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Document Type

Open Access Dissertation

Degree Name

Doctor of Philosophy (PhD)

Degree Program

Chemistry

Year Degree Awarded

Fall 2014

First Advisor

Prof. Vincent M. Rotello

Subject Categories

Biochemistry | Materials Chemistry | Organic Chemistry | Physical Chemistry

Abstract

A major goal in material science is achieving a desired function using structures fabricated with designed building blocks. Advanced synthetic and self-assembly techniques allow various nanomaterials to become promising building blocks, providing the control of the interaction between building blocks. The unique properties of nanomaterials can be transferred to structured systems. Among nanomaterials, inorganic nanoparticles such as gold nanoparticles (AuNPs), magnetic particles, and quantum dots (QDs) provide useful physical properties stemming from their inorganic core, large surface areas, and oriented surface functionalities. My research has focused on fabricating functional systems using gold nanoparticles (AuNPs), manipulating the interaction between AuNPs, bio-entities, and small molecules. To construct complicated three-dimensional structures and embed functions, emulsion templates for the fabrication of the capsule structures and various supramolecular chemistry between AuNPs or AuNP and enzyme were employed. My research consisted of 2 approaches: first, through both the design of the monolayer at the molecular level and the emulsion template, (1) enzyme-immobilized microparticles having high immobilization efficiency and reusability were fabricated; (2) correlations between the mechanical properties of the AuNP monolayer film and the binding affinities between nanoparticle components were investigated; and (3) stable 100 nm sized nanoparticle-dendrimer hybrid capsules as a drug delivery carrier were fabricated and evaluated in vivo. Second, by encapsulating various hydrophobic catalysts in the hydrophobic pockets of the monolayer of water-soluble AuNPs, (4) water-soluble nanoreactors were developed. By incorporating host-guest elements on the surface of water-soluble nanoreactors, (5) artificial enzymes capable of catalyzing bio-orthogonal chemical reactions inside living cells which can be regulated by the addition of host or guest molecules were fabricated. As can be seen, engineering of the AuNP surface at the molecular level opens new avenues for the fabrication of numerous functional materials.

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