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1.
Small ; : e2405635, 2024 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-39344596

RESUMO

The increasing incidence of serious bacterial keratitis, a sight-threatening condition often exacerbated by inadequate contact lens (CLs) care, highlights the need for innovative protective technology. This study introduces a long-lasting antibacterial, non-cytotoxic, transparent nanocoating for CLs via a solvent-free polymer deposition method, aiming to prevent bacterial keratitis. The nanocoating comprises stacked polymer films, with poly(dimethylaminomethyl styrene-co-ethylene glycol dimethacrylate) (pDE) as a biocompatible, antibacterial layer atop poly(2,4,6,8-tetramethyl-2,4,6,8-tetravinylcyclotetrasiloxane) (pV4D4) as an adhesion-promoting layer. The pD6E1-grafted (g)-pV4D4 film shows non-cytotoxicity toward two human cell lines and antibacterial activity of >99% against four bacteria, including methicillin-resistant Staphylococcus aureus (MRSA), an antibiotic-resistant bacteria and Pseudomonas aeruginosa, which causes ocular diseases. Additionally, the film demonstrates long-lasting antibacterial activity greater than 96% against MRSA for 9 weeks in phosphate-buffered saline. To the best knowledge, this duration represents the longest reported long-term stability with less than 5% decay of antibacterial performance among contact-killing antibacterial coatings. The film exhibits exceptional mechanical durability, retaining its antibacterial activity even after 15 washing cycles. The pD6E1-g-pV4D4-coated CL maintains full optical transmittance compared to that of pristine CL. It is expected that the unprecedentedly prolonged antibacterial performance of the coating will significantly alleviate the risk of infection for long-term CL users.

2.
Small ; 20(30): e2312283, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38409517

RESUMO

An ion-based synaptic transistor (synaptor) is designed to emulate a biological synapse using controlled ion movements. However, developing a solid-state electrolyte that can facilitate ion movement while achieving large-scale integration remains challenging. Here, a bio-inspired organic synaptor (BioSyn) with an in situ ion-doped polyelectrolyte (i-IDOPE) is demonstrated. At the molecular scale, a polyelectrolyte containing the tert-amine cation, inspired by the neurotransmitter acetylcholine is synthesized using initiated chemical vapor deposition (iCVD) with in situ doping, a one-step vapor-phase deposition used to fabricate solid-state electrolytes. This method results in an ultrathin, but highly uniform and conformal solid-state electrolyte layer compatible with large-scale integration, a form that is not previously attainable. At a synapse scale, synapse functionality is replicated, including short-term and long-term synaptic plasticity (STSP and LTSP), along with a transformation from STSP to LTSP regulated by pre-synaptic voltage spikes. On a system scale, a reflex in a peripheral nervous system is mimicked by mounting the BioSyns on various substrates such as rigid glass, flexible polyethylene naphthalate, and stretchable poly(styrene-ethylene-butylene-styrene) for a decentralized processing unit. Finally, a classification accuracy of 90.6% is achieved through semi-empirical simulations of MNIST pattern recognition, incorporating the measured LTSP characteristics from the BioSyns.

3.
Nanotechnology ; 35(44)2024 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-39082380

RESUMO

Gallium oxide (Ga2O3) is attracting attention as a next-generation semiconductor material for power device because it has a wide energy band gap and high breakdown electric field. We deposited a Sn polymer, poly-tetraallyl tin, on Ga2O3samples using a disclosed initiated chemical vapor deposition (iCVD) process. The Sn dopant of the Sn polymer layer is injected into the Ga2O3through a heat treatment process. Diffusion model of Sn into the Ga2O3is proposed through secondary ion mass spectroscopy analysis and bond dissociation energy. The fabricated device exhibited typical n-type field-effect transistor (FET) behavior. Ga2O3Sn-doping technology using iCVD will be applied to 3D structures and trench structures in the future, opening up many possibilities in the Ga2O3-based power semiconductor device manufacturing process.

