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Hemeproteins Bathed in Ionic Liquids: Examining the Role of Water and Protons in Redox Behavior and Catalytic Function

Moran, John Joseph
http://rave.ohiolink.edu/etdc/view?acc_num=csu1249089802

Abstract Details

2009, Doctor of Philosophy in Clinical-Bioanalytical Chemistry, Cleveland State University, College of Science.
We investigate the changing behaviors of myoglobin and nitric oxide synthase (NOS) in the near-absence of bulk water and/or protons by using ionic liquid butyl methyl imidazolium tetrafluoroborate as a non-aqueous milieu. Through direct charge transfer and metalloprotein-mediated catalytic reduction of oxygen and nitric oxide, we shed light on diverging aspects on how the two hemeproteins face the scarcity of water and/or protons in bulk. Isotopic effect investigations using D2O further elucidates kinetic aspects of proton transfer. Finally, in the case of NOS oxygenase, pterin cofactor binding and NOS-mediated catalytic oxidation of L-arginine in ionic liquids interrogates proton and water availability as a modulating factor affecting electrochemically-driven production of nitric oxide. Overall, our results indicate that the catalytic and redox properties of NOS and other heme-proteins change in a unique way as a function of available water. The redox and catalytic behavior of each metalloprotein is rationalized in terms of its inherent structural aspects.
Mekki Bayachou, PhD (Committee Chair)
Stanley Duraj, PhD (Committee Member)
Valentin Gogonea, PhD (Committee Member)
Yan Xu, PhD (Committee Member)
Ulrich Zurcher, PhD (Committee Member)
155 p.
Biochemistry
Electrochemistry; hemeproteins; nitric oxide synthase; NOS; myoglobin; proton transfer; ionic liquids; isotopic effects

Recommended Citations

Citations

  • Moran, J. J. (2009). Hemeproteins Bathed in Ionic Liquids: Examining the Role of Water and Protons in Redox Behavior and Catalytic Function [Doctoral dissertation, Cleveland State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=csu1249089802

    APA Style (7th edition)

  • Moran, John. Hemeproteins Bathed in Ionic Liquids: Examining the Role of Water and Protons in Redox Behavior and Catalytic Function. 2009. Cleveland State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=csu1249089802.

    MLA Style (8th edition)

  • Moran, John. "Hemeproteins Bathed in Ionic Liquids: Examining the Role of Water and Protons in Redox Behavior and Catalytic Function." Doctoral dissertation, Cleveland State University, 2009. http://rave.ohiolink.edu/etdc/view?acc_num=csu1249089802

    Chicago Manual of Style (17th edition)

csu1249089802
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© 2009, all rights reserved.
This open access ETD is published by Cleveland State University and OhioLINK.