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Construction of Supramolecular Structures by Mimicking Metallurgy

Liu, Tong
http://rave.ohiolink.edu/etdc/view?acc_num=akron160370390740064

Abstract Details

2020, Doctor of Philosophy, University of Akron, Polymer Science.
Structures of materials are the key to its properties. Recently complicated metal alloy structures have been found in broad area of soft matters, providing as steppingstones to create novel soft matter materials with novel properties. For soft matters, formation of such metal alloy phases generally adopts a hierarchical two-step process, during which the firstly assembles into spherical motifs, each spherical motif consists of tens of molecules and then the spherical motifs further served as `mesoatoms’ and close packed themselves to afford different metal alloy structures. It is now widely believed that size heterogeneity of mesoatoms is the key factor in achieve different structures. Thus, control the formation of these supramolecular mesoatoms are critically important in achieving diverse structures and yet remain a challenge. Currently, construction of these mesoatoms is generally by a `trial and error’ method in soft matter. This is because the size heterogeneity is a result of the delicate balance between enthalpic and entropic term. Such complicate factors make the prediction of nanostructure become extremely complicated. Intricate tuning is needed to balance the multiple enthalpic and entropic interactions in order to yield mesoatoms with specific size and size heterogeneity. Inspired by classic metal alloy metallurgy, a self-sorting approach to achieve the size heterogeneity of mesoatoms was discovered. This approach solved the key step in constructing diverse nanostructures. Herein, I report the bulk self-sorting mediated self-assembly of binary nano-sized giant molecules blends to overcome the critical symmetry breaking problem in hierarchical self-assembly. Such strategy enables structure construction in a predictable and controllable way. We discovered such self-sorting in condensed matter to mimic metallurgy. Surprisingly, classic intermetallic solid solution behavior in soft matter was discovered for the first time. The scarcely observed Frank-Kasper C14 and C15 phases were found dominantly and proved to be thermodynamically stable. Furthermore, these structures were fully visualized in both real space and reciprocal space. Diverse ordered spherical supramolecular structures can be achieved by variating composition or component. By carefully analyzed the data, such mechanism was fully confirmed by experimental data. Furthermore, the detail mechanism was fully studied and provide a great generality in access complex structures. A library of giant molecules was established, and their binary blending combination result was studied. A few surprising results was confirmed by both SAXS and TEM experiment. This approach discovered the great similarity which can serve as a bridge between the classic alloy metallurgy and the soft matter nanostructure assembling, it not only has the potentials to enable the discovery of currently hidden phases, but also can provide sufficiently new insights for nanostructure formation in soft matter.
Stephen Cheng (Advisor)
Tianbo Liu (Committee Chair)
Toshikazu Miyoshi (Committee Member)
Yu Zhu (Committee Member)
Yi Pang (Committee Member)
330 p.
Materials Science; Polymers

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Citations

  • Liu, T. (2020). Construction of Supramolecular Structures by Mimicking Metallurgy [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron160370390740064

    APA Style (7th edition)

  • Liu, Tong. Construction of Supramolecular Structures by Mimicking Metallurgy. 2020. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron160370390740064.

    MLA Style (8th edition)

  • Liu, Tong. "Construction of Supramolecular Structures by Mimicking Metallurgy." Doctoral dissertation, University of Akron, 2020. http://rave.ohiolink.edu/etdc/view?acc_num=akron160370390740064

    Chicago Manual of Style (17th edition)

akron160370390740064
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This open access ETD is published by University of Akron and OhioLINK.