4.
Small ; 18(17): e2106648, 2022 04.
Artigo em Inglês | MEDLINE | ID: mdl-35297560

RESUMO

Although the dendritic cell (DC)-based modulation of immune responses has emerged as a promising therapeutic strategy for tumors, infections, and autoimmune diseases, basic research and therapeutic applications of DCs are hampered by expensive growth factors and sophisticated culture procedures. Furthermore, the platform to drive the differentiation of a certain DC subset without any additional biochemical manipulations has not yet been developed. Here, five types of polymer films with different hydrophobicity via an initiated chemical vapor deposition (iCVD) process to modulate the interactions related to cell-substrate adhesion are introduced. Especially, poly(cyclohexyl methacrylate) (pCHMA) substantially enhances the expansion and differentiation of conventional type 1 DCs (cDC1s), the prime DC subset for antigen cross-presentation, and CD8+ T cell activation, by 4.8-fold compared to the conventional protocol. The cDC1s generated from the pCHMA-coated plates retain the bona fide DC functions including the expression of co-stimulatory molecules, cytokine secretion, antigen uptake and processing, T cell activation, and induction of antitumor immune responses. To the authors' knowledge, this is the first report highlighting that the modulation of surface hydrophobicity of the culture plate can be an incisive approach to construct an advanced DC culture platform with high efficiency, which potentially facilitates basic research and the development of immunotherapy employing DCs.


Assuntos
Células Dendríticas , Polímeros , Apresentação de Antígeno , Técnicas de Cultura de Células/métodos , Células Dendríticas/metabolismo , Ativação Linfocitária , Polímeros/metabolismo
5.
Chem Eng J ; 418: 129368, 2021 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-33746567

RESUMO

The ongoing pandemic caused by the novel coronavirus has turned out to be one of the biggest threats to the world, and the increase of drug-resistant bacterial strains also threatens the human health. Hence, there is an urgent need to develop novel anti-infective materials with broad-spectrum anti-pathogenic activity. In the present study, a fluorinated polycationic coating was synthesized on a hydrophilic and negatively charged polyester textile via one-step initiated chemical vapor deposition of poly(dimethyl amino methyl styrene-co-1H,1H,2H,2H-perfluorodecyl acrylate) (P(DMAMS-co-PFDA), PDP). The surface characterization results of SEM, FTIR, and EDX demonstrated the successful synthesis of PDP coating. Contact angle analysis revealed that PDP coating endowed the polyester textile with the hydrophobicity against the attachment of different aqueous foulants such as blood, coffee, and milk, as well as the oleophobicity against paraffin oil. Zeta potential analysis demonstrated that the PDP coating enabled a transformation of negative charge to positive charge on the surface of polyester textile. The PDP coating exhibited excellent contact-killing activity against both gram-negative Escherichia coli and gram-positive methicillin-resistant Staphylococcus aureus, with the killing efficiency of approximate 99.9%. In addition, the antiviral capacity of PDP was determined by a green fluorescence protein (GFP) expression-based method using lentivirus-EGFP as a virus model. The PDP coating inactivated the negatively charged lentivirus-EGFP effectively. Moreover, the coating showed good biocompatibility toward mouse NIH 3T3 fibroblast cells. All the above properties demonstrated that PDP would be a promising anti-pathogenic polymeric coating with wide applications in medicine, hygiene, hospital, etc., to control the bacterial and viral transmission and infection.

