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Gas-phase bond strength and atomic connectivity studies of the unsymmetrical two-center three-electron ion, [Et{sub 2}S...SMe{sub 2}]{sup +}

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/ja960455h· OSTI ID:374500
A computational and experimental study of the unsymmetrical 2c-3e bond in [Et{sub 2}S...SMe{sub 2}]{sup +} is presented. For the first time, MS/MS collision-induced dissociation experiments provide strong experimental support of the atomic connectivity in a gas-phase S...S 2c-3e association adduct. The strongest peak in the collision-induced dissociation spectrum corresponds to Et{sub 2}S{sup +}, consistent with the lower ionization potential of Et{sub 2}S compared to Me{sub 2}S and the proposed structure. High-pressure equilibrium mass spectrometry experiments yield a reaction enthalpy of -104 kJ/mol for the equilibrium reaction Et{sub 2}S{sup +} + Me{sub 2}S < [Et{sub 2}S...SMe{sub 2}]{sup +} at 506 K. Correcting this value to 0 K using ab initio molecular parameters results in a bond energy of 107 kJ/mol which can be compared to a calculated value of 107.9 kJ/mol at the B3LYP/6-31G(d)//B3LYP/ 6-31G(d)+ZPC level. Studies on a competing reaction, Et{sub 2} S{sup +} + Et{sub 2}S < [Et{sub 2}S...SEt{sub 2}]{sup +}, yield an experimental bond enthalpy of 119 kJ/mol at 506 K and a calculated bond energy of 121.3 kJ/mol, in excellent agreement with previously reported values. 24 refs., 9 figs., 3 tabs.
OSTI ID:
374500
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 33 Vol. 118; ISSN JACSAT; ISSN 0002-7863
Country of Publication:
United States
Language:
English