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Cellulose nanocrystals with tethered polymer chains: chemically patchy versus uniform decoration

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10.1021/acsmacrolett.7b00383
 
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hdl:2117/336254

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Zoppe, Justin OrazioMés informacióMés informació
Dupire, Alix
Lachat, Theo
Lemal, Philipp
Rodriguez Lorenzo, Laura
Petri-Fink, Alke
Weder, Christoph
Klok, Harm-Anton
Document typeArticle
Defense date2017-09-19
Rights accessOpen Access
Attribution-NonCommercial-NoDerivs 3.0 Spain
Except where otherwise noted, content on this work is licensed under a Creative Commons license : Attribution-NonCommercial-NoDerivs 3.0 Spain
Abstract
The site-specific surface modification of colloidal substrates, yielding “patchy” nanoparticles, is a rapidly expanding area of research as a result of the new complex structural hierarchies that are becoming accessible to chemists and materials scientists through colloidal self-assembly. The inherent directionality of cellulose chains, which feature a nonreducing and a reducing end, within individual cellulose nanocrystals (CNCs) renders them an interesting experimental platform for the synthesis of asymmetric nanorods with end-tethered polymer chains. Here, we present water-tolerant reaction pathways toward patchy and uniformly modified CNC hybrids based on atom transfer radical polymerization (ATRP) and initiators that were linked to the CNCs with carbodiimide-mediated coupling and Fischer esterification, respectively. Various monomers, including N-isopropylacrylamide (NIPAM), [2-(methacryloyloxy)ethyl]trimethylammonium chloride (METAC), and sodium 4-vinylbenzenesulfonate (4-SS), were polymerized from both types of initiator-modified CNCs, yielding chemically patchy and uniform CNC hybrids, via surface-initiated ATRP (SI-ATRP). Interestingly, the stereochemistry of tethered PNIPAM was affected by the precise location of ATRP initiating sites, as evidenced by 1H NMR and circular dichroism (CD) spectroscopy. This effect may be related to the inherent right-handed chirality of CNCs. CNC/PMETAC hybrids were labeled with gold nanoparticles (AuNPs) in order to visualize the precise location of polymer tethers via cryo-electron microscopy. In some instances, the AuNPs were indeed concentrated at the end groups of the patchy CNC hybrids.
CitationZoppe, J. [et al.]. Cellulose nanocrystals with tethered polymer chains: chemically patchy versus uniform decoration. "ACS Macro Letters", 19 Setembre 2017, vol. 6, núm. 9, p. 892-897. 
URIhttp://hdl.handle.net/2117/336254
DOI10.1021/acsmacrolett.7b00383
ISSN2161-1653
Publisher versionhttps://pubs.acs.org/doi/10.1021/acsmacrolett.7b00383
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