6.
Biotechnol Bioprocess Eng ; 26(2): 165-178, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-33821132

RESUMO

For last two decades, the demand for precisely engineered three-dimensional structures has increased continuously for the developments of biomaterials. With the recent advances in micro- and nano-fabrication techniques, various devices with complex surface geometries have been devised and produced in the pharmaceutical and medical fields for various biomedical applications including drug delivery and biosensors. These advanced biomaterials have been designed to mimic the natural environments of tissues more closely and to enhance the performance for their corresponding biomedical applications. One of the important aspects in the rational design of biomaterials is how to configure the surface of the biomedical devices for better control of the chemical and physical properties of the bioactive surfaces without compromising their bulk characteristics. In this viewpoint, it of critical importance to secure a versatile method to modify the surface of various biomedical devices. Recently, a vapor phase method, termed initiated chemical vapor deposition (iCVD) has emerged as damage-free method highly beneficial for the conformal deposition of various functional polymer films onto many kinds of micro- and nano-structured surfaces without restrictions on the substrate material or geometry, which is not trivial to achieve by conventional solution-based surface functionalization methods. With proper structural design, the functional polymer thin film via iCVD can impart required functionality to the biomaterial surfaces while maintaining the fine structure thereon. We believe the iCVD technique can be not only a valuable approach towards fundamental cell-material studies, but also of great importance as a platform technology to extend to other prospective biomaterial designs and material interface modifications for biomedical applications.

7.
Small ; 14(9)2018 03.
Artigo em Inglês | MEDLINE | ID: mdl-29251418

RESUMO

A high-performance top-gated graphene field-effect transistor (FET) with excellent mechanical flexibility is demonstrated by implementing a surface-energy-engineered copolymer gate dielectric via a solvent-free process called initiated chemical vapor deposition. The ultrathin, flexible copolymer dielectric is synthesized from two monomers composed of 1,3,5-trimethyl-1,3,5-trivinyl cyclotrisiloxane and 1-vinylimidazole (VIDZ). The copolymer dielectric enables the graphene device to exhibit excellent dielectric performance and substantially enhanced mechanical flexibility. The p-doping level of the graphene can be tuned by varying the polar VIDZ fraction in the copolymer dielectric, and the Dirac voltage (VDirac ) of the graphene FET can thus be systematically controlled. In particular, the VDirac approaches neutrality with higher VIDZ concentrations in the copolymer dielectric, which minimizes the carrier scattering and thereby improves the charge transport of the graphene device. As a result, the graphene FET with 20 nm thick copolymer dielectrics exhibits field-effect hole and electron mobility values of over 7200 and 3800 cm2 V-1 s-1 , respectively, at room temperature. These electrical characteristics remain unchanged even at the 1 mm bending radius, corresponding to a tensile strain of 1.28%. The formed gate stack with the copolymer gate dielectric is further investigated for high-frequency flexible device applications.

8.
ACS Appl Mater Interfaces ; 13(8): 10553-10563, 2021 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-33617220

RESUMO

Biofilm formation on indwelling medical devices is a major cause of hospital-acquired infections. Monofunctional antibacterial surfaces have been developed to resist the formation of biofilms by killing bacteria on contact, but the adsorption of killed bacterial cells and debris gradually undermines the function of these surfaces. Here, we report a facile approach to produce an antibacterial surface that can regenerate its function after contamination. The self-regenerating surface was achieved by sequential deposition of alternating antibacterial and biodegradable layers of coating using a solvent-free initiated chemical vapor deposition method. As the top antibacterial layer gradually loses its killing ability due to the accumulation of debris, the underlying biodegradable layer degrades, shedding off the top surface layers and exposing another fresh antibacterial surface. Urinary catheters coated with monofunctional and self-regenerating antibacterial coatings both showed more than 99% bacterial killing ability at the initial antibacterial test, but the monofunctional surface lost its killing ability after continued exposure to concentrated bacterial solution, whereas the self-regenerating surfaces regained strong bacterial killing ability after prolonged exposure. Employing poly(methacrylic anhydride) and its copolymers with varied composition as the degrading layer, the degradation kinetics can be well-tailored and the self-regeneration duration spanned from minutes to days. The designed self-regenerating antibacterial surfaces could provide an effective approach to resist biofilm formation and extend the service life of indwelling medical devices.


