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Document Type

Open Access Dissertation

Degree Name

Doctor of Philosophy (PhD)

Degree Program

Chemistry

Year Degree Awarded

2017

Month Degree Awarded

September

First Advisor

Vincent M. Rotello

Subject Categories

Materials Chemistry | Medicinal-Pharmaceutical Chemistry | Organic Chemistry

Abstract

Nanoparticles (NPs) are being investigated widely for many applications including imaging, drug delivery, therapeutics, materials, and catalysis due to their unique and tunable physical and chemical properties. Among NPs, gold nanoparticles (AuNPs) have attracted great attention due to ease of synthesis and surface functionalization, inertness of the core, biocompatibility, and functional versatility. Introducing supramolecular chemistry into the nanoparticle-based platforms brings out controllable properties, dynamic self assembly processes, and adjustable performance. My research has focused on the synthesis of AuNPs bearing different surface functionalities and their host-guest interactions with synthetic small molecules or commercially available hydrophobic catalysts for delivery and therapeutic applications. My research is consisted of two main sections. First part is the regulation of the exocytosis of AuNPs using host-guest interactions and characterization of these interactions in solution using isothermal titration calorimetry and inside cells using laser desorption/ionization/matrix assisted laser desorption/ionization mass spectrometry. Second part is about encapsulating various hydrophobic transition metal catalysts into the monolayer of AuNPs. These catalyst-embedded AuNPs were used to catalyze industrially important reactions in aqueous environment. For biological applications, this system was called as ‘nanozyme’ because it was used as an enzyme mimic to perform bioorthogonal activation of profluorophores and prodrugs for imaging and therapeutic applications, respectively. Using the host-guest chemistry, intracellular catalysis was supramolecularly regulated. Lastly, different monolayer designs were engineered to increase the catalyst loading and improve catalytic efficiency.

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