in-situ oxidative polymerization
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The additive manufacturing technique of direct laser writing by two-photon polymerization (2PP-DLW) enables the fabrication of three-dimensional microstructures with superior accuracy and flexibility. When combined with biomimetic hydrogel materials, 2PP-DLW can be used to recreate the microarchitectures of the extracellular matrix. However, there are currently only a limited number of hydrogels applicable for 2PP-DLW. In order to widen the selection of synthetic biodegradable hydrogels, in this work we studied the 2PP-DLW of methacryloylated and acryloylated poly(α-amino acid)s (poly(AA)s). The performance of these materials was compared to widely used poly(ethylene glycol) diacrylates (PEGdas) in terms of polymerization and damage thresholds, voxel size, line width, post-polymerization swelling and deformation. We found that both methacryloylated and acryloylated poly(AA) hydrogels are suitable to 2PP-DLW with a wider processing window than PEGdas. The poly(AA) with the highest degree of acryloylation showed the greatest potential for 3D microfabrication.
Implantable sensor devices require coatings that efficiently interface with the tissue environment to mediate biochemical analysis. In this regard, bioinspired polymer hydrogels offer an attractive and abundant source of coating materials. However, upon implantation these materials generally elicit inflammation and the foreign body reaction as a consequence of protein fouling on their surface and concomitant poor hemocompatibility. In this report we investigate a strategy to endow chitosan hydrogel coatings with antifouling properties by the grafting of polymer brushes in a "grafting-from" approach. Chitosan coatings were functionalized with polymer brushes of oligo(ethylene glycol) methyl ether methacrylate and 2-hydroxyethyl methacrylate using photoinduced single electron transfer living radical polymerization and the surfaces were thoroughly characterized by XPS, AFM, water contact angle goniometry, and in situ ellipsometry. The antifouling properties of these new bioinspired hydrogel-brush coatings were investigated by surface plasmon resonance. The influence of the modifications to the chitosan on hemocompatibility was assessed by contacting the surfaces with platelets and leukocytes. The coatings were hydrophilic and reached a thickness of up to 180 nm within 30 min of polymerization. The functionalization of the surface with polymer brushes significantly reduced the protein fouling and eliminated platelet activation and leukocyte adhesion. This methodology offers a facile route to functionalizing implantable sensor systems with antifouling coatings that improve hemocompatibility and pave the way for enhanced device integration in tissue.
- MeSH
- aktivace trombocytů účinky léků MeSH
- biokompatibilní potahované materiály chemie farmakologie MeSH
- biosenzitivní techniky metody MeSH
- buněčná adheze účinky léků MeSH
- chitosan chemie MeSH
- hydrogely chemie farmakologie MeSH
- implantabilní infuzní pumpy MeSH
- leukocyty cytologie účinky léků MeSH
- lidé MeSH
- methakryláty chemie MeSH
- polyethylenglykoly chemie MeSH
- polymerizace MeSH
- primární buněčná kultura MeSH
- trombocyty účinky léků MeSH
- volné radikály MeSH
- Check Tag
- lidé MeSH
- Publikační typ
- časopisecké články MeSH
Directing the organization of cells into a tissue with defined architectures is one use of biomaterials for regenerative medicine. To this end, hydrogels are widely investigated as they have mechanical properties similar to native soft tissues and can be formed in situ to conform to a defect. Herein, we describe the development of porous hydrogel tubes fabricated through a two-step polymerization process with an intermediate microsphere phase that provides macroscale porosity (66.5%) for cell infiltration. These tubes were investigated in a spinal cord injury model, with the tubes assembled to conform to the injury and to provide an orientation that guides axons through the injury. Implanted tubes had good apposition and were integrated with the host tissue due to cell infiltration, with a transient increase in immune cell infiltration at 1 week that resolved by 2 weeks post injury compared to a gelfoam control. The glial scar was significantly reduced relative to control, which enabled robust axon growth along the inner and outer surface of the tubes. Axon density within the hydrogel tubes (1744 axons/mm2) was significantly increased more than 3-fold compared to the control (456 axons/mm2), with approximately 30% of axons within the tube myelinated. Furthermore, implantation of hydrogel tubes enhanced functional recovery relative to control. This modular assembly of porous tubes to fill a defect and directionally orient tissue growth could be extended beyond spinal cord injury to other tissues, such as vascular or musculoskeletal tissue. STATEMENT OF SIGNIFICANCE: Tissue engineering approaches that mimic the native architecture of healthy tissue are needed following injury. Traditionally, pre-molded scaffolds have been implemented but require a priori knowledge of wound geometries. Conversely, hydrogels can conform to any injury, but do not guide bi-directional regeneration. In this work, we investigate the feasibility of a system of modular hydrogel tubes to promote bi-directional regeneration after spinal cord injury. This system allows for tubes to be cut to size during surgery and implanted one-by-one to fill any injury, while providing bi-directional guidance. Moreover, this system of tubes can be broadly applied to tissue engineering approaches that require a modular guidance system, such as repair to vascular or musculoskeletal tissues.
