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Spatiotemporal Formation and Growth Kinetics of Polyelectrolyte Complex Micelles with Millisecond Resolution

机译:用毫秒分辨率的聚电解质复合胶束的时空形成和生长动力学

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摘要

We have directly observed the in situ self-assembly kinetics of polyelectrolyte complex (PEC) micelles by synchrotron time-resolved small-angle X-ray scattering, equipped with a stopped-flow device that provides millisecond temporal resolution. A synthesized neutral-charged diblock polycation and homopolyanion that we have previously investigated as a model charge-matched, core–shell micelle system were selected for this work. The initial micellization of the oppositely charged polyelectrolytes was completed within the dead time of mixing of 100 ms, followed by micelle growth and equilibration up to several seconds. By combining the structural evolution of the radius of gyration (R _(g)) with complementary molecular dynamics simulations, we show how the self-assemblies evolve incrementally in size over time through a two-step kinetic process: first, oppositely charged polyelectrolyte chains pair to form nascent aggregates that immediately assemble into spherical micelles, and second, these PEC micelles grow into larger micellar entities. This work has determined one possible kinetic pathway for the initial formation of PEC micelles, which provides useful physical insights for increasing fundamental understanding self-assembly dynamics, driven by polyelectrolyte complexation that occurs on ultrafast time scales.
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著录项

  • 来源
    《ACS Macro Letters》 |2020年第11期|共7页
  • 作者单位

    Pritzker School of Molecular Engineering University of Chicago;

    Pritzker School of Molecular Engineering University of Chicago;

    Pritzker School of Molecular Engineering University of Chicago;

    Pritzker School of Molecular Engineering University of Chicago;

    Pritzker School of Molecular Engineering University of Chicago;

    Pritzker School of Molecular Engineering University of Chicago;

    Pritzker School of Molecular Engineering University of Chicago;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 有机化学;
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