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Design and Synthesis of Quick Setting Nonswelling Hydrogels via Brush Polymers.

ABSTRACT: Brush polymers have emerged as components of novel materials that show huge potential in multiple disciplines and applications, including self-assembling photonic crystals, drug delivery vectors, biomimetic lubricants, and ultrasoft elastomers. However, an understanding of how this unique topology can affect the properties of highly solvated materials like hydrogels remain under investigated. Here, it is investigated how the high functionality and large overall size of brush polymers enhances the gelation kinetics of low polymer weight percent gels, enabling 100-fold faster gelation rates and 15-fold higher stiffness values than gels crosslinked by traditional star polymers of the same composition and polymer chain length. This work demonstrates that brush polymer topology provides a useful means to control gelation kinetics without the need to manipulate polymer composition or crosslinking chemistry. The unique architecture of brush polymers also results in restrained or even nonswelling behavior at different temperatures, regardless of the polymer concentration. Brush polymers therefore are an interesting tool for examining how high-functionality polymer building blocks can affect structure-property relationships and chemical kinetics in hydrogel materials, and also provide a useful rapidly-setting hydrogel platform with tunable properties and great potential for multiple material applications.

SUBMITTER: Jia F

PROVIDER: S-EPMC8373163 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Bioactive Peptide Brush Polymers via Photoinduced Reversible-Deactivation Radical Polymerization.

Project description:Harnessing metal-free photoinduced reversible-deactivation radical polymerization (photo-RDRP) in organic and aqueous phases, we report a synthetic approach to enzyme-responsive and pro-apoptotic peptide brush polymers. Thermolysin-responsive peptide-based polymeric amphiphiles assembled into spherical micellar nanoparticles that undergo a morphology transition to worm-like micelles upon enzyme-triggered cleavage of coronal peptide sidechains. Moreover, pro-apoptotic polypeptide brushes show enhanced cell uptake over individual peptide chains of the same sequence, resulting in a significant increase in cytotoxicity to cancer cells. Critically, increased grafting density of pro-apoptotic peptides on brush polymers correlates with increased uptake efficiency and concurrently, cytotoxicity. The mild synthetic conditions afforded by photo-RDRP, make it possible to access well-defined peptide-based polymer bioconjugate structures with tunable bioactivity.

| S-EPMC7299178 | biostudies-literature

Synthesis of controlled, high-molecular weight poly(l-glutamic acid) brush polymers.

Project description:We report the synthesis and characterization of high-molecular weight poly(l-glutamic acid) based brush polymers. Utilizing a combination of ring-opening metathesis polymerization of norbornene based monomers and ring-opening polymerization of ?-benzyl-l-glutamate N-carboxyanhydride, high-molecular weight ?-benzyl protected poly(l-glutamic acid) brush polymers are synthesized. Controlled and complete deprotection of the benzyl groups using trimethylsilyl iodide resulted in poly(l-glutamic acid) based brush polymers with molecular weights up to 3.6 MDa, which may potentially be used to prepare size-controlled unimolecular polymeric nanomedicine for drug delivery applications. Camptothecin brush poly(l-glutamic acid) conjugates were prepared and their stability, drug release kinetics, and in vitro toxicity were studied.

| S-EPMC6716790 | biostudies-literature

One-pot synthesis of brush-like polymers via integrated ring-opening metathesis polymerization and polymerization of amino acid N-carboxyanhydrides.

Project description:We report here the integration of ring-opening metathesis polymerization (ROMP) and ring-opening polymerization of the amino acid N-carboxyanhydride (NCA) to allow facile synthesis of brush-like polymers containing polypeptide as the brush side chains. ROMP of N-trimethylsilyl norbornenes rendered the preparation of poly(norbornene)s bearing pendant N-TMS groups. With no need to purify the resulting polymers, such macromolecular initiators could subsequently initiate controlled NCA polymerizations. Brush-like poly(norbornene)s with grafted polypeptides or block copolypeptides were readily obtained with controlled molecular weights and narrow molecular weight distributions. Because numerous ROMP and NCA monomers are widely available, this novel polymerization technique will allow easy access to numerous brush-like hybrid macromolecules with unprecedented properties and broad applications.

| S-EPMC3222154 | biostudies-literature

Reversible Speed Regulation of Self-Propelled Janus Micromotors via Thermoresponsive Bottle-Brush Polymers.

Project description:This work reports a reversible braking system for micromotors that can be controlled by small temperature changes (?5?°C). To achieve this, gated-mesoporous organosilica microparticles are internally loaded with metal catalysts (to form the motor) and the exterior (partially) grafted with thermosensitive bottle-brush polyphosphazenes to form Janus particles. When placed in an aqueous solution of H2 O2 (the fuel), rapid forward propulsion of the motors ensues due to decomposition of the fuel. Conformational changes of the polymers at defined temperatures regulate the bubble formation rate and thus act as brakes with considerable deceleration/acceleration observed. As the components can be easily varied, this represents a versatile, modular platform for the exogenous velocity control of micromotors.

| S-EPMC7898474 | biostudies-literature

Precision Anisotropic Brush Polymers by Sequence Controlled Chemistry.

Project description:The programming of nanomaterials at molecular length-scales to control architecture and function represents a pinnacle in soft materials synthesis. Although elusive in synthetic materials, Nature has evolutionarily refined macromolecular synthesis with perfect atomic resolution across three-dimensional space that serves specific functions. We show that biomolecules, specifically proteins, provide an intrinsic macromolecular backbone for the construction of anisotropic brush polymers with monodisperse lengths via grafting-from strategy. Using human serum albumin as a model, its sequence was exploited to chemically transform a single cysteine, such that the expression of said functionality is asymmetrically placed along the backbone of the eventual brush polymer. This positional monofunctionalization strategy was connected with biotin-streptavidin interactions to demonstrate the capabilities for site-specific self-assembly to create higher ordered architectures. Supported by systematic experimental and computational studies, we envisioned that this macromolecular platform provides unique avenues and perspectives in macromolecular design for both nanoscience and biomedicine.

| S-EPMC6978811 | biostudies-literature

Tension Amplification in Tethered Layers of Bottle-Brush Polymers.

