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Author ORCID Identifier

https://orcid.org/0000-0003-0590-0545

AccessType

Open Access Dissertation

Document Type

dissertation

Degree Name

Doctor of Philosophy (PhD)

Degree Program

Chemistry

Year Degree Awarded

2022

Month Degree Awarded

September

First Advisor

Vincent M. Rotello

Subject Categories

Amino Acids, Peptides, and Proteins | Bacteriology | Biomedical and Dental Materials | Organic Chemicals | Other Analytical, Diagnostic and Therapeutic Techniques and Equipment | Other Chemicals and Drugs | Therapeutics

Abstract

Biomaterials are widely applied for the diagnosis and treatment of numerous diseases. In addition to fulfilling specific biological functions, biomaterials must also be non-toxic, biocompatible, and sterilizable to be regarded as safe-for-use. Polymers are excellent candidates for fabricating functional biomaterials due to their wide availability and varied properties and may be natural or synthetic. Polymer precursors are fabricated into coatings, foams, scaffolds, gels, composites, and nanomaterials for several biomedical applications. This dissertation focuses on two types of polymeric biomaterials – protein-based materials and synthetic polymeric nanoparticles. Proteins are biopolymers that naturally occur with a variety of structural and functional properties. However, the fabrication of protein-based materials is challenging due to their aqueous and mechanical instability. In this work we highlighted the development of an additive-free, thermal treatment approach that relies on heat-curing protein films in fluorous media (fluorous-curing). In doing so, we are able to minimize protein denaturation and retain surface properties. Charged protein films were utilized to prepare antimicrobial coatings and size-sorting devices. We also demonstrated the utility of fluorous-curing to enhance mechanical and enzymatic stability of collagen films with minimal denaturation. In the latter part of this work, we utilized ultrasound treatment to enhance the activity of biomaterials. Ultrasound is gaining interest as a tool used in combination with biomaterials for applications such as enhanced penetration of therapeutics into tissue, regulating drug release through ultrasound-responsive scaffolds, and sonodynamic therapy. However, these developments are limited and delayed due to the lack of effective in vitro models that prevent uncontrolled cell lysis during ultrasound. We developed 2D and 3D cell cultures for ultrasound treatment using collagen-based materials. We hypothesized that collagen would act as a support for the cells and absorb the energy exerted by ultrasound, thereby protecting the cells. We then utilized ultrasound in combination with antimicrobial polymeric nanomaterials for the synergistic eradication of bacterial biofilms. Antimicrobial polymer nanoparticles are an alternative to traditional antibiotics that prevent development of drug resistance. However, longer incubation durations and higher concentrations are required to allow for penetration into the bacterial biofilms which results in toxicity to mammalian cells. Ultrasound enhances the penetration of these nanoparticles into the biofilm EPS thereby reducing the incubation time and enhancing antimicrobial activity, with minimal toxicity to mammalian cells. Overall, this dissertation discusses significant developments in polymeric materials for varied potential applications as diagnostic sensors, antimicrobial materials, wound-healing, tissue engineering, and drug delivery applications.

DOI

https://doi.org/10.7275/30584014

Creative Commons License

Creative Commons Attribution 4.0 License
This work is licensed under a Creative Commons Attribution 4.0 License.

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