- MeSH
- axony účinky léků patologie MeSH
- hydrogely farmakologie MeSH
- jizva patologie MeSH
- lokomoce účinky léků MeSH
- maleimidy chemie MeSH
- mikrosféry MeSH
- myelinová pochva účinky léků metabolismus MeSH
- myši inbrední C57BL MeSH
- neuroglie patologie MeSH
- polyethylenglykoly chemie MeSH
- polymerizace MeSH
- poranění míchy patologie patofyziologie MeSH
- poréznost MeSH
- reagencia zkříženě vázaná chemie MeSH
- regenerace nervu účinky léků MeSH
- tkáňové podpůrné struktury chemie MeSH
- zadní končetina účinky léků fyziologie MeSH
- zvířata MeSH
- Check Tag
- ženské pohlaví MeSH
- zvířata MeSH
- Publikační typ
- časopisecké články MeSH
- Research Support, N.I.H., Extramural MeSH
Five poly(betaine) brushes were prepared, and their resistance to blood plasma fouling was studied. Two carboxybetaines monomers were copolymerized with 2-hydroxyethyl methacrylate (HEMA) to prepare novel hydrogels. By increasing the content of the zwitterionic comonomer, a 4-fold increase in the water content could be achieved while retaining mechanical properties close to the widely used poly(HEMA) hydrogels. All hydrogels showed an unprecedentedly low fouling from blood plasma. Remarkably, by copolymerization with 10 mol % of carboxybetaine acrylamide, hydrogels fully resistant to blood plasma were prepared.
- MeSH
- akrylamidy chemická syntéza MeSH
- betain chemie MeSH
- biokompatibilní materiály chemie MeSH
- hydrogely chemická syntéza MeSH
- krevní plazma chemie MeSH
- lidé MeSH
- methakryláty chemická syntéza MeSH
- polymerizace MeSH
- polymery chemie MeSH
- povrchová plasmonová rezonance MeSH
- povrchové vlastnosti MeSH
- spektroskopie infračervená s Fourierovou transformací MeSH
- voda chemie MeSH
- Check Tag
- lidé MeSH
- Publikační typ
- časopisecké články MeSH
- práce podpořená grantem MeSH
Research on the subject of smart biomaterials has become a cornerstone of tissue engineering and regenerative medicine. Herein, the authors report on developing magnetic hydrogels that combine high biocompatibility and remarkable activity in magnetic fields. We fabricated magnetic hydrogels based on poly(2-ethyl-2-oxazoline) (POx) via living ring-opening cationic polymerization with in-situ embedding of the carbonyl iron (CI) particles. Investigation was made as to the effect exerted by the concentration of CI on magnetic, viscoelastic/magnetorheological properties, the degree of equilibrium swelling, and cytotoxicity. The hydrogels exhibited an open pore structure, as evidenced by computed tomography (CT) imaging. Susceptibility measurements revealed the concentration-dependent field-induced particle restructuration indicating elongation/contraction of the material, thereby determining the potential for magneto-mechanical stimulation of the cells. The POx-based magnetic hydrogels were amphiphilic in character, showing decrease in their capability to hold liquid alongside increase in CI concentration. Viscoelastic measurements suggested that interaction occurred between the particles and matrix based on inconsistency between the experimental storage modulus and the Krieger-Dougherty model. The synthesized materials exhibited excellent biocompatibility toward the 3T3 fibroblast cell line in tests of extract toxicity and direct contact cytotoxicity (ISO standards). The unique combination of properties exhibited by the material - magneto-mechanical activity and biocompatibility - could prove favorable in fields such as biomedicine and biomechanics.
