Polymerization-Induced Self-Assembly of Galactose-Functionalized Biocompatible Diblock Copolymers for Intracellular Delivery

Ladmiral, Vincent; Semsarilar, Mona; Cantón, Irene; Armes, Steven P.

doi:10.1021/ja407033x

Cited by 187 publications

(194 citation statements)

References 75 publications

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“…While such post-polymerization modification undoubtedly adds both cost and complexity to PISA syntheses, this approach may yet be cost-effective for certain high-value biomedical applications suggested for block copolymer nanoparticles. 123,133,150−152 Nevertheless, the relatively high cost, intrinsic color, and malodorous nature of the sulfur-based RAFT CTAs may well prove to be detrimental to the development of next-generation paints and coatings or even relatively “high-value” cosmetics additives. On the other hand, it is perhaps worth emphasizing that a series of RAFT-synthesized star copolymers have already been commercialized by the Lubrizol Corporation as high-performance thickeners for automotive engine oils.…”

Section: Potential Applications and Opportunities For Pisa Formulationsmentioning

confidence: 99%

A Critical Appraisal of RAFT-Mediated Polymerization-Induced Self-Assembly

2016

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Recently, polymerization-induced self-assembly (PISA) has become widely recognized as a robust and efficient route to produce block copolymer nanoparticles of controlled size, morphology, and surface chemistry. Several reviews of this field have been published since 2012, but a substantial number of new papers have been published in the last three years. In this Perspective, we provide a critical appraisal of the various advantages offered by this approach, while also pointing out some of its current drawbacks. Promising future research directions as well as remaining technical challenges and unresolved problems are briefly highlighted.

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Section: Potential Applications and Opportunities For Pisa Formulationsmentioning

confidence: 99%

A Critical Appraisal of RAFT-Mediated Polymerization-Induced Self-Assembly

2016

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“…Recently, polymerizationinduced self-assembly (PISA) has been developed by various research groups. [14][15][16][17][18][19][20] This highly attractive approach enables bespoke organic nanoparticles to be prepared directly during the copolymer synthesis at much higher concentrations. The most versatile PISA formulation is based on dispersion polymerization, which can be performed in either water, 21 polar solvents such as alcohols, [22][23][24][25][26][27][28][29][30][31] or non-polar solvents such as n-alkanes.…”

Section: -10mentioning

confidence: 99%

Semi-crystalline diblock copolymer nano-objects prepared via RAFT alcoholic dispersion polymerization of stearyl methacrylate

et al. 2015

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nano-objects prepared via RAFT alcoholic dispersion polymerization of stearyl methacrylate. Polymer Chemistry, 6 (10). pp. 1751 -1757 . ISSN 1759 https://doi.org/10.1039/c4py01664e eprints@whiterose.ac.uk https://eprints.whiterose.ac.uk/ Reuse Unless indicated otherwise, fulltext items are protected by copyright with all rights reserved. The copyright exception in section 29 of the Copyright, Designs and Patents Act 1988 allows the making of a single copy solely for the purpose of non-commercial research or private study within the limits of fair dealing. The publisher or other rights-holder may allow further reproduction and re-use of this version -refer to the White Rose Research Online record for this item. Where records identify the publisher as the copyright holder, users can verify any specific terms of use on the publisher's website. TakedownIf you consider content in White Rose Research Online to be in breach of UK law, please notify us by emailing eprints@whiterose.ac.uk including the URL of the record and the reason for the withdrawal request. Semi-Crystalline Diblock Copolymer Nano-Objects Prepared via RAFT Alcoholic Dispersion Polymerization of Stearyl MethacrylateMona Semsarilar, Nicholas J. W. Penfold, Elizabeth R. Jones and Steven P. Armes* Abstract. The RAFT dispersion polymerization of stearyl methacrylate (SMA) is conducted in ethanol at 70°C using a poly(2-(dimethylamino)ethyl methacrylate) [PDMA] chain transfer agent. The growing PSMA block becomes insoluble in ethanol, which leads to polymerization-induced self-assembly (PISA) and hence produces a range of copolymer morphologies depending on the precise PDMA y -PSMA x formulation. More specifically, pure phases corresponding to either spherical nanoparticles, worm-like nanoparticles or vesicles can be prepared as judged by transmission electron microscopy. However, the worm phase space is relatively narrow, so construction of a detailed phase diagram is required for reproducible syntheses of this morphology. Interdigitation of the stearyl (C 18 ) side-groups leads to a semi-crystalline PSMA core block and the effect of systematically varying the mean degree of polymerization of both the PDMA and PSMA blocks on the T m and T c is investigated using differential scanning calorimetry. Finally, it is demonstrated that these cationic nanoparticles can be employed as colloidal templates for the in situ deposition of silica from aqueous solution.

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“…[1][2][3][4][5][6][7][8] Among these, cylindrical structures have exhibited extensive potential in various unique applications, such as additives for polymer resin toughening 9,10 and templates for electronic materials.…”

Section: Introductionmentioning

confidence: 99%

Understanding the CDSA of poly(lactide) containing triblock copolymers

et al. 2017

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Crystallisation-driven self-assembly (CDSA) has become an extremely valuable technique in the preparation of well-defined nanostructures using diblock copolymers. The use of triblock copolymers is considerably less well-known on account of more complex syntheses and assembly methods despite the functional advantages provided by a third block. Herein, we show the simple preparation of well-defined tuneable 1D and 2D structures based on poly(lactide) triblock copolymers of different block ratios synthesised by ring-opening polymerisation (ROP) and reversible addition-fragmentation chain transfer (RAFT) polymerisation, where a phase diagram based on a novel unimer solubility approach is proposed. Using a series of poly(L-lactide)-b-poly(N,N-dimethylacrylamide) (PLLA-b-PDMA) diblock copolymers and PDMA-b-PLLA-b-PDMA triblock copolymers with different core/corona ratios, single solvent CDSA processes revealed that comparatively hydrophilic polymers were liable to achieve 2D platelets, while the less hydrophilic counterparts yield 'transition state' wide cylinders and pure 1D cylinders. The length of crystalline core block is also shown to play an important role in fixed corona/core ratio systems, where a longer core block is prone to form cylindrical structures due to a lack of overall solubility, whereas a shorter block forms platelets. Importantly, this approach reveals contrary results to conventional theories, which state that longer solvophilic blocks relative to the core-forming block should favour more curved core/corona interfaces. Our morphological transitions are shown in both di-and tri-block copolymer systems, showing the generalisation of these assembly methods towards promising methodologies for the rational design of PLLA-based nanocarriers in the biomedical realm.

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Polymerization-Induced Self-Assembly of Galactose-Functionalized Biocompatible Diblock Copolymers for Intracellular Delivery

Cited by 187 publications

References 75 publications

A Critical Appraisal of RAFT-Mediated Polymerization-Induced Self-Assembly

A Critical Appraisal of RAFT-Mediated Polymerization-Induced Self-Assembly

Semi-crystalline diblock copolymer nano-objects prepared via RAFT alcoholic dispersion polymerization of stearyl methacrylate

Understanding the CDSA of poly(lactide) containing triblock copolymers

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