Assuntos
Antibacterianos/farmacologia , Biofilmes/efeitos dos fármacos , Materiais Revestidos Biocompatíveis/química , Dimetilaminas/farmacologia , Ácidos Polimetacrílicos/química , Poliestirenos/farmacologia , Antibacterianos/química , Dimetilaminas/química , Escherichia coli/efeitos dos fármacos , Escherichia coli/fisiologia , Testes de Sensibilidade Microbiana , Poliestirenos/química , Staphylococcus aureus/efeitos dos fármacos , Staphylococcus aureus/fisiologia , Cateteres Urinários/microbiologia
9.
Mater Sci Eng C Mater Biol Appl ; 110: 110623, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32204065

RESUMO

The presence of various functional groups in the structure of gelatin nanofibers (GNFs) has made it a suitable candidate for biomedical applications, yet its fast dissolution in aqueous media has been a real challenge for years. In the present work, we propose an efficient procedure to improve the durability of the GNFs. The electrospun GNFs were coated with poly(ethylene glycol dimethacrylate) (pEGDMA) using initiated chemical vapor deposition (iCVD) as a completely dry polymerization method. Morphological and chemical analysis revealed that an ultrathin layer formed around nanofibers (iCVD-GNFs) which has covalently bonded to gelatin chains. Against the instant dissolution of GNFs, the in vitro biodegradability test showed the iCVD-GNFs, to a large extent, preserve their morphology after 14 days of immersion and did not lose its integrity even after 31 days. In vitro cell culture studies, also, revealed cytocompatibility of the iCVD-GNFs for human fibroblast cells (hFC), as well as higher cell proliferation on the iCVD-GNFs compared to control made from tissue culture plate (TCP). Furthermore, contact angle measurements indicated that the hydrophilic GNFs became hydrophobic after the iCVD, yet FE-SEM images of cell-seeded iCVD-GNFs showed satisfactory cell adhesion. Taken together, the proposed method paves a promising way for the production of water-resistant GNFs utilized in biomedical applications; for instance, tissue engineering scaffolds and wound dressings.


Assuntos
Materiais Revestidos Biocompatíveis , Fibroblastos/metabolismo , Gelatina , Teste de Materiais , Membranas Artificiais , Nanofibras/química , Linhagem Celular , Materiais Revestidos Biocompatíveis/química , Materiais Revestidos Biocompatíveis/farmacologia , Fibroblastos/citologia , Gelatina/química , Gelatina/farmacologia , Humanos , Metacrilatos/química , Metacrilatos/farmacologia
10.
ACS Appl Mater Interfaces ; 12(16): 18978-18986, 2020 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-32212671

RESUMO

We report initiated chemical vapor deposition of model-graded polymer coatings enabling antibacterial, antifouling, and biocompatible surfaces. The graded coating was constructed by a bottom layer consisting of bactericidal poly(dimethyl amino methyl styrene) and a surface layer consisting of both dimethyl amino methyl styrene (DMAMS) and hydrophilic vinyl pyrrolidone (VP) moieties. Fourier transform infrared spectra showed existence of both DMAMS and VP in the coating with DMAMS as the major component, while X-ray photoelectron spectroscopy analysis and water contact angle measurement revealed a VP-enriched coating surface. The resultant coating exhibited more than 99.9% killing rate against both Gram-negative Escherichia coli and Gram-positive Bacillus subtilis despite the incorporation of VP on the surface. We believe that such bactericidal capability resulted because of its high surface zeta potential, which could be originated from the DMAMS units distributed both on the top surface and underneath. The graded coating achieved more than 85% bacterial fouling resistance than the pristine substrate, as well as improved biocompatibility, owing to the abundant surface lactam groups from the VP moiety. Furthermore, the graded coating maintained good bactericidal capability after multicycle challenges of bacterial solutions and was durable against continuous rigorous washing, suggesting potential applications in biomedical devices.