- MeSH
- buňky 3T3 MeSH
- fibroblasty účinky léků MeSH
- hydrogely chemická syntéza chemie farmakologie MeSH
- magnetické pole MeSH
- myši MeSH
- oxazoly chemická syntéza chemie farmakologie MeSH
- povrchové vlastnosti MeSH
- velikost částic MeSH
- viabilita buněk účinky léků MeSH
- zvířata MeSH
- Check Tag
- myši MeSH
- zvířata MeSH
- Publikační typ
- časopisecké články MeSH
Two-dimensional (2D) materials remain highly interesting for assembling three-dimensional (3D) structures, amongst others, in the form of macroscopic hydrogels. Herein, we present a novel approach for inducing chemical inter-sheet crosslinks via an ethylenediamine mediated reaction between Ti3C2Tx and graphene oxide in order to obtain a reduced graphene oxide-MXene (rGO-MXene) hydrogel. The composite hydrogels are hydrophilic with a stiffness of ~20 kPa. They also possess a unique inter-connected porous architecture, which led to a hitherto unprecedented ability of human cells across three different types, epithelial adenocarcinoma, neuroblastoma and fibroblasts, to form inter-connected three-dimensional networks. The attachments of the cells to the rGO-MXene hydrogels were superior to those of the sole rGO-control gels. This phenomenon stems from the strong affinity of cellular protrusions (neurites, lamellipodia and filopodia) to grow and connect along architectural network paths within the rGO-MXene hydrogel, which could lead to advanced control over macroscopic formations of cellular networks for technologically relevant bioengineering applications, including tissue engineering and personalized diagnostic networks-on-chip. STATEMENT OF SIGNIFICANCE: Conventional hydrogels are made of interconnected polymeric fibres. Unlike conventional case, we used hydrothermal and chemical approach to form interconnected porous hydrogels made of two-dimensional flakes from graphene oxide and metal carbide from a new family of MXenes (Ti3C2Tx). This way, we formed three-dimensional porous hydrogels with unique porous architecture of well-suited chemical surfaces and stiffness. Cells from three different types cultured on these scaffolds formed extended three-dimensional networks - a feature of extended cellular proliferation and pre-requisite for formation of organoids. Considering the studied 2D materials typically constitute materials exhibiting enhanced supercapacitor performances, our study points towards better understanding of design of tissue engineering materials for the future bioengineering fields including personalized diagnostic networks-on-chip, such as artificial heart actuators.
- MeSH
- grafit * MeSH
- hydrogely * MeSH
- lidé MeSH
- titan MeSH
- tkáňové inženýrství MeSH
- Check Tag
- lidé MeSH
- Publikační typ
- časopisecké články MeSH
- práce podpořená grantem MeSH
Inflammatory bowel disease (IBD) is a relapsing and remitting inflammatory disease affecting millions of people worldwide. The active phase of IBD is characterized by excessive formation of reactive oxygen species (ROS) in the intestinal mucosa, which further accelerates the inflammatory process. A feasible strategy for the IBD treatment is thus breaking the oxidation-inflammation vicious circle by scavenging excessive ROS with the use of a suitable antioxidant. Herein, we have developed a novel hydrogel system for oral administration utilizing sterically hindered amine-based redox polymer (SHARP) incorporating covalently bound antioxidant SHA groups. SHARP was prepared via free-radical polymerization by covalent crosslinking of 2-hydroxyethyl methacrylate (HEMA), poly(ethylene oxide) methyl ether methacrylate (PEGMA) and a SHA-based monomer, N-(2,2,6,6-tetramethyl-piperidin-4-yl)-methacrylamide. The SHARP hydrogel was resistant to hydrolysis and swelled considerably (∼90% water content) under the simulated gastrointestinal tract (GIT) conditions, and exhibited concentration-dependent antioxidant properties in vitro against different ROS. Further, the SHARP hydrogel was found to be non-genotoxic, non-cytotoxic, non-irritating, and non-absorbable from the gastrointestinal tract. Most importantly, SHARP hydrogel exhibited a statistically significant, dose-dependent therapeutic effect in the mice model of dextran sodium sulfate (DSS)-induced acute colitis. Altogether, the obtained results suggest that the SHARP hydrogel strategy holds a great promise with respect to IBD treatment.
