Date of Graduation

12-2021

Document Type

Dissertation

Degree Name

Doctor of Philosophy in Chemistry (PhD)

Degree Level

Graduate

Department

Chemistry & Biochemistry

Advisor/Mentor

Sakon, Joshua

Committee Member

Kim, Jin-Woo

Second Committee Member

Fan, Chenguang

Third Committee Member

Wang, Feng

Fourth Committee Member

Allison, Neil T.

Keywords

Nanomedicine; Nanotechnology; Photodynamic therapy

Abstract

Developing methodologies to control the architecture of nanoparticles (NPs) at the atomic level prevents their inhomogeneity and leads to a variety of expected functions. Rationally designed nanoparticles can either be programmed or crystallized structures into pre-determined structures achieving tunable particle pore size and physiochemistry. In this dissertation, two broad classes of multifunctional nanoparticles are developed, metal-organic frameworks and DNA-NP aggregates.

Metal-organic frameworks are a novel class of highly porous crystalline materials built from organic linkers and metal cluster-based secondary building units. However, applications in bioremediation have not been developed very well especially in applications regarding drug delivery systems (DDS). The first studies in this dissertation aimed to develop a new MOF DDS that can be applied to photodynamic therapy (PDT) and achieved the difficult targeted treatment of triple-negative breast cancer (TNBC) cells, tumor-associated macrophages (TAM), and pancreatic cancer cells. The successful development of DDS for MOFs with maltotrionate potassium was the first step in the studies. Then the development of a new stable and effective PDT ligand in the oxidative environment and a bioconjugation method was further developed. Finally, the MOF platform was completed for the dual therapy MOF, which can be used for PDT and chemotherapy treatments, showed a more significant effect to kill cancer cells than with only PDT.

Another study was the development and analysis of programable architecture with DNA and multiple kinds of metal NPs. The well-defined base-pairing interactions of DNA allow it to behave as a programmable bond on a nanoparticle scaffold. Binary metal NPs have been increasingly receiving significant attention due to the surface plasmonic response (SPR) and multifunctional abilities. However, the technique of dual-metal NP synthesis and studies in the quantum field have not been established. As the second study, binary and multiple-metal NP structure in programmed spatial organization using DNA-based technology was developed.

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