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1.
J Sep Sci ; 46(17): e2300206, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37385796

RESUMEN

The addition of bisphenol A has been frequently used in industrial manufacturing because it imparts plastic products with characteristics such as transparency, durability, and excellent impact resistance. However, its widespread use raises concerns about potential leakage into the surrounding environment, which poses a significant risk to human health. In this study, molecularly imprinted polymers with specific recognition of bisphenol A were synthesized through surface-initiated atom transfer radical polymerization using poly(glycidyl methacrylate-co-ethylene glycol dimethacrylate) as the substrate, bisphenol A as the template molecule, 4-vinylpyridine as the monomer, and ethylene glycol dimethacrylate as the cross-linker. The bisphenol A adsorption capacity was experimentally investigated, and the kinetic analysis of the molecularly imprinted polymers produced an adsorption equilibrium time of 25 min, which is consistent with the pseudo-second-order kinetic model. The results of the static adsorption experiments exhibited consistency with the Langmuir adsorption model, revealing a maximum adsorption capacity of 387.2 µmol/g. The analysis of molecularly imprinted polymers-enriched actual samples using high-performance liquid chromatography demonstrated excellent selectivity for bisphenol A, with a linear range showing 93.4%-99.7% recovery and 1.1%-6.4% relative standard deviation, demonstrating its high potential for practical bisphenol A detection and enrichment applications.

2.
Molecules ; 25(1)2020 Jan 03.
Artículo en Inglés | MEDLINE | ID: mdl-31947738

RESUMEN

This paper introduces the synthesis of well-defined 2-(tert-butylamino)ethyl methacrylate-b-poly(ethylene glycol) methyl ether methacrylate diblock copolymer, which has been grafted onto mesoporous silica nanoparticles (PTBAEMA-b-PEGMEMA-MSNs) via atom transfer radical polymerization (ATRP). The ATRP initiators were first attached to the MSN surfaces, followed by the ATRP of 2-(tert-butylamino)ethyl methacrylate (PTBAEMA). CuBr2/bipy and ascorbic acid were employed as the catalyst and reducing agent, respectively, to grow a second polymer, poly(ethylene glycol) methyl ether methacrylate (PEGMEMA). The surface structures of these fabricated nanomaterials were then analyzed using Fourier Transform Infrared (FTIR) spectroscopy. The results of Thermogravimetric Analysis (TGA) show that ATRP could provide a high surface grafting density for polymers. Dynamic Light Scattering (DLS) was conducted to investigate the pH-responsive behavior of the diblock copolymer chains on the nanoparticle surface. In addition, multifunctional pH-sensitive PTBAEMA-b-PEGMEMA-MSNs were loaded with doxycycline (Doxy) to study their capacities and long-circulation time.


Asunto(s)
Doxiciclina/química , Portadores de Fármacos , Metacrilatos/química , Nanopartículas/química , Polietilenglicoles/química , Dióxido de Silicio/química , Portadores de Fármacos/síntesis química , Portadores de Fármacos/química , Polimerizacion
3.
Nano Lett ; 18(1): 314-325, 2018 01 10.
Artículo en Inglés | MEDLINE | ID: mdl-29232130

RESUMEN

We propose an effective siRNA delivery system by preparing poly(DAMA-HEMA)-multilayered gold nanoparticles using multiple surface-initiated atom transfer radical polymerization processes. The polymeric multilayer structure is characterized by transmission electron microscopy, matrix-associated laser desorption/ionization time-of-flight mass spectrometry, UV-vis spectroscopy, Fourier transform infrared spectroscopy, dynamic light scattering, and ζ-potential. The amount of siRNA electrostatically incorporated into the nanoparticle can be tuned by the number of polymeric shells, which in turn influences the cellular uptake and gene silencing effect. In a bioreductive environment, the interlayer disulfide bond breaks to release the siRNA from the degraded polymeric shells. Intravenously injected c-Myc siRNA-incorporated particles accumulate in the tumor site of a murine lung carcinoma model and significantly suppress the tumor growth. Therefore, the combination of a size-tunable AuNP core and an ATRP-functionalized shell offers control and versatility in the effective delivery of siRNA.


