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    Mechanism of Spatial and Temporal Control in Precision Cyclic Vinyl Polymer Synthesis by Lewis Pair Polymerization

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    Name:
    Meshanism of....Angewandte Chemie Intl Edit - 2022 - Chen - Mechanism of Spatial and Temporal Control in Precision Cyclic Vinyl Polymer.pdf
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    3.855Mb
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    PDF
    Description:
    Accepted manuscript
    Embargo End Date:
    2023-02-08
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    Type
    Article
    Authors
    Chen, Eugene Y.-X.
    McGraw, Michael L.
    Reilly, Liam T.
    Clarke, Ryan W.
    Cavallo, Luigi cc
    Falivene, Laura
    KAUST Department
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2022-02-08
    Embargo End Date
    2023-02-08
    Submitted Date
    2021-11-30
    Permanent link to this record
    http://hdl.handle.net/10754/675496
    
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    Abstract
    In typical cyclic polymer synthesis via ring-closure, chain growth and cyclization events are competing with each other, thus affording cyclic polymers with uncontrolled molecular weight or ring size and high dispersity. Here we uncover a mechanism by which Lewis pair polymerization (LPP) operates on polar vinyl monomers that allows the control of where and when cyclization takes place, thereby achieving spatial and temporal control to afford precision cyclic vinyl polymers or block copolymers with predictable molecular weight and low dispersity (~1.03). A combined experimental and theoretical study demonstrates that cyclization occurs only after all monomers have been consumed (when) via conjugate addition of the propagating chain end to the specific site of the initiating chain end (where), allowing the cyclic polymer formation steps to be regulated and executed with precision in space and time.
    Citation
    Chen, McGraw, M. L., Reilly, L. T., Clarke, R. W., Cavallo, L., & Falivene, L. (2022). Mechanism of Spatial and Temporal Control in Precision Cyclic Vinyl Polymer Synthesis by Lewis Pair Polymerization. Angewandte Chemie International Edition. Portico. https://doi.org/10.1002/anie.202116303
    Sponsors
    We gratefully acknowledge support by the U.S. National Science Foundation (NSF-1904962) for the work by MLM and LTR, and the U.S. Army Research Office (W911NF1810435) for the work by RWC. We thank Dr. Roy Geiss for his expertise and assistance with acquiring TEM images.
    Publisher
    Wiley
    Journal
    Angewandte Chemie International Edition
    DOI
    10.1002/anie.202116303
    Additional Links
    https://onlinelibrary.wiley.com/doi/10.1002/anie.202116303
    ae974a485f413a2113503eed53cd6c53
    10.1002/anie.202116303
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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