Date of Award

Spring 2017

Project Type

Thesis

Program or Major

Chemistry

Degree Name

Master of Science

First Advisor

Samuel Pazicni

Second Advisor

Christine Caputo

Third Advisor

Sterling Tomellini

Abstract

Carbon dioxide has become an ever growing problem facing life on Earth due to the theory that the increase in CO2 levels has been the leading cause of global warming and could initiate significant climate change. Most of the CO2 produced by humans comes from the burning of fossil fuels for energy. Because of this, the development of a clean alternative fuel is a primary concern. Dihydrogen is looked at as a possible alternative because it has already demonstrated the ability to produce energy in fuel cells and could conceivably replace fossil fuels in every aspect of its use. The main problem facing dihydrogen as an alternative fuel is hydrogen production. The purpose of this research is to design a novel dihydrogen catalyst modeled after the active site of [FeFe]-Hydrogenase. Past research has shown that this enzyme can very efficiently catalyze the forward reaction of protons and electrons to form dihydrogen. Diiron cluster mimics were synthesized with a spectrum of clickable terminal alkene bridgeheads with chain lengths ranging from 3 to 6 carbons for the purpose of attaching them to amorphous carbon surfaces. In addition, the effect of steric hindrance on the diiron cluster bridgehead is being investigated. This was done by creating diiron cluster mimics with the alkene chain attached to the carbon atom of the bridgehead as opposed to the nitrogen. It is thought that reducing the steric hindrance around the nitrogen will increase the rate of proton shuttling to the iron metal center thereby increasing the turn over frequency. The synthetic routes to create these mimics were explored and the products were characterized using 1H NMR, 13C NMR, and IR spectroscopies. This research provides the initial steps in designing a dihydrogen catalyst that can efficiently generate hydrogen fuel.

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