Temperature‐Dependent Gelation Behaviour of Double Responsive P2VP‐b‐PEO‐b‐P(GME‐co‐EGE) Triblock Terpolymers: A SANS Study

Karg, Matthias; Reinicke, Stefan; Lapp, Alain; Hellweg, Thomas; Schmalz, Holger

doi:10.1002/masy.201000142

Cited by 3 publications

(4 citation statements)

References 57 publications

(40 reference statements)

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“…Thermoresponsive triblock terpolymers have gained a lot of interest because they have fascinating self-assembly behaviour and form micelles with complex structures like core-shell micelles. [33][34][35][36][37][38][39][40][41][42][43][44][45][46][47][48][49][50] Furthermore at the right concentration and temperature they form multicompartment injectable gels. 36,39,[43][44][45][46][47][48][49][50] The gel formation has been shown to be affected by many parameters like the MW, composition, block length, chemistry of the polymer as well as the polymer architecture.…”

Section: Introductionmentioning

confidence: 99%

Multicompartment thermoresponsive gels: does the length of the hydrophobic side group matter?

Ward

Georgiou

2013

Polym. Chem.

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Multicompartment thermoresponsive gels are novel materials with fascinating self-assembly and interesting applications. The aim of this study was to investigate for the first time the effect of the length of the alkyl side group of a hydrophobic monomer on the thermoresponsive and self-assembly behaviour of terpolymers. Specifically twelve well-defined terpolymers based on the hydrophilic monomers 2-(dimethylamino)ethyl methacrylate (DMAEMA) and poly(ethylene glycol) methyl ether methacrylate (PEGMA), and on the hydrophobic monomer ethyl-, n-butyl or n-hexyl methacrylate (EtMA, BuMA or HMA) of varying architectures (ABC, ACB, BAC and statistical) were synthesised using Group Transfer Polymerisation. The A, B and C blocks were based on PEGMA, the alkyl containing methacrylate monomer, and DMAEMA, respectively. The molecular weights (MWs) and compositions of the polymers were kept the same. The polymers and their precursors were characterised in terms of their MWs, MW distributions and compositions. Aqueous solutions of the polymers were studied by turbidimetry, hydrogen ion titration, light scattering and rheology to determine their cloud points, pK a s, hydrodynamic diameters and thermoresponsive behaviour and investigate the effect of the architecture and the hydrophobic alkyl side group of the terpolymers. It was found that the pK a s and the T g s were mostly affected by the hydrophobicity of the side groups and not by the architecture, while the cloud points and the sol-gel transition of the polymers were affected by both the length of the alkyl side group and the polymer architecture. Interestingly the sharpest sol-gel transitions and stable multicompartment hydrogels were observed for the ABC triblock copolymers with the short alkyl-side groups even though the sol-gel transition occurred at higher temperatures.

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Section: Introductionmentioning

confidence: 99%

Multicompartment thermoresponsive gels: does the length of the hydrophobic side group matter?

Ward

Georgiou

2013

Polym. Chem.

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“…Schmalz and co-workers investigated the temperature-dependent gelation behavior of double responsive P2VP 62 - b -PEG 452 - b -P(GME 36 - co -EGE 36 ) terpolymers, while the 2VP units introduced pH responsivity. Hydrogel formation was observed, if one of the end blocks was insoluble and further showed a temperature-induced gel–sol–gel transition. , These block copolymers were part of a review by Manners and co-workers in 2012, presenting functional block copolymers utilized as nanostructured materials . In 2014, Kamata et al demonstrated the synthesis of “nonswellable” hydrogels without mechanical hysteresis, capitalizing on star-shaped four-arm P(GME- co -EGE) copolymers .…”

Section: Bioapplication Of Thermoresponsive P(scage)smentioning

confidence: 99%

“…In 2011, Schmalz and co-workers synthesized ABC block copolymers by the use of phosphazene bases, incorporating a copolymer block consisting of GME and EGE. 75 In contrast to classic AROP of epoxides where the oxyanion and lithium form strong ionic aggregates, 16 catalysis by phosphazene bases enables polymerization despite the presence of lithium counterions. During the reaction, the phosphazene base forms a [Li-tBuP 4 ] + complex while suppressing ion pair association of the lithium alkoxide.…”

Section: ■ Polymerization Of Scagesmentioning

confidence: 99%

“…Hydrogel formation was observed, if one of the end blocks was insoluble and further showed a temperature-induced gel−sol−gel transition. 41,75 These block copolymers were part of a review by Manners and co-workers in 2012, presenting functional block copolymers utilized as nanostructured materials. 128 In 2014, Kamata et al demonstrated the synthesis of "nonswellable" hydrogels without mechanical hysteresis, capitalizing on starshaped four-arm copolymers.…”

Section: ■ Bioapplication Of Thermoresponsive P(scage)smentioning

confidence: 99%

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Polyethers Based on Short-Chain Alkyl Glycidyl Ethers: Thermoresponsive and Highly Biocompatible Materials

Matthes

Frey

2022

Biomacromolecules

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The polymerization of short-chain alkyl glycidyl ethers (SCAGEs) enables the synthesis of biocompatible polyethers with finely tunable hydrophilicity. Aliphatic polyethers, most prominently poly(ethylene glycol) (PEG), are utilized in manifold biomedical applications due to their excellent biocompatibility and aqueous solubility. By incorporation of short hydrophobic side-chains at linear polyglycerol, control of aqueous solubility and the respective lower critical solution temperature (LCST) in aqueous solution is feasible. Concurrently, the chemically inert character in analogy to PEG is maintained, as no further functional groups are introduced at the polyether structure. Adjustment of the hydrophilicity and the thermoresponsive behavior of the resulting poly(glycidyl ether)s in a broad temperature range is achieved either by the combination of the different SCAGEs or with PEG as a hydrophilic block. Homopolymers of methyl and ethyl glycidyl ether (PGME, PEGE) are soluble in aqueous solution at room temperature. In contrast, n-propyl glycidyl ether and iso-propyl glycidyl ether lead to hydrophobic polyethers. The use of a variety of ring-opening polymerization techniques allows for controlled polymerization, while simultaneously determining the resulting microstructures. Atactic as well as isotactic polymers are accessible by utilization of the respective racemic or enantiomerically pure monomers. Polymer architectures varying from statistical copolymers, di- and triblock structures to star-shaped architectures, in combination with PEG, have been applied in various thermoresponsive hydrogel formulations or polymeric surface coatings for cell sheet engineering. Materials responding to stimuli are of increasing importance for “smart” biomedical systems, making thermoresponsive polyethers with short-alkyl ether side chains promising candidates for future biomaterials.

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ABC block copolymer micelles driving the thermogelation: Scattering, imaging and spectroscopy

Constantinou,

Nele,

Doutch

et al. 2024

Polymer

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Temperature‐Dependent Gelation Behaviour of Double Responsive P2VP‐b‐PEO‐b‐P(GME‐co‐EGE) Triblock Terpolymers: A SANS Study

Cited by 3 publications

References 57 publications

Multicompartment thermoresponsive gels: does the length of the hydrophobic side group matter?

Multicompartment thermoresponsive gels: does the length of the hydrophobic side group matter?

Polyethers Based on Short-Chain Alkyl Glycidyl Ethers: Thermoresponsive and Highly Biocompatible Materials

ABC block copolymer micelles driving the thermogelation: Scattering, imaging and spectroscopy

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