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DISSERTATION_Xinyu Sun.pdf (6.39 MB)

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The Control and Visualization of Intermolecular Interactions in Self-Assembly: From Star-Like and Dendron-Like Ionic Hybrid Macromolecules to Biomolecules

Sun, Xinyu
http://rave.ohiolink.edu/etdc/view?acc_num=akron161980047445729

Abstract Details

2021, Doctor of Philosophy, University of Akron, Polymer Science.
In the past decades, the study of intermolecular interactions during the self-assembly in solution has been expanded from small molecules, surfactants, and block-copolymers to nanosized macroions and macroionic cluster-based hybrids. Macroions have the size of nanometer scale, well-defined molecular structures, and uniform shapes, demonstrating intriguing solution behaviors. Their self-assembly in solution can be regulated by the electrostatic interactions when moderately charged. Tethering macroions with functional (e.g., emissive, light or temperature responsive, etc.) molecules or macroions of different amphiphilicity can build up Janus macromolecules. Their intermolecular interactions can be regulated through good control of molecular geometry as well as surface chemistry, to construct various supramolecular morphologies. In addition, the included functional molecules can help visualize these interactions. In this work, giant hybrid molecules of different molecular symmetry, molecular surfaces, and functions are prepared to study the control and visualization of intermolecular interactions during self-assembly. The star-like multi-headed hybrid molecules based on polyhedral oligomeric silsesquioxane (POSS) or polyoxometalate (POM) with aggregation-induced emission (AIE) luminophores are synthesized. The change in fluorescence emission provides direct visualization of intermolecular distances in different molecular states. The dendron-like multi-headed POSS-based hybrid molecules are featured by a symmetry breaking in molecular geometry. Their crystallization into flat nanosheets and well-defined pyramidal structures induced by mixed solvents are surprisingly observed, in contrast to spherical motifs as found in bulk. The impact of molecular construction and solvent composition is therefore explored. Furthermore, to compare the role of intermolecular interactions between charged inorganic macromolecules and charged biomolecules, the self-assembly of the viral capsid protein HBV Cp149 is used as a model molecule, to tell the effect of electrostatic interaction on capsid assembly, kinetically and thermodynamically. The solution behaviors and the assemblies in the above systems are characterized by laser-light scattering (LLS), transmission electron microscopy (TEM), atomic force microscopy (AFM), fluorescence spectroscopy, etc.
Tianbo Liu (Advisor)
Toshikazu Miyoshi (Committee Chair)
Mesfin Tsige (Committee Member)
Junpeng Wang (Committee Member)
Yi Pang (Committee Member)
156 p.
Chemistry
macromolecule; macroion; hybrid; self-assembly

Recommended Citations

Citations

  • Sun, X. (2021). The Control and Visualization of Intermolecular Interactions in Self-Assembly: From Star-Like and Dendron-Like Ionic Hybrid Macromolecules to Biomolecules [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron161980047445729

    APA Style (7th edition)

  • Sun, Xinyu. The Control and Visualization of Intermolecular Interactions in Self-Assembly: From Star-Like and Dendron-Like Ionic Hybrid Macromolecules to Biomolecules. 2021. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron161980047445729.

    MLA Style (8th edition)

  • Sun, Xinyu. "The Control and Visualization of Intermolecular Interactions in Self-Assembly: From Star-Like and Dendron-Like Ionic Hybrid Macromolecules to Biomolecules." Doctoral dissertation, University of Akron, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=akron161980047445729

    Chicago Manual of Style (17th edition)

akron161980047445729
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This open access ETD is published by University of Akron and OhioLINK.