Responsive single-chain polymer nanoparticles with host–guest features

Song, Cunfeng; Li, Longyu; Dai, Lizong; Thayumanavan, S.

doi:10.1039/c5py00600g

Cited by 53 publications

(51 citation statements)

References 43 publications

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“…So far, several types of strategies to mediate the single chain collapse to form SCNPs have been explored, [16][17][18][19][20][21][22] ranging from hydrogen bonding, 23-27, 10, 28-31 covalent bonding, [32][33][34][35][36] to dynamic covalent bonding. [37][38][39][40] All these recent advances have provided versatile approaches to induce the folding of a single polymer chain. However, the limitation of most of these approaches is the lack of control regarding the polymer sequence and, therefore, lacking precision of the foldable moieties.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Sequence-Controlled Multiblock Single Chain Nanoparticles by a Stepwise Folding–Chain Extension–Folding Process

et al. 2016

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Copyright and reuse:The Warwick Research Archive Portal (WRAP) makes this work by researchers of the University of Warwick available open access under the following conditions. Copyright © and all moral rights to the version of the paper presented here belong to the individual author(s) and/or other copyright owners. To the extent reasonable and practicable the material made available in WRAP has been checked for eligibility before being made available.Copies of full items can be used for personal research or study, educational, or not-for profit purposes without prior permission or charge. Provided that the authors, title and full bibliographic details are credited, a hyperlink and/or URL is given for the original metadata page and the content is not changed in any way. Publisher's statement:"This document is the Accepted Manuscript version of a Published Work that appeared in final form in Macromolecules copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work http://pubs.acs.org/page/policy/articlesonrequest/index.html ." A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP URL above for details on accessing the published version and note that access may require a subscription. ABSTRACTThe specific activity of proteins can be traced back to their highly defined tertiary structure, which is a result of a perfectly controlled intra-chain folding process. In the herein presented work the folding of different distinct domains within a single macromolecule is demonstrated. RAFT polymerization was used to produce multi-block copolymers, which are decorated with pendant hydroxyl groups in foldable sections, separated by non-functional spacer blocks in between. OH-bearing blocks were folded using an isocyanate cross linker prior to chain extension to form single chain nanoparticles (SCNP). After addition of a spacer block and a further OH decorated block, folding was repeated to generate individual SCNP within a polymer chain. Control experiments were performed indicating the absence of inter block cross linking. SCNP were found to be condensed by a combination of covalent and supra molecular (hydrogen bonds) linkage. The approach was used to create a highly complex penta-block copolymer having three individually folded subdomains with an overall dispersity of 1.21. The successful formation of SCNP was confirmed by size exclusion chromatography (SEC), nuclear magnetic resonance (NMR), differential scanning calorimetry (DSC) and atomic force microscopy (AFM).

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Section: Introductionmentioning

confidence: 99%

Synthesis of Sequence-Controlled Multiblock Single Chain Nanoparticles by a Stepwise Folding–Chain Extension–Folding Process

et al. 2016

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“…Rev. XXXX, XXX, XXX−XXX encapsulating hydrophobic guest molecules and release them in response to a redox stimulus 206. Thus, a random copolymer poly((HEMA) x -co-(PDSEMA) y ) (M n = 76.9 kDa, PDI = 1.24) was synthesized by RAFT polymerization of 2-hydroxyethyl methacrylate (HEMA) and pyridyl disulfide ethyl methacrylate (PDSEMA).…”

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confidence: 99%

Intramolecular Cross-Linking Methodologies for the Synthesis of Polymer Nanoparticles

et al. 2015

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“…Compared to the linear polymer, the chain mobility of SCNPs will decrease, resulting in an increased glass transition temperature (T g ) value. 31,[75][76][77] The T g value of the AB 1 SCNP increased significantly to 172.4 °C from the initial value of 147.9 °C for linear polymer AB 1 (Table 1, Figure S7, the value at around 90 °C was identified as measurement artefact, see Figure S8 and the ESI for the detailed explanation). On the other hand, the linear copolymer AB 2 contains a larger fraction of GLA in the second block (B 2 ) which leads to a broader glass transition process and a decreased T g (95.8 °C, Table 1, Figure S9) compared to AB 1 (147.9 °C).…”

Section: Resultsmentioning

confidence: 98%

Self-assembly and disassembly of stimuli responsive tadpole-like single chain nanoparticles using a switchable hydrophilic/hydrophobic boronic acid cross-linker

et al. 2017

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Sébastien. (2017) Self-assembly and dis-assembly of stimuli responsive tadpole-like single chain nanoparticles using a switchable hydrophilic/hydrophobic boronic acid cross-linker. Polymer Chemistry, 28 (8). pp. 4079-4087. Permanent WRAP URL:http://wrap.warwick.ac.uk/93551 Copyright and reuse:The Warwick Research Archive Portal (WRAP) makes this work by researchers of the University of Warwick available open access under the following conditions. Copyright © and all moral rights to the version of the paper presented here belong to the individual author(s) and/or other copyright owners. To the extent reasonable and practicable the material made available in WRAP has been checked for eligibility before being made available.Copies of full items can be used for personal research or study, educational, or not-for-profit purposes without prior permission or charge. Provided that the authors, title and full bibliographic details are credited, a hyperlink and/or URL is given for the original metadata page and the content is not changed in any way. A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP URL' above for details on accessing the published version and note that access may require a subscription. Living systems are driven by molecular machines that are composed of folded polypeptide chains, which are assembled together to form a multimeric complex. Although replicating this type of systems is a long standing goal in polymer science, the complexity of the structures imposes is synthetically very challenging, and generating synthetic polymers to mimic the process of these assemblies appears to be a more appealing approach. To this end, we report a linear polymer programmable for stepwise folding and assembly to higher-order structures. To achieve this, a diblock copolymer composed of 4-Acryloylmorpholine and glycerol acrylate was synthesised with high precision via reversible addition fragmentation chain transfer polymerisation (Ð < 1.22). Both intramolecular folding and intermolecular assembly was driven by pH responsive cross-linker, benzene-1,4-diboronic acid. The resulting intramolecular folded single chain nanoparticles were well defined (Ð < 1.16) and successfully assembled into a multimeric structure (Dh = 245 nm) at neutral pH with no chain entanglement. The assembled multimer was observed with a spherical morphology as confirmed by TEM and AFM. These structures were capable of unfolding and disassembling either at low pH or in the presence of sugar. This work offers new perspective for the generation of adaptive smart materials.

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Responsive single-chain polymer nanoparticles with host–guest features

Abstract: We report a facile approach to form ultra-fine single-chain polymer nanoparticles (SCPNs)viadisulfide-based intrachain crosslinking of single polymer chains of a random copolymer poly(HEMA-co-PDSEMA).

Cited by 53 publications

References 43 publications

Synthesis of Sequence-Controlled Multiblock Single Chain Nanoparticles by a Stepwise Folding–Chain Extension–Folding Process

Synthesis of Sequence-Controlled Multiblock Single Chain Nanoparticles by a Stepwise Folding–Chain Extension–Folding Process

Intramolecular Cross-Linking Methodologies for the Synthesis of Polymer Nanoparticles

Self-assembly and disassembly of stimuli responsive tadpole-like single chain nanoparticles using a switchable hydrophilic/hydrophobic boronic acid cross-linker

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