Carnegie Mellon University
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Functional Inorganic Nanoparticle/Polymer Hybrid Materials: Synthesis, Characterization and Self-assembly Behavior

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posted on 2020-04-01, 19:43 authored by Zongyu WangZongyu Wang
This thesis describes the preparation of ZnO/polymer hybrid and polymer grafted silica particle brushes and explores their properties and applications.
The introductory chapter (Chapter 1) reviews the history and development of ZnO/polymer hybrid synthesis. The synthetic approaches include “grafting from”, “grafting onto” and “polymer templates” methods.
Chapters 2-6 cover the synthesis of polymer capped ZnO nanocrystals by the “ligand exchange” method and their applications. In Chapter 2, the preparation of PSAN capped ZnO nanocrystals from octylamine capped ZnO nanoparticles by the “ligand exchange” method is discussed. The morphologies of the product were tuned by the ratios of ZnO nanoparticle/polymer ligands in the reaction mixture. Chapter 3 shows a detailed characterization of the polymer ligands/surfactants capped ZnO nanocrystals by MALDI-TOF mass spectrum. ZnO-based materials exhibit excellent optical, thermal, photocatalytic and electrical properties. Chapters 4-6 discuss three important properties and applications of the obtained nano-ZnO/polymer composites, which include high refractive index glass fillers, photocatalyst, and high stability ZnO/carbon supercapacitors.
The second part of the thesis (Chapters 7-13) focuses on the study of polymer grafted silica particle brushes. By using surface-initiated atom transfer polymerization, polymer chains were grown from the surfaces of nanoparticles. With covalent bonding, comparing to ZnO/polymer hybrids synthesized by the “ligand exchange” method, the chemistry to synthesize polymer grafted silica particle brush system is more robust and well established. Chapters 7-8 illustrate the synthesis of SiO2-g-PMMA/PS particle brushes by low ppm catalyst ATRP. The effect of initiator and catalyst concentrations on the polymerization was investigated. Chapter 9 describes the synthesis of ultra-high molecular weight SiO2-g-PMMA particle brushes and Chapter 10 presents the mechanical properties of SiO2-g-PMMA/PS particle brushes with different grafting densities. The preparation and phase separation study of SiO2-g-PMMA-b-PS block copolymer particle brushes is included in Chapter 11. Their unique self-assembly behavior is explored. At last, the study of gradient copolymer grafted silica particle brushes are covered in Chapter 12-13. Chapter 12 emphasizes the synthesis of SiO2-g-PBA-grad-PMMA particle brushes by semi-batch copolymerization method, and Chapter 13 highlights their mechanical properties and compositionally sensitive self-healing features.
Two published works with minor relevance to this thesis (polymerization-induced self-assembly of acrylonitrile and organoSiO2-g-PMMA particle brushes synthesis) are included as appendices.

History

Date

2019-12-20

Degree Type

  • Dissertation

Department

  • Chemistry

Degree Name

  • Doctor of Philosophy (PhD)

Advisor(s)

Krzysztof Matyjaszewski Michael Bockstaller

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