Project description:Molecular dynamics simulations of a coarse-grained bead-spring model have been used to study the effects of molecular crowding on the accumulation of tension in the backbone of bottle-brush polymers tethered to a flat substrate. The number of bottle-brushes per unit surface area, ?, as well as the lengths of the bottle-brush backbones Nbb (50 ? Nbb ? 200) and side chains Nsc (50 ? Nsc ? 200) were varied to determine how the dimensions and degree of crowding of bottle-brushes give rise to bond tension amplification along the backbone, especially near the substrate. From these simulations, we have identified three separate regimes of tension. For low ?, the tension is due solely to intramolecular interactions and is dominated by the side chain repulsion that governs the lateral brush dimensions. With increasing ?, the interactions between bottle-brush polymers induce compression of the side chains, transmitting increasing tension to the backbone. For large ?, intermolecular side chain repulsion increases, forcing side chain extension and reorientation in the direction normal to the surface and transmitting considerable tension to the backbone.

| S-EPMC5040463 | biostudies-literature

GAP Peptide Synthesis via Design of New GAP Protecting Group: An Fmoc/tBu Synthesis of Thymopentin Free from Polymers, Chromatography and Recrystallization.

Project description:A novel method for Fmoc/tBu solution-phase peptide synthesis and the development of a new benzyl-type GAP protecting group is reported. This new GAP protecting group is utilized in place of a polymer support, facilitating C?N Fmoc peptide synthesis without chromatography, recrystallization, or polymer supports. The GAP group can be added and removed in high yield, and was used to synthesize over 1 gram of the immunostimulant, thymopentin, in high overall yield (83%) and purity (99%).

| S-EPMC5486986 | biostudies-literature

Drug-loaded, bivalent-bottle-brush polymers by graft-through ROMP.

Project description:Graft-through ring-opening metathesis polymerization (ROMP) using ruthenium N-heterocyclic carbene catalysts has enabled the synthesis of bottle-brush polymers with unprecedented ease and control. Here we report the first bivalent-brush polymers; these materials were prepared by graft-through ROMP of drug-loaded polyethylene-glycol (PEG) based macromonomers (MMs). Anticancer drugs doxorubicin (DOX) and camptothecin (CT) were attached to a norbornene-alkyne-PEG MM via a photocleavable linker. ROMP of either or both drug-loaded MMs generated brush homo- and co-polymers with low polydispersities and defined molecular weights. Release of free DOX and CT from these materials was initiated by exposure to 365 nm light. All of the CT and DOX polymers were at least 10-fold more toxic to human cancer cells after photoinitiated drug release while a copolymer carrying both CT and DOX displayed 30-fold increased toxicity upon irradiation. Graft-through ROMP of drug-loaded macromonomers provides a general method for the systematic study of structure-function relationships for stimuli-responsive polymers in biological systems.

| S-EPMC3083120 | biostudies-literature

Aqueous lubrication and wear properties of nonionic bottle-brush polymers.

Project description:The usage of aqueous lubricants in eco-friendly bio-medical friction systems has attracted significant attention. Several bottle-brush polymers with generally ionic functional groups have been developed based on the structure of biological lubricant lubricin. However, hydrophilic nonionic brush polymers have attracted less attention, especially in terms of wear properties. We developed bottle-brush polymers (BP) using hydrophilic 2-hydroxyethyl methacrylate (HEMA), a highly biocompatible yet nonionic molecule. The lubrication properties of polymer films were analyzed in an aqueous state using a ball-on-disk, which revealed that BPHEMA showed a lower aqueous friction coefficient than linear poly(HEMA), even lower than hyaluronic acid (HA) and polyvinyl alcohol (PVA), which are widely used as lubricating polymers. Significantly, we discovered that the combination of HA, PVA, and BPHEMA is demonstrated to be essential in influencing the surface wear properties; the ratio of 1 : 2 (HA : BPHEMA) had the maximum wear resistance, despite a slight increase in the aqueous friction coefficient.

| S-EPMC9199083 | biostudies-literature

Polyoxazoline-Based Bottlebrush and Brush-Arm Star Polymers via ROMP: Syntheses and Applications as Organic Radical Contrast Agents.

Project description:The synthesis of functional poly(2-alkyl-2-oxazoline) (PAOx) copolymers with complex nanoarchitectures using a graft-through ring-opening metathesis polymerization (ROMP) approach is described. First, well-defined norbornene-terminated poly(2-ethyl-2-oxazoline) (PEtOx) macromonomers (MM) were prepared by cationic ringopening polymerization. ROMP of these MMs produced bottlebrush copolymers with PEtOx side chains. In addition, PEtOx-based branched MMs bearing a terminal alkyne group were prepared and conjugated to an azide-containing bis-spirocyclohexyl nitroxide via Cu-catalyzed azide-alkyne cycloaddition (CuAAC). ROMP of this branched MM, followed by in situ cross-linking, provided PEtOx-based brush-arm star polymers (BASPs) with nitroxide radicals localized at the core-shell interface. These PEtOx-based nitroxide-containing BASPs displayed relaxivity values on par with state-of-the-art polyethylene glycol (PEG)-based nitroxide materials, making them promising as organic radical contrast agents for metal-free magnetic resonance imaging (MRI).

| S-EPMC6615754 | biostudies-literature

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