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Ab initio study of thiol aqueous phase ionization energies. Methyl mercaptan and cysteamine

Journal Article · · Journal of Physical Chemistry; (United States)
DOI:https://doi.org/10.1021/j100092a017· OSTI ID:7070030
;  [1]
  1. Oakland Univ., Rochester, MI (United States)

The ionization energies of two thiol model compounds (methyl mercaptan and cysteamine) are calculated at the ROHF/6-31G* level to aid our understanding of the mechanisms involved in DNA radioprotection. Methyl mercaptan, the thiolate anion, and its trihydrated form are fully geometry optimized. The resulting gas-phase Koopmans ionization energies are 9.68, 1.67, and 3.63 eV, respectively. The ionization energy for the solvated methylthiolate anion, CH[sub 3]S[sup [minus]](aq), calculated through the use of the SCRF model ([epsilon] = 78), the Born charge term, and a discrete hydration shell, leads to a Koopmans value of 5.6 eV. This result is in good agreement with the corrected vertical solution-phase ionization energy calculated by using the same model (5.4 eV) and with experiment (5.7 [+-] 0.2 eV). The gas-phase ionization energy of cysteamine, its cation, zwitterion, and the pentahydrated form of the latter are reported. We find the Koopmans ionization energy of the anti-configuration of the zwitterion to be ca. 6.0 eV. 53 refs., 6 figs., 2 tabs.

DOE Contract Number:
FG02-86ER60455
OSTI ID:
7070030
Journal Information:
Journal of Physical Chemistry; (United States), Journal Name: Journal of Physical Chemistry; (United States) Vol. 98:41; ISSN JPCHAX; ISSN 0022-3654
Country of Publication:
United States
Language:
English