Assuntos
Antibacterianos , Materiais Revestidos Biocompatíveis , Gases/química , Polímeros/química , Antibacterianos/química , Antibacterianos/farmacologia , Antibacterianos/toxicidade , Bactérias/efeitos dos fármacos , Linhagem Celular , Sobrevivência Celular/efeitos dos fármacos , Materiais Revestidos Biocompatíveis/química , Materiais Revestidos Biocompatíveis/farmacologia , Materiais Revestidos Biocompatíveis/toxicidade , Reutilização de Equipamento , Humanos , Viabilidade Microbiana/efeitos dos fármacos
11.
ACS Biomater Sci Eng ; 6(4): 2240-2250, 2020 04 13.
Artigo em Inglês | MEDLINE | ID: mdl-33455337

RESUMO

The aggregation of mesenchymal stem cells (MSCs) into three-dimensional (3D) spheroids has emerged as a promising therapeutic candidate for the treatment of a variety of diseases. In spite of the numerous 3D culture methods suggested recently for MSC spheroid generation, it is still elusive to fully reflect real stem cell niches; this effort majorly suffers from a lack of cell-extracellular matrix (ECM) interactions within the 3D spheroids. In this study, we develop a simple but versatile method for generating human MSC (hMSC) spheroids by culturing the cells on a functional polymer film surface, poly(2,4,6,8-tetravinyl-2,4,6,8-tetramethyl cyclotetrasiloxane) (pV4D4). Interestingly, the pV4D4-coated surface allows a dynamic cell adhesion to the polymer surface while developing the formation of 3D spheroids. The corresponding mechanotransduction promotes the expression of the endogenous ECM and, in turn, results in a remarkable improvement in self-renewal abilities, pro-angiogenic potency, and multilineage differentiation capabilities. This observation highlights the significance of our method compared to the conventional spheroid-generating methods in terms of recreating the ECM-rich microenvironment. We believe the developed surface can serve as a versatile but reliable method for stem cell-based tissue engineering and regenerative medicine.


Assuntos
Polímeros , Esferoides Celulares , Células-Tronco , Matriz Extracelular , Humanos , Mecanotransdução Celular
12.
ACS Appl Bio Mater ; 3(11): 7654-7665, 2020 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-35019506

RESUMO

For efficient therapeutic use of human mesenchymal stem cells (hMSCs), maximizing their self-renewal performance and multipotency must be fully retained. However, conventional trypsin-based cell passaging methods are known to damage the attached cells to be detached because of the inherent corrosive nature of trypsin, and continuous passaging substantially degrades the self-renewal and differentiation capacity of hMSCs. Therefore, it is imperative to secure a damage-free passaging method that supports cell growth as well as their stem cell function. Here, an enzyme-free cell detachment method using a poly(ethylene glycol dimethacrylate) (pEGDMA)-coated surface is developed, which allows for reduced integrin-dependent cell adhesion. Cell detachment can be facilitated simply by treating the plated cells on the pEGDMA surface with Ca2+ and Mg2+-depleted DPBS. Spontaneous cell detachment occurs within 10 min with the full retention of the cell viability and proliferation ability of hMSCs. Especially, the detachment method can minimize the surface protein damage of hMSCs compared to the conventional trypsin treatment and preserve the self-renewal property and differentiation capacity even with an increased passage number over 10. The developed enzyme-free detachment method using the pEGDMA-coated surface is highly promising for a culture platform to broaden its application to the field of tissue engineering and regenerative medicine.

13.
Adv Mater ; 32(16): e1907225, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32157771

RESUMO

Cell sheet engineering, a technique utilizing a monolayer cell sheet, has recently emerged as a promising technology for scaffold-free tissue engineering. In contrast to conventional tissue-engineering approaches, the cell sheet technology allows cell harvest as a continuous cell sheet with intact extracellular matrix proteins and cell-cell junction, which facilitates cell transplantation without any other artificial biomaterials. A facile, non-thermoresponsive method is demonstrated for a rapid but highly reliable platform for cell-sheet engineering. The developed method exploits the precise modulation of cell-substrate interactions by controlling the surface energy of the substrate via a series of functional polymer coatings to enable prompt cell sheet harvesting within 100 s. The engineered surface can trigger an intrinsic cellular response upon the depletion of divalent cations, leading to spontaneous cell sheet detachment under physiological conditions (pH 7.4 and 37 °C) in a non-thermoresponsive manner. Additionally, the therapeutic potential of the cell sheet is successfully demonstrated by the transplantation of multilayered cell sheets into mouse models of diabetic wounds and ischemia. These findings highlight the ability of the developed surface for non-thermoresponsive cell sheet engineering to serve as a robust platform for regenerative medicine and provide significant breakthroughs in cell sheet technology.