Asunto(s)
Oro/química , Neoplasias Pulmonares/terapia , Nanopartículas del Metal/química , ARN Interferente Pequeño/administración & dosificación , ARN Interferente Pequeño/uso terapéutico , Tratamiento con ARN de Interferencia , Células A549 , Animales , Cationes/química , Humanos , Neoplasias Pulmonares/genética , Nanopartículas del Metal/ultraestructura , Ratones , Polimerizacion , Polímeros/química , Proteínas Proto-Oncogénicas c-myc/genética , Interferencia de ARN , ARN Interferente Pequeño/genética , Propiedades de Superficie
4.
Sheng Wu Yi Xue Gong Cheng Xue Za Zhi ; 36(2): 260-266, 2019 Apr 25.
Artículo en Zh | MEDLINE | ID: mdl-31016943

RESUMEN

A diblock copolymer, poly(ethylene glycol) methacrylate-block-glycidyl methacrylate (PEGMA-GMA), was prepared on glass substrate by surface-initiated atom transfer radical polymerization (SI-ATRP), and endothelial specific peptide Arg-Glu-Asp-Val (REDV) was immobilized at the end of the PEGMA-GMA polymer brush by ring opening reaction through the rich epoxy groups in the GMA. The structure and hydrophilicity of the polymer brushes were characterized by static water contact angle, X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM). The results showed that the REDV modified copolymer brushes were successfully constructed on the glass substrates. The REDV peptide immobilized onto surface was quantitatively characterized by ultraviolet-visible spectroscopy (UV-VIS). The blood compatibility of the coating was characterized by recalcification time and platelet adhesion assay. The results showed that the polymer coating had good blood compatibility. The multifunctional active polymer coating with PEGMA and peptide produced an excellent prospect in surface construction with endothelial cells selectivity.


Asunto(s)
Materiales Biocompatibles , Metacrilatos , Adhesividad Plaquetaria , Polietilenglicoles , Células Cultivadas , Células Endoteliales , Vidrio , Humanos , Proteínas Inmovilizadas , Oligopéptidos , Polímeros , Propiedades de Superficie
5.
Small ; 13(21)2017 06.
Artículo en Inglés | MEDLINE | ID: mdl-28383186

RESUMEN

The propagation control of chemical waves via a pentagonal patterned structure in a self-oscillating polymer brush composed of N-isopropylacrylamide and a metal catalyst for the Belousov-Zhabotinsky (BZ) reaction is reported. The patterned self-oscillating polymer brush is prepared by combining surface-initiated atom transfer radical polymerization and maskless photolithography. Surface modification is confirmed by X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, 3D measuring laser microscopy, and fluorescence microscopy. The polymer brush patterns are fabricated with gaps between the pentagonal regions, and investigations on the effect of the gap distance on the BZ reaction reveal that at the appropriate distance, chemical waves propagate across the array from the plane to the corner between the patterns. Unidirectional control is achieved not only in the 1D array, but also in a 2D curved array. This patterned self-oscillating polymer brush is a novel and advantageous approach for creating an autonomous dynamic soft interface.

6.
Macromol Rapid Commun ; 37(13): 1079-86, 2016 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-27145108

RESUMEN

Self-initiated photografting polymerization is used to couple the polymerizable initiator monomer 2-(2-chloropropanoyloxy)ethyl acrylate to a range of polymeric substrates. The technique requires only UV light to couple the initiator to surfaces. The initiator surface density can be varied by inclusion of a diluent monomer or via selection of initiator and irradiation parameters. The functionality of the initiator surface is demonstrated by subsequent surface-initiated atom transfer radical polymerization. Surfaces are characterized by x-ray photoelectron spectroscopy (XPS), ellipsometry, and atomic force microscopy (AFM), and UV-induced changes to the initiator are assessed by (1) H NMR and gel permeation chromatography (GPC). This is the first time this one-reactant one-step technique has been demonstrated for creating an initiator surface of variable density.


Asunto(s)
Acrilatos/química , Polimerizacion , Polímeros/síntesis química , Microscopía de Fuerza Atómica , Procesos Fotoquímicos , Espectroscopía de Fotoelectrones , Polímeros/química , Propiedades de Superficie , Rayos Ultravioleta
7.
Food Chem ; 439: 138167, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38071847

