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Stefan Ilic_Master Thesis.pdf (1.53 MB)

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Utilizing NAD+/NADH Analogs for the Solar Fuel Forming Reductions

Ilic, Stefan
http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1499262103862098

Abstract Details

2017, Master of Science (MS), Bowling Green State University, Chemistry.
Recent scientific efforts aim to blend light harvesting with the fuel forming catalysis, as a novel method to store the energy captured from the Sun. Our approach is to construct an efficient photoelectrochemical cell using earth-abundant materials. The proposed system contains bioinspired metal-free hydride donors suitable for fuel forming reductions and a p-type semiconductor that serve as a light harvester and source of electrons. In this thesis, we investigate fundamental steps that determine the efficiency of the photoelectrochemical cell: photoreduction of NAD+ dyes by p-GaP semiconductor and the hydricity of NADH analogs. First, thermodynamics for photo-induced electron transfer from p-GaP to NAD+ dyes are evaluated using steady-state UV/Vis absorption and cyclic voltammetry experiments. Photoelectrochemical measurement conducted on p-GaP electrodes immersed in aqueous electrolytes and dye show sensitization for only two dyes. Pump-probe measurements reveal that the “inefficient” dyes have short-lived excited states, inhibiting the successful charge transfer into p-GaP surface. This work provides an insight on timescales of hole-injection rates during dye-sensitization processes. Furthermore, we evaluate the hydricity for model NADH analogs using experimental methods and calculations. The obtained hydricity values display a strong dependence on structural and electronic properties of the model compounds. When compared with metal-based analogs, NADH analogs show similar hydride donor ability. However, the high reduction potentials for metal-free hydride donors hinder their applicability in the catalysis. This work offers a reasonable explanation on why NADH analogs have not been utilized in fuel forming catalysis and provides the answers how to overcome these limitations.
Ksenija D. Glusac, Prof. Dr. (Advisor)
R. Marshall Wilson, Prof. Dr. (Committee Member)
94 p.
Chemistry
CO2 reduction; molecular catalysts; light harvesting; solar fuel; artificial photosynthesis; hydricity; metal free

Recommended Citations

Citations

  • Ilic, S. (2017). Utilizing NAD+/NADH Analogs for the Solar Fuel Forming Reductions [Master's thesis, Bowling Green State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1499262103862098

    APA Style (7th edition)

  • Ilic, Stefan. Utilizing NAD+/NADH Analogs for the Solar Fuel Forming Reductions. 2017. Bowling Green State University, Master's thesis. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1499262103862098.

    MLA Style (8th edition)

  • Ilic, Stefan. "Utilizing NAD+/NADH Analogs for the Solar Fuel Forming Reductions." Master's thesis, Bowling Green State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1499262103862098

    Chicago Manual of Style (17th edition)

bgsu1499262103862098
357
© 2017, all rights reserved.
This open access ETD is published by Bowling Green State University and OhioLINK.