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Stabilized Photocatalytic Hydrogen Generation using a Molecular Ru(II) Sensitizer, a Molecular Cobalt Catalyst and an Amine Derivative as an Electron Donor

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2013, Master of Science (MS), Bowling Green State University, Chemistry.
Transient absorption and photoluminescence studies were carried out on a homogeneous photocatalytic proton reduction composition using tris(4,7-diphenyl-1,10-phenanthroline)-ruthenium(II) ([Ru(dpp)3]2+) as photosensitizer, a cobalt glyoxime ([CoIII(dmgH)2pyCl]) water reduction catalyst and N,N-dimethyl-p-toluidine (DMT) as the sacrificial donor in water:acetonitrile solvent mixtures. Dynamic photoluminescence studies revealed that DMT reductively quenched the excited state of *Ru(dpp)32+ with a bimolecular rate constant of k q = 4.9 × 109 M-1 s-1. Similarly time resolved spectroscopy was used to determine the rate of electron transfer from the reduced sensitizer to the [CoIII(dmgH)2pyCl] to be k Co = 2.4 ×109 M-1 s-1. H2 production photocatalysis independently monitored using pressure, GC, and mass spectroscopy illustrated that the composition yields high TONs with respect to sensitizer TON ~ 10,000 (H2/Ru) while deuteration studies showed that 90% of the reduced protons comes from water. The rationale behind the large photostability imparted by the use of the DMT reductive quencher was postulated to be its ability to form stable dimer in solution following electron donation.
Felix Castellano (Advisor)
Mikhail Zamkov (Committee Member)
Ksenija Glusac (Committee Member)
51 p.

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Citations

  • Olaiya, B. S. (2013). Stabilized Photocatalytic Hydrogen Generation using a Molecular Ru(II) Sensitizer, a Molecular Cobalt Catalyst and an Amine Derivative as an Electron Donor [Master's thesis, Bowling Green State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1371066177

    APA Style (7th edition)

  • Olaiya, Babatunde. Stabilized Photocatalytic Hydrogen Generation using a Molecular Ru(II) Sensitizer, a Molecular Cobalt Catalyst and an Amine Derivative as an Electron Donor. 2013. Bowling Green State University, Master's thesis. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1371066177.

    MLA Style (8th edition)

  • Olaiya, Babatunde. "Stabilized Photocatalytic Hydrogen Generation using a Molecular Ru(II) Sensitizer, a Molecular Cobalt Catalyst and an Amine Derivative as an Electron Donor." Master's thesis, Bowling Green State University, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=bgsu1371066177

    Chicago Manual of Style (17th edition)