RESUMEN

The work provided a method for synthesizing a simple fluorescent molecularly imprinted polymer by surface-initiated atom transfer radical polymerization (SI-ATRP) and its application in real sample. Poly(glycidyl methacrylate-co-ethylene glycol dimethacrylate) microspheres were selected as a matrix, 4-vinylpyridine, ethylene glycol dimethacrylate, 2,4-dichlorophenoxyacetic acid (2,4-D) as functional monomer, cross-linker and template molecule, respectively, to fabricate MAR@MIP with core-shell structure. For comparison, carbon dot (CD) as a fluorescence source was synthesized with o-phenylenediamine and tryptophan as precursors via hydrothermal method and integrated into MIP to acquire MAR@CD-MIP. MAR@CD-NIP was also prepared without adding the template molecule. The adsorption capacity of MAR@CD-MIP reached 104 mg g-1 for 2,4-D, which was higher than that of MAR@MIP (60 mg g-1). However, the adsorption capacity of MAR@CD-NIP was only 13.2 mg g-1. The linear range of fluorescence detection for 2,4-D was 18-72 µmol/L, and the limit of detection (LOD) was 0.35 µmol/L. The fluorescent MAR@CD-MIP was successfully applied in enrichment of lettuce samples. The recoveries of the three spiked concentrations of 2,4-D in lettuce were tested by fluorescence spectrophotometry and ranged in 97.3-101.7 %. Meanwhile, the results were also verified by HPLC. As a result, bi-functional molecularly imprinted resin was successfully fabricated to detect and enrich 2,4-D in real samples, and exhibited good selectivity, sensitivity and great application prospect in food detection.


Asunto(s)
Herbicidas , Impresión Molecular , Carbono , Lactuca , Polímeros/química , Fenoxiacetatos , Ácido 2,4-Diclorofenoxiacético , Impresión Molecular/métodos
8.
Carbohydr Polym ; 319: 121160, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37567704

RESUMEN

The ingenious design of sustainable thermoplastic elastomers (STPEs) is of great significance for the goal of the sustainable development. However, the preparation of STPEs with good mechanical performance is still complicated and challenging. Herein, to achieve a simple preparation of STPEs with strong mechanical properties, two biobased monomers (tetrahydrofurfuryl methacrylate (THFMA) and lauryl methacrylate (LMA)) were copolymerized into poly (THFMA-co-LMA) (PTL) and grafted onto TEMPO oxidized cellulose nanofiber (TOCN) via one-pot surface-initiated atom transfer radical polymerization (SI ATRP). The grafting modified TOCN could be self-assembled into nano-enhanced phases in STPEs, which are conducive to the double enhancement of the strength and toughness of the STPEs, and the size of nano-enhanced phases is mainly affected by TOCN fiber length and molecular weight of grafting chains. Especially, with the addition of 7 wt% TOCN, tensile strength, tensile strain, toughness, and glass transition temperature (Tg) of TOCN based STPEs (TOCN@PTL) exhibited 140 %, 36 %, 215 %, and 6.8 °C increase respectively, which confirmed the leading level in the field of bio-based elastomers. In general, this work constitutes a proof for the chemical modification and self-assembly behavior of TOCN by one-pot SI ATRP, and provides an alternative strategy for the preparation of high-performance STPEs.

9.
J Chromatogr A ; 1689: 463774, 2023 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-36630850

RESUMEN

A hydrophilic adsorbent (Cys@poly(AMA)@MAR) was successfully prepared for the enrichment of N-glycopeptides via surface-initiated atom transfer radical polymerization (SI-ATRP) and photo-initiated "thiol-ene" reaction using monodisperse macroporous adsorbent resin (MAR) as adsorption matrix. Due to the presence of electron-deficient acrylic groups and electron-rich vinyl groups in allyl methacrylate (AMA), both of them can participate in free radical reaction. Therefore, the polymerization time of SI-ATRP was optimized. The resulting poly(AMA)@MAR was modified with l-cysteine (L-Cys) via photo-initiated "thiol-ene" reaction, and the amount of vinyl retained was determined by measuring the adsorption of Cu2+. The Cys@poly(AMA)@MAR pendant brushes with high density of amine and carboxyl groups could capture N-glycopeptides from IgG digest and human serum digest by hydrophilic interaction. The 22 N-glycopeptides were identified from IgG digest and the limit of detection reached 10 fmol. The 319 N-glycosylation sites and 583 N-glycopeptides were identified from 2 µL human serum digest and mapped to 147 glycoproteins. It demonstrates great potential and commercialization prospects for the enrichment of N-glycopeptides.