- MeSH
- aminy MeSH
- hydrogely MeSH
- idiopatické střevní záněty * farmakoterapie MeSH
- kolitida * chemicky indukované farmakoterapie MeSH
- myši MeSH
- oxidace-redukce MeSH
- polymery MeSH
- zvířata MeSH
- Check Tag
- myši MeSH
- zvířata MeSH
- Publikační typ
- časopisecké články MeSH
Skin represents the largest organ in the human body, functioning as a protective barrier against environmental factors while playing a critical role in thermoregulation. Acne vulgaris is recognized as the most common dermatological condition affecting adolescents, and if left untreated, it can result in lasting skin damage and associated psychosocial challenges. This study aims to develop innovative polymeric biomaterials that could effectively support the treatment of acne vulgaris. The synthesis of these biomaterials involves the use of polyethylene glycol 6000, sodium alginate, and the antioxidant protein glutathione (GHS) to create polymeric hydrogels. These hydrogels were generated via a UV-mediated crosslinking process. To enhance the functional properties of the hydrogels, zinc oxide microparticles (ZnO), synthesized through a wet precipitation method, were incorporated into the formulations. Characterization of the ZnO was performed using Fourier-Transform Infrared Spectroscopy (FTIR), X-ray Diffraction (XRD), particle sizer analysis, and Scanning Electron Microscopy (SEM). Additionally, the bioactivity of the synthesized materials was evaluated through incubation in media simulating physiological body fluids. The cytotoxic effects of the biomaterials were assessed using an indirect test on mouse fibroblast (L929) cells, in accordance with ISO 10993-5 guidelines. The results of our research indicate that the developed biomaterials exhibit potential as a carrier for active substances, contributing positively to the treatment of acne vulgaris and potentially improving overall skin health.
- MeSH
- acne vulgaris farmakoterapie MeSH
- algináty chemie MeSH
- biokompatibilní materiály chemie farmakologie MeSH
- buněčné linie MeSH
- fibroblasty účinky léků metabolismus MeSH
- glutathion * metabolismus MeSH
- hydrogely * chemie MeSH
- kůže * účinky léků metabolismus MeSH
- lidé MeSH
- myši MeSH
- nosiče léků chemie MeSH
- oxid zinečnatý * chemie farmakologie MeSH
- regenerace účinky léků MeSH
- spektroskopie infračervená s Fourierovou transformací MeSH
- zvířata MeSH
- Check Tag
- lidé MeSH
- myši MeSH
- zvířata MeSH
- Publikační typ
- časopisecké články MeSH
Several studies have reported on application of cellulose particles for stabilizing Pickering emulsions (PE). Here we employ an original approach that involves using these particles as a part of advanced composite colloids made of conducting polymer polyaniline (PANI) and cellulose nanocrystals (CNC) or nanofibrils (CNF). PANI/cellulose particles were prepared using oxidative polymerization of aniline in situ in the presence of CNC or CNF. The type and amount of celluloses (CNC vs CNF) and concentration of precursors (aniline monomer and oxidant) used in the reaction determined properties of the colloidal particles, such as size, morphology and content of PANI. The particles demonstrated intriguing biological characteristics, including no cytotoxicity, antibacterial activity against Staphylococcus aureus and Escherichia coli, antioxidant activity and related immunomodulatory activity. For the first time, such composites were used to successfully stabilize oil-in-water PE with undecane or capric/caprylic triglyceride oils. The properties of the emulsions were determined by the PANI/cellulose particles and oil used. The key finding of the study is the demonstrated ability of PANI/cellulose particles to stabilize PE, as well as the excellent antioxidant activity and ROS scavenging action originating from PANI presence, indicating potential of such systems for use in biomedicine, particularly for wound healing.
We have developed nanoparticle-modified monoliths in pipette tips for selective and efficient enrichment of phosphopeptides. The 5 μL monolithic beds were prepared by UV-initiated polymerization in 200 μL polypropylene pipette tips and either iron oxide or hydroxyapatite nanoparticles were used for monolith modification. Iron oxide nanoparticles were prepared by a co-precipitation method and stabilized by citrate ions. A stable coating of iron oxide nanoparticles on the pore surface of the monolith was obtained via multivalent electrostatic interactions of citrate ions on the surface of nanoparticles with a quaternary amine functionalized poly(2-hydroxyethyl methacrylate-co-ethylene dimethacrylate) monolith. Hydroxyapatite nanoparticles were incorporated into the poly(2-hydroxyethyl methacrylate-co-ethylene dimethacrylate) monolith by simply admixing them in the polymerization mixture followed by in situ polymerization. The nanoparticle-modified monoliths were compared with commercially available titanium dioxide pipette tips. Performance of the developed and commercially available sorbents was demonstrated with the efficient and selective enrichment of phosphopeptides from peptide mixtures of α-casein and β-casein digests followed by off-line MALDI/MS analysis.
- MeSH
- chromatografie přístrojové vybavení metody MeSH
- fosfopeptidy chemie izolace a purifikace MeSH
- hydroxyapatit chemie MeSH
- kaseiny chemie MeSH
- nanočástice chemie MeSH
- poréznost MeSH
- syntetické pryskyřice chemická syntéza chemie MeSH
- železité sloučeniny chemie MeSH
- Publikační typ
- časopisecké články MeSH
- hodnotící studie MeSH
- práce podpořená grantem MeSH
