Efficient Utilization of Solar Energy in Dye-Sensitized Solar Cells and in the Photocatalytic Reduction of Carbon Dioxide

One of the most important questions humanity will face in the next 100 years is going to be "What will happen when oil runs out?" This dissertation describes efforts to utilize solar energy to improve renewable energy technology in two ways: First, through the improvement of dye sensitized solar cells by theimprovement of D-π-A dye subunits, the development of practical sensitizers, and progress towards stable, tunable redox shuttles. A novel indolizine donor subunit was synthesized that was shown to be the strongest reported donor. Dyes made from this novel donor and devices using the Γ-/I 3- reached up to 5.4% efficiency. This donor was then systematically improved by the addition of non-conjugated substituents, which acted as good surface blocking groups and thus facilitated high performance during device testing. Dyes made using this donor and devices using the Γ-/I 3- redox shuttle reached up to 6.7% efficiency. Second, this thesis describes efforts to close the carbon cycle through utilization of solar energy in CO2 reduction. The described efforts regard the improvement of known catalysts through increased stability and performance, and of the use of a simulated solar spectrum to improve the practicality of photocatalyticCO2 reduction. By the substitution of a pyridyl chelating group for an N-Heterocyclic Carbene (NHC) ligand, the synthesized complexes were more stable while still absorbing visible light. The synthesized complexes operated as photocatalysts with or without a photosensitizer, making this the fourth reported series ofnon-sensitized photocatalysts for CO2 reduction.

Name thesis:degree_name

Ph.D. in Chemistry

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemistry and Biochemistry

Year dc:date.available

2015

Author dc:creator

• Huckaba, Aron Joel

Contributors dc:contributor

• Jared H. Delcamp
• John M. Rimoldi
• Amala Dass

• CO2 Reduction
• Dye-Sensitized Solar Cell
• Indolizine
• Photocatalysis
• Photosensitized
• Re-NHC complex
• Organic Chemistry

Repository record dc:identifier

https://egrove.olemiss.edu/etd/1369

OAI identifier oai:identifier

oai:egrove.olemiss.edu:etd-2368