Asunto(s)
Glicopéptidos , Compuestos de Sulfhidrilo , Humanos , Polimerizacion , Química Clic/métodos , Adsorción , Cisteína , Inmunoglobulina G , Interacciones Hidrofóbicas e Hidrofílicas
10.
Polymers (Basel) ; 14(23)2022 Nov 27.
Artículo en Inglés | MEDLINE | ID: mdl-36501554

RESUMEN

Previous reports have shown that colloidal crystal (CC) films with visible Bragg reflection characteristics can be fabricated by the surface modification of monodisperse silica particles (SiPs) with poly(methyl methacrylate) (PMMA) chains, followed by hot-pressing at 150 °C. However, the reflection bands of the CC films were very broad due to their relative disordering of SiPs. In this report, we attempted to fabricate the CC films using SiPs surface-modified with poly(n-octyl acrylate) (POA) chains by hot-pressing. When the cast films of POA-grafted SiPs were prepared by hot-pressing at 100 °C, the reflection bands were narrow rather than those of CC films of PMMA-grafted SiPs. This can be ascribed to easy disentanglement of POA chains during the hot-pressing process, thereby enabling the formation of well-ordered CC structures. Moreover, the reflection colors of CC films could be easily tuned by controlling the molecular weight of POA chains grafted on the SiP surface.

11.
Polymers (Basel) ; 14(17)2022 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-36080763

RESUMEN

A novel dual green and red-emitting photoluminescent polymer composite ZnAl2O4:Mn-bonded GO/polymethyl methacrylate (PMMA) was synthesized in a single-step reaction by surface-initiated atom transfer radical polymerization (SI-ATRP). The polymer chain was surface-initiated from the ZnAl2O4:Mn/GO, and the final products have a homogenous photoluminescent property from ZnAl2O4:Mn and better mechanical properties strengthened by graphene oxide (GO). The morphologies of ZnAl2O4:Mn/GO and the polymer composites were verified by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). X-ray diffraction analysis (XRD) revealed the two valence states of Mn (Mn2+, Mn4+) existing in the ZnAl2O4 host lattice, while Fourier-transform infrared spectroscopy (FTIR) spectra proved the transference of the active group, C-Br, from the initiator to the monomer during the polymerization. Gel permeation chromatography (GPC) shows the narrow dispersity of polymer composites fabricated through SI-ATRP. The SEM and FTIR results show the successful 'graft' of the polymer chains from the surface of ZnAl2O4:Mn/GO. The dual green and red-emitting polymer composites were synthesized, confirmed by the photoluminescence (PL) and photoluminescence excitation (PLE) results.

12.
ACS Appl Bio Mater ; 5(4): 1364-1390, 2022 04 18.
Artículo en Inglés | MEDLINE | ID: mdl-35377592

RESUMEN

Bacteria-assisted infections on biomaterials used inside a body as an implant/device are one of the major threats to human health. Microbial-resistant coatings on biomaterials can potentially be considered to mitigate the biomaterial-associated infections. Usually biomaterials with leachable antimicrobial coatings, though economically attractive, provide only short-term protection of the surface against bacteria. Therefore, a stable, nonfouling or bactericidal, and biocompatible polymeric coating is highly desirable. In this regard, polymer brushes, defined as polymer chains tethered to a surface by one end, with suitable anti-infective functionality, represent a useful class of stable coatings which are covalently connected to the underlying surface, thus prolonging the infection resistance of the coated surface. Surface-initiated atom transfer radical polymerization (SI-ATRP) is a versatile technique for the generation of polymeric brushes via "grafting from" way. In this review, we have attempted to give a brief overview about the recent developments of surface coatings by infection-resistant polymer brushes synthesized via SI-ATRP and their applications in the biomedical field. On the basis of their charges, these anti-infective brushes can be classified into five different categories such as neutral, cationic, anionic, zwitterionic, and mixed brushes. The working mechanism of each type of brush in repelling (nonfouling/bacteriostatic) and/or killing (bactericidal) the bacteria has also been discussed. A brief summary of their future scope is also highlighted.


Asunto(s)
Materiales Biocompatibles , Polímeros , Antibacterianos/farmacología , Humanos , Polimerizacion , Propiedades de Superficie
13.
Macromol Biosci ; 22(12): e2200292, 2022 12.
Artículo en Inglés | MEDLINE | ID: mdl-36122179

RESUMEN

Blood loss causes an estimated 1.9 million deaths per year globally, making new methods to stop bleeding and promote clot formation immediately following injury paramount. The fabrication of functional hemostatic materials has the potential to save countless lives by limiting bleeding and promoting clot formation following an injury. This work describes the melt manufacturing of poly(ε-caprolactone) nanofibers and their chemical functionalization to produce highly scalable materials with enhanced blood clotting properties. The nanofibers are manufactured using a high throughput melt coextrusion method. Once isolated, the nanofibers are functionalized with polymers that promote blood clotting through surface-initiated atom transfer radical polymerization. The functional nanofibers described herein speed up the coagulation cascade and produce more robust blood clots, allowing for the potential use of these functional nonwoven mats as advanced bandages.


