Document Type

Dissertation

Degree

Doctor of Philosophy (PhD)

Major/Program

Chemistry

First Advisor's Name

Raphael G Raptis

First Advisor's Committee Title

Committee Chair

Second Advisor's Name

Konstantinos Kavallieratos

Second Advisor's Committee Title

Committee Member

Third Advisor's Name

John Landrum

Third Advisor's Committee Title

Committee Member

Fourth Advisor's Name

Wenzhi Li

Fourth Advisor's Committee Title

Committee Member

Fifth Advisor's Name

Alexander Mebel

Fifth Advisor's Committee Title

Committee Member

Keywords

Chemistry

Date of Defense

6-7-2018

Abstract

The urgent need to find alternative sources of energy has been recognized as a major challenge of the 21st century. Many ideas have been proposed, but harvesting the energy of the Sun has been identified by many as the most promising alternative to satisfy the world’s increasing energy demand. Among the current technologies to harness solar energy, photovoltaics and artificial photosynthesis (photocatalysis) stand out. Although very different in their strategies, both technologies entail a core principle, the generation of a charge-separated state. To this end, both methods employ electron acceptors that will receive the photo-electron; in most cases this role is played by C60 or its derivatives. Our research group has synthesized and characterized an octanuclear iron-oxo cluster with remarkable electrochemical properties which compares favorably with the reduction potentials of C60 and derivatives. This dissertation explores the use of this octanuclear cluster as electron acceptor for solar energy applications.

To assess the viability of Fe8 as an electron acceptor in photocatalysis, electron donors that could coordinate to its iron atoms via phenol groups were synthesized and characterized. These electron donors were used in efforts to make molecular dyads, but coordination was not achieved. The altenative strategy studied was the preparation of Fe8-based hybrid materials that can be casted with known polymer electron donors. Several hybrid materials were prepared and their general properties investigated. These materials exhibited the desired electrochemical traits as well as the general castable behavior of the polymer host. These hybrids are now ready to be tested in polymer solar cells.

Identifier

FIDC006828

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Chemistry Commons

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