Date of Award

Spring 2019

Document Type

Open Access Dissertation

Department

Chemistry and Biochemistry

First Advisor

Chuanbing Tang

Abstract

In this dissertation, the development of sustainable polymers and antimicrobial biomaterials from multicyclic natural products is illustrated. In Chapter 1, an overall background and recent development of sustainable polymers from natural product-based renewable biomass, antimicrobial biomaterials, and polymerization methods are introduced. Afterward, the primary research objectives of my doctoral research work are illustrated.

In chapter 2, designing block copolymer architectures toward tough bioplastics from renewable natural rosin was described. One of the most abundant natural biomasses is resin acids, however, most of the polymers derived from resin acids are brittle because of their bulky hydrophenanthrene pendant group. To overcome the brittleness, rosin containing pentablock and triblock copolymers were synthesized through living sequential ring opening metathesis polymerization (ROMP). Their thermal and mechanical properties were investigated. The phase behaviors were also studied for the microphase-separated pentablock and triblock copolymers using small angle x-ray scattering (SAXS) and atomic force microscopy.

A new class of true facial amphiphilic cationic antimicrobial polymers was illustrated in chapter 3. Facially amphiphilic antimicrobial polymers were prepared from multicyclic natural products (e.g. bile acids) via reversible-addition fragmentation chain transfer (RAFT) polymerization. The antimicrobial activity against a range of bacteria and hemolysis activity with mammalian cells is investigated. In addition, the antimicrobial mechanistic aspects of facially amphiphilic polymers were also illustrated. Chapter 4 is explained about the facial amphiphilicity-induced self-assembly (FAISA) of multicyclic natural product-based cationic copolymers. The detail self-assembly behavior of copolymers with different polyethylene glycol was explained. The self-assembly of these copolymers to form antimicrobial nanoparticles was investigated in Chapter 5. The nanoaggregates exhibited strong antimicrobial activity against Gram-negative bacteria and showed minimal toxicity against mammalian cell.

Finally, a summary and future directions of this dissertation research are provided in chapter 6. In future work, some suggestions about future directions involving renewable biomass for sustainable development are given.

Available for download on Monday, May 11, 2020

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