Synthesis of Biocompatible, Stimuli-Responsive, Physical Gels Based on ABA Triblock Copolymers

ABA triblock copolymers [A = 2-(diisopropylamino)ethyl methacrylate), DPA or 2-(diethylamino)ethyl methacrylate), DEA; B = 2-methacryloyloxyethyl phosphorylcholine, MPC] prepared using atom transfer radical polymerization dissolve in acidic solution but form biocompatible free-standing gels at aroun...

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Veröffentlicht in:Biomacromolecules 2003-07, Vol.4 (4), p.864-868
Hauptverfasser: Ma, Yinghua, Tang, Yiqing, Billingham, Norman C, Armes, Steven P, Lewis, Andrew L
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container_end_page 868
container_issue 4
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container_title Biomacromolecules
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creator Ma, Yinghua
Tang, Yiqing
Billingham, Norman C
Armes, Steven P
Lewis, Andrew L
description ABA triblock copolymers [A = 2-(diisopropylamino)ethyl methacrylate), DPA or 2-(diethylamino)ethyl methacrylate), DEA; B = 2-methacryloyloxyethyl phosphorylcholine, MPC] prepared using atom transfer radical polymerization dissolve in acidic solution but form biocompatible free-standing gels at around neutral pH in moderately concentrated aqueous solution (above approximately 10 w/v % copolymer). Proton NMR studies indicate that physical gelation occurs because the deprotonated outer DPA (or DEA) blocks become hydrophobic, which leads to attractive interactions between the chains:  addition of acid leads to immediate dissolution of the micellar gel. Release studies using dipyridamole as a model hydrophobic drug indicate that sustained release profiles can be obtained from these gels under physiologically relevant conditions. More concentrated DPA−MPC−DPA gels give slower release profiles, as expected. At lower pH, fast, triggered release can also be achieved, because gel dissolution occurs under these conditions. Furthermore, the nature of the outer block also plays a role; the more hydrophobic DPA−MPC−DPA triblock gels are formed at lower copolymer concentrations and retain the drug longer than the DEA−MPC−DEA triblock gels.
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Proton NMR studies indicate that physical gelation occurs because the deprotonated outer DPA (or DEA) blocks become hydrophobic, which leads to attractive interactions between the chains:  addition of acid leads to immediate dissolution of the micellar gel. Release studies using dipyridamole as a model hydrophobic drug indicate that sustained release profiles can be obtained from these gels under physiologically relevant conditions. More concentrated DPA−MPC−DPA gels give slower release profiles, as expected. At lower pH, fast, triggered release can also be achieved, because gel dissolution occurs under these conditions. 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subjects Applied sciences
Biocompatible Materials - chemical synthesis
Biocompatible Materials - chemistry
Exact sciences and technology
Gels - chemical synthesis
Gels - chemistry
Methacrylates - chemistry
Micelles
Molecular Structure
Organic polymers
Phosphorylcholine - analogs & derivatives
Phosphorylcholine - chemistry
Physicochemistry of polymers
Polymers - chemical synthesis
Polymers - chemistry
Polymers with particular properties
Preparation, kinetics, thermodynamics, mechanism and catalysts
title Synthesis of Biocompatible, Stimuli-Responsive, Physical Gels Based on ABA Triblock Copolymers
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