Assuntos
Polímeros/química , Engenharia Tecidual/métodos , Adsorção , Fibronectinas/química , Propriedades de Superfície , Temperatura , Fatores de Tempo
14.
ACS Biomater Sci Eng ; 6(10): 5632-5644, 2020 10 12.
Artigo em Inglês | MEDLINE | ID: mdl-33320585

RESUMO

3D spheroids are considered as the improved in vitro model to mimic the distinct arrangements of the cells in vivo. To date, low-attachment surfaces have been most widely used to induce the spontaneous aggregation of cells in suspension by simply tuning the relative strength of the cell-cell adhesion over cell-substrate adhesion. However, aggregating cancer cells into 3D clusters should mean more than just adjoining the cells in the physical proximity. The tumor cell functionality is strongly affected by the adhesion networks between cancer cells and extracellular matrix (ECM). Here, we performed an in-depth analysis of how the nonmetastatic breast cancer cells (MCF7) can be transformed to gain invasive phenotypes through compact aggregation into 3D spheroids on a functional polymer film surface, poly(2,4,6,8-tetravinyl-2,4,6,8-tetramethyl cyclotetrasiloxane) (pV4D4). By comparing the adhesion networks and invasion dynamics between 3D spheroids cultured on the pV4D4 surface with those cultured on conventional ultra-low-attachment (ULA) dishes, we report that only spheroids on the pV4D4 display active and sporadic cell-surface binding activities via dynamic protrusions, which correlates strongly with an increase in integrin ß1. Moreover, localized laminin expression at the core of the pV4D4-cultured spheroids confirms the prominence of the intimate integrin-laminin interactions prompted by the exposure to pV4D4. This study suggests that structurally and functionally dissimilar 3D spheroids can be generated from the same type of cells on the surfaces of different physicochemical properties without any chemical treatment or genetic manipulation.


Assuntos
Neoplasias , Esferoides Celulares , Adesão Celular , Comunicação Celular , Matriz Extracelular , Polímeros
15.
ACS Nano ; 13(11): 13092-13099, 2019 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-31600440

RESUMO

Block copolymer (BCP) lithography is an effective nanopatterning methodology exploiting nanoscale self-assembled periodic patterns in BCP thin films. This approach has a critical limitation for nonplanar substrate geometry arising from the reflow and modification of BCP films upon the thermal or solvent annealing process, which is inevitable to induce the mobility of BCP chains for the self-assembly process. Herein, reflow-free, 3D BCP nanopatterning is demonstrated by introducing a conformally grown adlayer by the initiated chemical vapor deposition (iCVD) process. A highly cross-linked poly(divinylbenzene) layer was deposited directly onto the BCP thin film surface by iCVD, which effectively prevented the reflow of BCP thin film during an annealing process. BCP nanopatterns could be stabilized on various substrate geometry, including a nonplanar deformed polymer substrate, a pyramid shape substrate, and a graphene fiber surface. A fiber-type hydrogen evolution reaction (HER) catalyst is suggested by stabilizing lamellar Pt nanopatterns on severely rough graphene fiber surfaces.