Asunto(s)
Hemostáticos , Nanofibras , Trombosis , Humanos , Nanofibras/química , Coagulación Sanguínea , Hemostáticos/química , Vendajes , Hemorragia
14.
Colloids Surf B Biointerfaces ; 217: 112705, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35863235

RESUMEN

A composite immobilized-metal affinity agarose particle was designed for the selective separation and purification of histidine-tagged proteins from complicated biological samples. The composite particle was constructed using superporous agarose particles as supporting matrix, flexible copolymer brushes as scaffolds to render higher ligand densities, and Ni2+-chelated iminodiacetic acids as recognition elements. Superporous agarose composite particles endow high permeability and interfering substance tolerance. The copolymer brush was prepared by surface-initiated atom transfer radical polymerization of N-isopropylacrylamide and glycidyl methacrylate, followed by iminodiacetic acids and Ni2+ ions. The physical and chemical properities of the composite particle were thoroughly investigated. The composite particles were shown to be able to selectively separate histidine-tagged recombinant proteins in the presence of high quantities of interfering chemicals in a model protein-binding experiment. By altering the temperature, the protein binding of the composite particles can be modulated. The superporous agarose particles supported polymer brush enables fast and efficient separation and purification of target proteins with high permeability, low backpressure, and high interfering matrix tolerance, which pave the path for bioseparation through designing and fabrication of novel agarose particles-based functional materials.


Asunto(s)
Histidina , Polímeros , Cromatografía de Afinidad/métodos , Geles , Polímeros/química , Proteínas/química , Sefarosa
15.
Macromol Biosci ; 22(5): e2100454, 2022 05.
Artículo en Inglés | MEDLINE | ID: mdl-35102705

RESUMEN

Micropatterned polymer brushes have attracted attention in several biomedical areas, i.e., tissue engineering, protein microarray, biosensors, etc., for precise arrangement of biomolecules. Herein, a facile and scalable approach is reported to create microtextured polymer brushes with the ability to generate different type of protein patterns. Nanosecond fiber laser is exploited to generate micropatterns on poly(poly(ethylene glycol) methacrylate) (polyPEGMA) brush modified Ti alloy substrate. Surface initiated atom transfer radical polymerization is employed to grow PolyPEGMA brush (11-87 nm thick) on Ti alloy surface immobilized with initiator having an initiator density (σ*) of 1.5 initiators per nm2 . Polymer brushes are then selectively laser ablated and their presence on nontextured area is confirmed by atomic force microscopy, fluorescence microscopy, and X-ray photoelectron spectroscopy. Spatial orientation of biomolecules is first achieved by nonspecific protein adsorption on areas ablated by the laser, via physisorption. Further, patterned brushes of polyPEGMA are modified to activated ester that gives rise to protein conjugation specifically on nonlaser ablated brush areas. Moreover, the laser ablated brush modified patterned template is also successfully utilized for generating alternate patterns of bacteria. This promising technique can be further extended to create interesting patterns of several biomolecules which are of great interest to biomedical research community.


Asunto(s)
Rayos Láser , Polímeros , Aleaciones , Microscopía de Fuerza Atómica , Polimerizacion , Polímeros/química , Propiedades de Superficie
16.
Sci Technol Adv Mater ; 12(1): 015003, 2011 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-27877380

