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1D vs. 2D shape selectivity in the crystallization-driven self-assembly of polylactide block copolymers

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Inam, Maria, Cambridge, Graeme, Pitto-Barry, Anaïs, Laker, Zachary P. L., Wilson, Neil R., Mathers, Robert T., Dove, Andrew P. and O'Reilly, Rachel K. (2017) 1D vs. 2D shape selectivity in the crystallization-driven self-assembly of polylactide block copolymers. Chemical Science, 8 (6). pp. 4223-4230. doi:10.1039/C7SC00641A ISSN 2041-6520.

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Official URL: http://dx.doi.org/10.1039/C7SC00641A

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Abstract

2D materials such as graphene, LAPONITE® clays or molybdenum disulfide nanosheets are of extremely high interest to the materials community as a result of their high surface area and controllable surface properties. While several methods to access 2D inorganic materials are known, the investigation of 2D organic nanomaterials is less well developed on account of the lack of ready synthetic accessibility. Crystallization-driven self-assembly (CDSA) has become a powerful method to access a wide range of complex but precisely-defined nanostructures. The preparation of 2D structures, however, particularly those aimed towards biomedical applications, is limited, with few offering biocompatible and biodegradable characteristics as well as control over self-assembly in two dimensions. Herein, in contrast to conventional self-assembly rules, we show that the solubility of polylactide (PLLA)-based amphiphiles in alcohols results in unprecedented shape selectivity based on unimer solubility. We use log Poct analysis to drive solvent selection for the formation of large uniform 2D diamond-shaped platelets, up to several microns in size, using long, soluble coronal blocks. By contrast, less soluble PLLA-containing block copolymers yield cylindrical micelles and mixed morphologies. The methods developed in this work provide a simple and consistently reproducible protocol for the preparation of well-defined 2D organic nanomaterials, whose size and morphology are expected to facilitate potential applications in drug delivery, tissue engineering and in nanocomposites.

Item Type: Journal Article
Subjects: Q Science > QD Chemistry
Divisions: Faculty of Science, Engineering and Medicine > Science > Chemistry
Faculty of Science, Engineering and Medicine > Science > Physics
Library of Congress Subject Headings (LCSH): Block copolymers, Self-assembly (Chemistry), Graphene, Nanostructured materials
Journal or Publication Title: Chemical Science
Publisher: Royal Society of Chemistry
ISSN: 2041-6520
Official Date: 2017
Dates:
DateEvent
2017Published
24 April 2017Available
24 March 2017Accepted
Volume: 8
Number: 6
Page Range: pp. 4223-4230
DOI: 10.1039/C7SC00641A
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Open Access (Creative Commons)
Date of first compliant deposit: 19 October 2017
Date of first compliant Open Access: 20 October 2017
Funder: University of Warwick, Materials GRP (Frim), Engineering and Physical Sciences Research Council (EPSRC), Royal Society (Great Britain), European Research Council (ERC)
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
UNSPECIFIEDUniversity of Warwickhttp://dx.doi.org/10.13039/501100000741
UNSPECIFIEDMaterials GRPUNSPECIFIED
UNSPECIFIED[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
UNSPECIFIED[RS] Royal Societyhttp://dx.doi.org/10.13039/501100000288
UNSPECIFIEDH2020 European Research Councilhttp://dx.doi.org/10.13039/100010663

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