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    Molecular rheology of branched polymers: Decoding and exploring the role of architectural dispersity through a synergy of anionic synthesis, interaction chromatography, rheometry and modeling

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    Type
    Article
    Authors
    Van Ruymbeke, Evelyne
    Lee, Heecheong
    Chang, Taihyun
    Nikopoulou, Anastasia
    Hadjichristidis, Nikos cc
    Snijkers, Frank
    Vlassopoulos, Dimitris
    KAUST Department
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Polymer Synthesis Laboratory
    Date
    2014
    Permanent link to this record
    http://hdl.handle.net/10754/563208
    
    Metadata
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    Abstract
    An emerging challenge in polymer physics is the quantitative understanding of the influence of a macromolecular architecture (i.e., branching) on the rheological response of entangled complex polymers. Recent investigations of the rheology of well-defined architecturally complex polymers have determined the composition in the molecular structure and identified the role of side-products in the measured samples. The combination of different characterization techniques, experimental and/or theoretical, represents the current state-of-the-art. Here we review this interdisciplinary approach to molecular rheology of complex polymers, and show the importance of confronting these different tools for ensuring an accurate characterization of a given polymeric sample. We use statistical tools in order to relate the information available from the synthesis protocols of a sample and its experimental molar mass distribution (typically obtained from size exclusion chromatography), and hence obtain precise information about its structural composition, i.e. enhance the existing sensitivity limit. We critically discuss the use of linear rheology as a reliable quantitative characterization tool, along with the recently developed temperature gradient interaction chromatography. The latter, which has emerged as an indispensable characterization tool for branched architectures, offers unprecedented sensitivity in detecting the presence of different molecular structures in a sample. Combining these techniques is imperative in order to quantify the molecular composition of a polymer and its consequences on the macroscopic properties. We validate this approach by means of a new model asymmetric comb polymer which was synthesized anionically. It was thoroughly characterized and its rheology was carefully analyzed. The main result is that the rheological signal reveals fine molecular details, which must be taken into account to fully elucidate the viscoelastic response of entangled branched polymers. It is important to appreciate that, even optimal model systems, i.e., those synthesized with high-vacuum anionic methods, need thorough characterization via a combination of techniques. Besides helping to improve synthetic techniques, this methodology will be significant in fine-tuning mesoscopic tube-based models and addressing outstanding issues such as the quantitative description of the constraint release mechanism. © 2014 the Partner Organisations.
    Citation
    Van Ruymbeke, E., Lee, H., Chang, T., Nikopoulou, A., Hadjichristidis, N., Snijkers, F., & Vlassopoulos, D. (2014). Molecular rheology of branched polymers: decoding and exploring the role of architectural dispersity through a synergy of anionic synthesis, interaction chromatography, rheometry and modeling. Soft Matter, 10(27), 4762. doi:10.1039/c4sm00105b
    Sponsors
    We are very grateful to Paul Kim for his precious help with the samples characterization. We acknowledge partial support from EU (ITN DYNACOP, grant 214627; FP7 Infrastructure ESMI, GA 262348). EVR thanks the Fonds National de la Recherche Scientique (FNRS) for financial support. TC acknowledges the supports from NRF (2012R1A2A2A01015148).
    Publisher
    Royal Society of Chemistry (RSC)
    Journal
    Soft Matter
    DOI
    10.1039/c4sm00105b
    ae974a485f413a2113503eed53cd6c53
    10.1039/c4sm00105b
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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