RESUMEN

We report the fabrication of shortened electrospun polymer fibers with a well-defined concentrated polymer brush. We first prepared electrospun nanofibers from a random copolymer of styrene and 4-vinylbenzyl 2-bromopropionate, with number-average molecular weight Mn=105 200 and weight-average molecular weight Mw=296 700 (Mw/Mn=2.82). The fibers had a diameter of 593±74 nm and contained initiating sites for surface-initiated atom transfer radical polymerization (SI-ATRP). Then, SI-ATRP of hydrophilic styrene sodium sulfonate (SSNa) was carried out in the presence of a free initiator and the hydrophobic fibers. Gel permeation chromatography confirmed that Mn and Mw/Mn values were almost the same for free polymers and graft polymers. Mn agreed well with the theoretical prediction, and Mw/Mn was relatively low (<1.3) in all the examined cases, indicating that this polymerization proceeded in a living manner. Using the values of the graft amount measured by Fourier transform infrared spectroscopy, the surface area, and Mn, we calculated the graft density σ as 0.22 chains nm-2. This value was nearly equal to the density obtained on silicon wafers (σ=0.24 chains nm-2), which is categorized into the concentrated brush regime. Finally, we mechanically cut the fibers with a concentrated poly(SSNa) brush by a homogenizer. With increasing cutting time, the fiber length became shorter and more homogenous (11±17 µm after 3 h). The shortened fibers exhibited excellent water dispersibility owing to the hydrophilic poly(SSNa) brush layer.

17.
Food Chem ; 358: 129907, 2021 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-33930712

RESUMEN

Rapid detection of pathogenic bacteria particularly in food samples demands efficient separation and enrichment strategies. Here, hydrophilic temperature-responsive boronate affinity magnetic nanocomposites were established for selective enrichment of bacteria. The thermo-responsive polymer brushes were developed by surface-initiated atom transfer radical polymerization of N-isopropylacrylamide (NIPAm) and allyl glycidyl ether (AGE), followed by a reaction of epoxy groups, and incorporation of fluorophenylboronic acid. The physical and chemical characteristics of the magnetic nanocomposites were analyzed systematically. After optimization, S. aureus and Salmonella spp. showed high binding capacities of 32.14 × 106 CFU/mg and 50.98 × 106 CFU/mg in 0.01 M PBS (pH 7.4) without bacteria death. Bacterial bindings can be controlled by altering temperature and the application of competing monosaccharides. The nanocomposite was then utilized to enrich S. aureus and Salmonella spp. from the spiked tap water, 25% milk, and turbot extraction samples followed by multiplex polymerase chain reaction (mPCR), which resulted in high bacteria enrichment, and demonstrated great potential in separation of bacteria from food samples.


Asunto(s)
Bacterias/aislamiento & purificación , Microbiología de Alimentos/instrumentación , Microbiología de Alimentos/métodos , Nanocompuestos/química , Acrilamidas/química , Animales , Bacterias/metabolismo , Técnicas Bacteriológicas/instrumentación , Técnicas Bacteriológicas/métodos , Concentración de Iones de Hidrógeno , Interacciones Hidrofóbicas e Hidrofílicas , Fenómenos Magnéticos , Leche/microbiología , Polimerizacion , Polímeros/química , Salmonella/aislamiento & purificación , Salmonella/metabolismo , Staphylococcus aureus/metabolismo , Temperatura , Microbiología del Agua
18.
ACS Appl Bio Mater ; 4(11): 7893-7902, 2021 11 15.
Artículo en Inglés | MEDLINE | ID: mdl-35006770

RESUMEN

Infectious diseases triggered by bacteria cause a severe risk to human health. To counter this issue, surfaces coated with antibacterial materials have been widely used in daily life to kill these bacteria. The substrates enabled with a hybrid kill and release strategy can be employed not only to kill the bacteria but also to wash them using external stimuli (temperature, pH, etc.). Utilizing this concept, we develop thermoresponsive antibacterial-cellulose papers to exhibit hybrid kill and release properties. Thermoresponsive copolymers [p(NIPAAm-co-AEMA)] are grafted on cellulose papers using a surface-initiated atom transfer radical polymerization approach for bacterial debris release. Later for antibacterial properties, silver nanoparticles (AgNPs) are immobilized on thermoresponsive copolymer-grafted cellulose papers using electrostatic interactions. We confirm the thermoresponsive copolymer grafting and AgNP coating by attenuated total reflection Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy. Thermoresponsiveness and reusability of the modified cellulose papers are confirmed through water contact angle measurements. The interaction potency between AgNPs and modified cellulose is validated by inductively coupled plasma atomic emission spectroscopy analysis. Gram-negative bacteria Escherichia coli (E. coli DH5-α) is used to demonstrate antibacterial hybrid kill and release performance. Agar-diffusion testing demonstrates the antibacterial nature of the modified cellulose papers. The fluorescence micrograph reveals that modified cellulose papers can effectively release almost all the dead bacterial debris from their surfaces after thermal stimulus wash. The modified cellulose paper surfaces are expected to have wide applications in the field of exploring more antibacterial and smart surfaces.


