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Free Energy Landscapes for S-H Bonds in (Cp2Mo2S4)-Mo-star Complexes

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/ja8093179· OSTI ID:952894

Extensive thermochemical data have been determined for a series of complexes derived from Cp*Mo(μ S)2(μ SMe)(μ SH)MoCp* and Cp*Mo(μ S)2(μ SH)2MoCp*. These data include electrochemical potentials, pKa values, homolytic solution bond dissociation free energies (SBDFEs), and hydride donor abilities in acetonitrile. Thermochemical data ranged from +0.6 to -2.0 V vs FeCp2+/o for electrochemical potentials, 5 to 31 for pKa values, 43 to 68 kcal/mol for homolytic SBDFEs, and 44 to 84 kcal/mol for hydride donor abilities. The observed values for these thermodynamic parameters are comparable to those of many transition metal hydrides, which is consistent with the many parallels in the chemistry of these two classes of compounds. The wealth of thermochemical data are presented in free energy landscapes as a useful approach to visualizing and understanding the relative stabilities of all of the species under specified conditions. This work was supported by the U.S. Department of Energy's (DOE) Office of Basic Energy Sciences, Chemical Sciences program. The Pacific Northwest National Laboratory is operated by Battelle for DOE.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
952894
Report Number(s):
PNNL-SA--63520; KC0302010
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 14 Vol. 131; ISSN JACSAT; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English