16.
ACS Appl Mater Interfaces ; 11(32): 29113-29123, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31333023

RESUMO

Polymer dielectric materials with hydroxyl functionalities such as poly(4-vinylphenol) and poly(vinyl alcohol) have been utilized widely in organic thin-film transistors (OTFTs) because of their excellent insulating performance gained by hydroxyl-mediated cross-linking. However, the polar hydroxyl functionality also deleteriously affects the performance of OTFTs and significantly impairs the device stability. In this study, a sub-20 nm, high-k copolymer dielectric with hydroxyl functionality, poly(2-hydroxyethyl acrylate-co-di(ethylene glycol) divinyl ether), was synthesized in the vapor phase via initiated chemical vapor deposition. The inherently dry environment offered by the vapor-phase polymer synthesis prompted the snuggling of polar hydroxyl functionalities into the bulk polymer film to form a molecular thin hydrophobic skin layer at its surface, verified by near-edge X-ray absorption fine structure analysis. The chemical composition of the copolymer dielectric was optimized systematically to achieve high dielectric constant (k ≈ 6.2) as well as extremely low leakage current densities (less than 3 × 10-8 A/cm2 in the range of ±2 MV/cm) even with sub-20 nm thickness, leading to one of the highest capacitance (higher than 300 nF/cm2) achieved by a single polymer dielectric to date. Exploiting the structural advantage of the cross-linked high-k polymer dielectric, high-performance OTFTs were obtained. Notably, the spontaneously formed molecular thin, hydrophobic skin layer in the copolymer film substantially suppressed the hysteresis in the transistor operation. The trap analysis also suggested the formation of bulk trap with a high energy barrier and sufficiently low trap densities at the semiconductor/dielectric interface, owing to the surface skin layer. Furthermore, the OTFTs with the -OH-containing copolymer dielectric showed an unprecedentedly excellent operational stability. No apparent OTFT degradation was observed up to 50 000 s of high constant voltage stress (corresponding to the applied electric field of 1.4 MV/cm) because of the markedly suppressed interfacial trap density by the hydrophobic skin layer, together with the current compensation by the bulk hydroxyl functionalities. We believe that the surface modification-free, one-step polymer dielectric synthetic strategy will provide a new insight into the design of polymer dielectric materials for high-performance, low-power soft electronic devices with high operational stability.

17.
ACS Appl Mater Interfaces ; 10(44): 38449-38458, 2018 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-30360069

RESUMO

We present the design of a novel pH-responsive drug release system that is achieved by solventless encapsulation of drugs within a microporous membrane using a thin capping layer of biodegradable poly(methacrylic anhydride) (PMAH) coating. The coating was synthesized via a mild vapor polymerization process, namely, initiated chemical vapor deposition, which allowed perfect retention of the anhydride groups during deposition. The synthesized polyanhydride underwent degradation upon exposure to aqueous buffers, resulting in soluble poly(methacrylic acid). The degradation behavior of PMAH is highly pH-dependent, and the degradation rate under pH 10 is 15 times faster than that under pH 1. The release profile of a model drug rifampicin clearly exhibited two stages: the initial stage when the coatings were being degraded but the drugs were well stored and the second stage when drugs were gradually exposed to the medium and released. The drug release also showed strong pH responsiveness where the duration of the initial stage under pH 1 was more than 7 and 3 times longer than that under pH 10 and 7.4, respectively, and the release rates at pH 7.4 and 10 were significantly faster than that at pH 1. The pH-dependent degradation of the encapsulant thus enabled good preservation of drugs under low-pH environment but high drug release efficiency under neutral and alkaline environment, suggesting potential applications in site-specific drug delivery systems.


Assuntos
Plásticos Biodegradáveis/química , Preparações de Ação Retardada/química , Sistemas de Liberação de Medicamentos , Liberação Controlada de Fármacos , Plásticos Biodegradáveis/farmacologia , Preparações de Ação Retardada/farmacologia , Portadores de Fármacos/química , Portadores de Fármacos/farmacologia , Humanos , Hidrogéis/química , Hidrogéis/farmacologia , Concentração de Íons de Hidrogênio , Polímeros/química , Ácidos Polimetacrílicos/química , Rifampina/química , Rifampina/farmacologia
18.
ACS Biomater Sci Eng ; 4(7): 2614-2622, 2018 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-33435124

