(PEI)n(PW12)n film were found to be a better photocatalytic activity than other multilayer films, specially, Ag-(PEI)2(PW12)2 exhibited the most excellent activity due to the influence of the synergy in the hybrid materials.

Polymer Chromophore-Catalyst Assembly for Solar Fuel Generation.

A polystyrene-based chromophore-catalyst assembly (poly-2) has been synthesized and assembled at a mesoporous metal oxide photoanode. The assembly contains water oxidation catalyst centers based on [Ru(trpy) (phenq)]2+ (Ru-Cat) and [Ru(bpy)3]2+ derivatives (Ru-C) as chromophores (trpy= 2,2';6,2″- terpyridine, phenq = 2-(quinol-8'-yl)-1,10-phenanthroline and bpy = 2,2'-bipyridine). The photophysical and electrochemical properties of the polychromophore-oxidation catalyst assembly were investigated in solution and at the surface of mesoporous metal oxide films. The layer-by-layer (LbL) method was utilized to construct multilayer films with cationic poly-2 and anionic poly(acrylic acid) (PAA) for light-driven photochemical oxidations. Photocurrent measurements of (PAA/poly-2)10 LbL films on mesoporous TiO2 demonstrate light-driven oxidation of phenol and benzyl alcohol in aqueous solution. Interestingly, illumination of (PAA/poly-2)5 LbL films on a fluorine doped SnO2/TiO2 core/shell photoanode in aqueous solution gives rise to an initial photocurrent (∼18.5 μA·cm-2) that is in part ascribed to light driven water oxidation.

Phenylboronic Acid-Functionalized Layer-by-Layer Assemblies for Biomedical Applications.

Recent progress in the development of phenylboronic acid (PBA)-functionalized layer-by-layer (LbL) assemblies and their biomedical applications was reviewed. Stimuli-sensitive LbL films and microcapsules that exhibit permeability changes or decompose in response to sugars and hydrogen peroxide (H2O2) have been developed using PBA-bearing polymers. The responses of PBA-modified LbL assemblies arise from the competitive binding of sugars to PBA in the films or oxidative decomposition of PBA by H2O2. Electrochemical glucose sensors have been fabricated by coating the surfaces of electrodes by PBA-modified LbL films, while colorimetric and fluorescence sensors can be prepared by modifying LbL films with boronic acid-modified dyes. In addition, PBA-modified LbL films and microcapsules have successfully been used in the construction of drug delivery systems (DDS). Among them, much effort has been devoted to the glucose-triggered insulin delivery systems, which are constructed by encapsulating insulin in PBA-modified LbL films and microcapsules. Insulin is released from the PBA-modified LbL assemblies upon the addition of glucose resulting from changes in the permeability of the films or decomposition of the film entity. Research into insulin DDS is currently focused on the development of high-performance devices that release insulin in response to diabetic levels of glucose (>10 mM) but remain stable at normal levels (~5 mM) under physiological conditions.

Information Visualization and Feature Selection Methods Applied to Detect Gliadin in Gluten-Containing Foodstuff with a Microfluidic Electronic Tongue.

The fast growth of celiac disease diagnosis has sparked the production of gluten-free food and the search for reliable methods to detect gluten in foodstuff. In this paper, we report on a microfluidic electronic tongue (e-tongue) capable of detecting trace amounts of gliadin, a protein of gluten, down to 0.005 mg kg-1 in ethanol solutions, and distinguishing between gluten-free and gluten-containing foodstuff. In some cases, it is even possible to determine whether gluten-free foodstuff has been contaminated with gliadin. That was made possible with an e-tongue comprising four sensing units, three of which made of layer-by-layer (LbL) films of semiconducting polymers deposited onto gold interdigitated electrodes placed inside microchannels. Impedance spectroscopy was employed as the principle of detection, and the electrical capacitance data collected with the e-tongue were treated with information visualization techniques with feature selection for optimizing performance. The sensing units are disposable to avoid cross-contamination as gliadin adsorbs irreversibly onto the LbL films according to polarization-modulated infrared reflection absorption spectroscopy (PM-IRRAS) analysis. Small amounts of material are required to produce the nanostructured films, however, and the e-tongue methodology is promising for low-cost, reliable detection of gliadin and other gluten constituents in foodstuff.

Nanoarchitecturing of Natural Melanin Nanospheres by Layer-by-Layer Assembly: Macroscale Anti-inflammatory Conductive Coatings with Optoelectronic Tunability.

