Date of Award
1-1-2022
Document Type
Dissertation
Degree Name
Ph.D. in Chemistry
First Advisor
Jared H. Delcamp
Second Advisor
Nathan I. Hammer
Third Advisor
Jonah W. Jurss
School
University of Mississippi
Relational Format
dissertation/thesis
Abstract
Solar energy technologies, such as dye-sensitized solar cells (DSCs) and photoelectrochemical cells (PECs), rely on electron transfer reactions to convert light waves from the Sun to usable electrical energy. These electron transfers are vital to the performance of solar energy technologies. However, two main unproductive electron transfers (recombination and back electron transfer) are possible in these systems, making it vital to study and increase the efficiency of the beneficial electron transfers while hindering the possibility of unproductive pathways from occurring. Through modulation of the organic chromophore/dye used in DSCs, lower recombination rates, and back electron transfer rates are afforded. Three approaches are utilized in this work: varying the number of bulky alkyl chains, increasing the bond angle of the π-bridge spacer unit by using methyl groups, and accessing the Marcus inverted region by lowering the highest occupied molecular orbital (HOMO) using withdrawing groups on the donor of the dye. These approaches yielded various results, including a champion strong photooxidant dye, RR9, controlling recombination and producing a 1.4 V high voltage (HV) DSC device, a lowered rate of back electron transfer by 22x by dye CC10, and accessing the Marcus inverted region leading to lowered rates of recombination through the use of the energetically record-breaking HV dye, QL14.
Recommended Citation
Curiac, Christine, "Controlling Rate of Interfacial Electron Transfers via Synthetic Modulation of Organic Chromophores" (2022). Electronic Theses and Dissertations. 2672.
https://egrove.olemiss.edu/etd/2672