Document Type

Dissertation

Degree

Doctor of Philosophy

Major

Chemistry

Date of Defense

11-19-2020

Graduate Advisor

Keith J. Stine

Committee

Alexei V. Demchenko

Chung F. Wong

Michael R. Nichols

Abstract

Nanoporous gold (NPG) is a versatile material because of its three-dimensional nanoscale network, facile surface functionalization, biocompatibility, and potential usage in biotechnology applications. The field of glycoscience is growing in significance as the importance of glycans in human health and disease becomes more fully understood at the molecular level. NPG can be applied to several needs in the field of glycoscience. Our lab has applied NPG to applications in glycoscience including the capture and release of glycoproteins, and the detection of glycoprotein interactions by using either electrochemical methods or localized surface plasmon spectroscopy (LSPR). The capture of glycoproteins onto high surface area NPG is demonstrated using both lectin-glycan interactions and interaction between glycoproteins and NPG modified with boronic acid functional groups. Thermogravimetric analysis and use of a UV-visible HPLC detector in a flow cell containing monoliths of NPG were applied to monitor the capture of glycoprotein and its elution by the flow of free ligand. The modification of NPG by self-assembled monolayers (SAMs) with terminal boronic acid groups has been used together with LSPR to monitor the capture of glycoprotein by the induced shift in the LSPR peak wavelength. Square-wave voltammetry methods can also be applied to monitor the binding of glycoproteins to NPG modified either by SAMs with terminal boronic acid groups or by conjugated lectins.

Thiolated β-cyclodextrin modified NPG wire was used for the pH-sensitive release of doxorubicin (DOX) in a controlled manner, with an ultra-high DOX payload. Thiolated β-cyclodextrins are attractive macrocycles as they can form supramolecular inclusion complexes with doxorubicin affording the possibility of altering the controlled release behavior. Doxorubicin is one of the most potent anti-tumor drugs used in the treatment of different cancers. The binding of thiolated β-cyclodextrin with the anti-cancer drug doxorubicin has been examined with the use of spectroscopy and electrochemistry. Moreover, the prepared structure exhibited excellent properties for controlled drug release outlining the potential of a pH-sensitive drug implant or carrier for biomedical application. This delivery system could improve localized targeting of the drug as well as alter the rate of release of the doxorubicin near a tumor.

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