Natural melanins are biocompatible conductors with versatile functionalities. Here, we report fabrication of multifunctional poly(vinyl alcohol)/melanin nanocomposites by layer-by-layer (LBL) assembly using melanin nanoparticles (MNPs) directly extracted from sepia officinalis inks. The LBL assembly offers facile manipulation of nanotextures as well as nm-thickness control of the macroscale film by varying solvent qualities. The time-resolved absorption was monitored during the process and quantitatively studied by fractal dimension and lacunarity analysis. The capability of nanoarchitecturing provides confirmation of complete monolayer formation and leads to tunable iridescent reflective colors of the MNP films. In addition, the MNP films have durable electrochemical conductivities as evidenced by enhanced charge storage capacities for 1000 cycles. Moreover, the MNP covered ITO (indium tin oxide) substrates significantly reduced secretion of inflammatory cytokines, TNF-α, by raw 264.7 macrophage cells compared to bare ITO, by a factor of 5 and 1.8 with and without lipopolysaccharide endotoxins, respectively. These results highlight the optoelectronic device-level tunability along with the anti-inflammatory biocompatibility of the MNP LBL film. This combination of performance should make these films particularly interesting for bioelectronic device applications such as electroceuticals, artificial bionic organs, biosensors, and implantable devices.

Alizarin Red S-Confined Layer-By-Layer Films as Redox-Active Coatings on Electrodes for the Voltammetric Determination of L-Dopa.

The preparation of redox-active coatings is a key step in fabricating electrochemical biosensors. To this goal, a variety of coating materials have been used in combination with redox-active compounds. In this study, alizarin red S (ARS) was confined in layer-by-layer (LbL) films composed of poly(ethyleneimine) (PEI) and carboxymethylcellulose (CMC) to study the redox properties. A gold (Au) disc electrode coated with PEI/CMC LbL film was immersed in an ARS solution to uptake ARS into the film. ARS was successfully confined in the LbL film through electrostatic interactions. The cyclic voltammogram (CV) of ARS-confined PEI/CMC film-coated electrodes thus prepared exhibited redox waves in the potential range from −0.5 to −0.7 V originating from 9,10-anthraquinone moiety in ARS, demonstrating that ARS preserves its redox activity in the LbL film. An additional oxidation peak appeared around −0.4 V in the CV recorded in the solution containing phenylboronic acid (PBA), due to the formation of a boronate ester of ARS (ARS-PBA) in the film. The oxidation peak current at −0.4 V decreased upon addition of 3,4-dihydroxyphenylalanine (L-dopa) to the solution. Thus, the results suggest a potential use of the ARS-confined PEI/CMC films for constructing voltammetric sensors for L-dopa.

Inkjet Printing-Based Patchable Multilayered Biomolecule-Containing Nanofilms for Biomedical Applications.

Thin films including biocompatible polymers and biological materials as building blocks can be produced with a variety of critical film characteristics, including various materials, thicknesses, roughnesses, amounts of compound released, and release rates for biomedical purposes. We developed a multilayer fabrication system via high-throughput layer-by-layer (LbL) assembly of a nanofilm with inkjet printing to facilitate practical biomedical applications. Our system was used to generate biomolecule (ovalbumin and basic fibroblast growth factor)-containing printed LbL films. This is the first demonstration of the clinical benefits of nanofilm-type nanobiomaterials based on molecular organization, suggesting that novel therapeutic human skin patches could be realized without the need for conventional surgical practices.

Phosphoprotein/chitosan electrospun nanofibrous scaffold for biomineralization

In this study, negatively charged phosvitin (PV) and positively charged chitosan (CS) were alternately deposited on negatively charged cellulose mats via layer-by-layer (LBL) self-assembly technique. Morphologies of the LBL films coating mats were observed by scanning electron microscope (SEM). Afterwards, in vitro biomimetic mineralization was carried out through incubation of the fibrous mats in a simulated body fluid (SBF) solution for different time. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) were used to characterize the morphology and structure of the deposited mineral phase on the scaffolds. In addition, the cell culture experiment demonstrated that the scaffolds with the LBL structured films were of good cell compatibility for MC3T3-E1 cells. Moreover, the cell proliferation was affected by the number of deposition layers and the composition of outer-most layer. Confocal laser scanning microscopy (CLSM) and SEM imaging revealed a good performance of cell adhesion and spreading of MC3T3-E1 cells on the surface of biocomposite scaffold. So CS/PV nanofibrous mats were satisfactory for the composite to be used in bioapplications.