Asunto(s)
Escherichia coli , Nanopartículas del Metal , Antibacterianos/farmacología , Bacterias , Celulosa/farmacología , Humanos , Nanopartículas del Metal/química , Polimerizacion , Polímeros/química , Plata/farmacología
19.
J Biomater Sci Polym Ed ; 32(5): 678-693, 2021 04.
Artículo en Inglés | MEDLINE | ID: mdl-33250001

RESUMEN

Poly(dimethylsiloxane) (PDMS) elastomer is now a well-known material for packaging implantable biomedical micro-devices owing to unique bulk properties such as biocompatibility, low toxicity, excellent rheological properties, good flexibility, and mechanical stability. Despite the desirable bulk characteristics, PDMS is generally regarded as a high-flux material for oxygen and water vapor to penetrate compared with other polymeric barrier materials, which is related to the defect-induced penetration through the packaging coating prepared by the traditional deposition techniques. Besides, its hydrophobic nature causes serious fouling problems and limits the practical application of PDMS-based devices. In this work, the performance of silicone thin films as a packaging layer was improved by the fabrication of the roller-casted multiple thin layers to minimize a defect-induced failure. To confer hydrophilicity and cell fouling resistance, high-density and well-defined poly(oligo(ethylene glycol) methacrylate) (POEGMA) brushes were tethered via the surface-initiated atom transfer radical polymerization (SI-ATRP) technique on the roller-casted multiple thin PDMS layers. The characteristics of fabricated substrates were determined by static water contact angle measurement, X-ray photoelectron spectroscopy, and attenuated total reflection-Fourier transform infrared spectroscopy. In vitro cell behavior of POEGMA-grafted PDMS substrates was evaluated to examine cell-fouling resistance.


Asunto(s)
Incrustaciones Biológicas , Incrustaciones Biológicas/prevención & control , Adhesión Celular , Metacrilatos , Polimerizacion , Polímeros , Propiedades de Superficie
20.
Mater Sci Eng C Mater Biol Appl ; 118: 111465, 2021 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-33255047

RESUMEN

Biomaterials with anti-infective coatings are usually found to suffer from low cyto-compatibility and therefore, development of a stable, effective polymeric anti-bacterial substrate without compromising the biocompatibility is still an unmet challenge. Addressing this, a simple strategy for developing non-leaching antibacterial coating on a biodegradable substrate is reported here. The strategy can be utilized for mitigating serious biomedical implant related complications arising from generation of biocide resistant bacterial strains, losing antibacterial activity over time etc. without significantly compromising the cytocompatibility of the biomaterials. To develop the infection resistant yet cytocompatible biomaterials comprised of tartaric acid based biodegradable aliphatic polyester, we have primarily focussed on attaching anti-infective polymer brushes such as poly (2-hydroxyethyl methacrylate) (PHEMA), poly (poly (ethylene glycol) methacrylate) (PPEGMA) and poly[(2-methacryloyloxyethyl] trimethyl ammonium chloride) (PMETA) on hydroxyl functionalized polyester substrate via surface initiated atom transfer radical polymerization (SIATRP). The brushes were thoroughly characterized for reaction kinetics, grafting yield, surface density, topography and hydrophilicity. Among the various brushes, cationic polymer brush (PMETA) was found to exhibit highest antibacterial activity, with only ~3% and ~4% adherence of E. coli (Escherichia coli) and S. aureus (Staphylococcus aureus), respectively. In order to show its widespread use and also to vary initiator density, polylactic acid (PLA) was blended with this tartaric acid based aliphatic polyester and a 3D (three-dimensional) scaffold was fabricated by 3D printing using the blend. Finally, PMETA brush was grown onto the scaffold surface for various time periods and the evaluation of antibacterial activity (using gram positive and gram-negative bacteria) and cytocompatibility (using mammalian osteoblast cells) were carried out on the brush modified scaffold. A balance between antibacterial activity and cytocompatibility was found at optimum brush length achieved after 18 h of SIATRP suggesting that this composition offers a stable, non-leaching, anti-infective, but cytocompatible coating on biodegradable polymeric implant surface for addressing several biomaterials associated infections.


Asunto(s)
Escherichia coli , Staphylococcus aureus , Animales , Poliésteres , Polihidroxietil Metacrilato , Polimerizacion , Propiedades de Superficie
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