RESUMO

Fabrication of new antibacterial surfaces has become a primary strategy for preventing device-associated infections (DAIs). Although considerable progress has recently been made in reducing DAIs, current antibacterial coating methods are technically complex and do not allow selective bacterial killing. Here, we propose novel anti-infective surfaces made of a cross-linked ionic polymer film that achieve selective bacteria killing while simultaneously favoring the survival of mammalian cells. A one-step polymerization process known as initiated chemical vapor deposition was used to generate a cross-linked ionic polymer film from 4-vinylbenzyl chloride and 2-(dimethylamino) ethyl methacrylate monomers in the vapor phase. In particular, the deposition process produced a polymer network with quaternary ammonium cross-linking sites, which provided the surface with an ionic moiety with an excellent antibacterial contact-killing property. This method confers substrate compatibility, which enables various materials to be coated with ionic polymer films for use in medical implants. Moreover, the ionic polymer-deposited surfaces supported the healthy growth of mammalian cells while selectively inhibiting bacterial growth in coculture models without any detectable cytotoxicity. Thus, the cross-linked ionic polymer-based antibacterial surface developed in this study can serve as an ideal platform for biomedical applications that require a highly sterile environment.

19.
ACS Appl Mater Interfaces ; 10(38): 32668-32677, 2018 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-30175915

RESUMO

A new fabrication method for an ultrathin (500 nm thick) pressure-sensitive adhesive (PSA) was demonstrated by utilizing a series of in situ cross-linked viscoelastic copolymer films. Viscoelastic films composed of poly(2-hydroxyethyl acrylate- co-2-ethylhexyl acrylate) were synthesized successfully in a one-step manner by an initiated chemical vapor deposition (iCVD) process, where free-radical polymerization is triggered in the vapor phase either by heat or UV, or a combination of both. In particular, the photoinitiated chemical vapor deposition method generated a highly cross-linked polymer film, whereas cross-linking of the copolymer film was suppressed greatly in the conventional thermal iCVD method. A combination of thermal and photoinitiated chemical vapor deposition could regulate the cross-linking density of the copolymer films. We controlled the cross-linking density of the copolymer films to exhibit a viscoelastic property so that they would readily adhere to various kinds of substrates with only 500 nm thick copolymer PSA. The adhesion performance of the PSA was systematically optimized by tuning the copolymer composition as well as the cross-linking density, and consequently a high shear strength of more than 85.2 ± 5 N/cm2 was achieved despite the 500 nm thickness. In addition, the PSA was completely transparent. We expect that the ultrathin PSAs developed in this work will be utilized widely for the realization of various soft electronic devices, which usually require strong adhesion, tunable viscoelastic properties, and optical transparency.

20.
Adv Healthc Mater ; 6(20)2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28714572

RESUMO

Rapid and convenient isolation of nucleic acids (NAs) from cell lysate plays a key role for onsite gene expression analysis. Here, this study achieves one-step and efficient capture of NA directly from cell lysate by developing a cationic surface-modified mesh filter (SMF). By depositing cationic polymer via vapor-phase deposition process, strong charge interaction is introduced on the surface of the SMF to capture the negatively charged NAs. The NA capturing capability of SMF is confirmed by X-ray photoelectron spectroscopy, fluorescent microscopy, and zeta potential measurement. In addition, the genomic DNAs of Escherichia Coli O157:H7 can be extracted by the SMF from artificially infected food, and fluorescent signal is observed on the surface of SMF after amplification of target gene. The proposed SMF is able to provide a more simplified, convenient, and fast extraction method and can be applied to the fields of food safety testing, clinical diagnosis, or environmental pollutant monitoring.


Assuntos
DNA Bacteriano/isolamento & purificação , Escherichia coli O157/genética , Polímeros/química , Extração em Fase Sólida/métodos , DNA Bacteriano/análise , Monitoramento Ambiental , Genoma Bacteriano , Limite de Detecção , Microscopia Eletrônica de Varredura , Espectroscopia Fotoeletrônica , Extração em Fase Sólida/instrumentação , Análise Espectral Raman , Propriedades de Superfície
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