Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Deuterium isotope effects on the carbon-13 chemical shifts of carbocations

Thesis/Dissertation ·
OSTI ID:6036331

The deuterium isotope effect on the carbon-13 NMR spectrum of several carbocations and neutral molecules have been examined. The carbon-13 resonance of the cationic carbon atom in the heavy isotopomer of the carbocations was found to be shifted upfield, to be unaffected, or to be shifted downfield, upon ..beta..-deuteration from the corresponding carbon in the nondeuterated compound. These effects ranged from -2.5 ppm to +1.6 ppm and were found to be consistent with previous work of Servis and Shue. The two bond chemical shift isotope effects determined for 2-methyl-2-norbornyl cation and for 2-(3,5-bis-(trifluoromethyl)-phenyl)-2-norbornyl cation provide evidence for partial delocalization of positive charge away from C2 into a three-center two-electron bond. The deuterium isotope effects determined for the 2-(p-fluorophenyl)-2-norbornyl cation and the 2-phenyl-2-norbornyl cation provide evidence about the stereochemical dependence of the two bond chemical shift isotope effect. The effect of exo C3 deuterium substitution on the C2-resonance in the carbon-13 NMR spectrum of the 2-(p-fluorophenyl)-2-norbornyl cation and the 2-phenyl-2-norbornyl cation is small and positive while the effect of endo C3 deuterium substitution is small and negative. This is the first case reported in which stereochemically distinct isotope effects at the same carbon are of opposite sign. The two bond chemical shift isotope effects determined for 2,3-dimethyl-2-butene bromonium ion and for 2,3-dimethyl-2-butene mercurinium ion permit the elucidation of the electronic structure of these cations.

Research Organization:
University of Southern California, Los Angeles (USA)
OSTI ID:
6036331
Country of Publication:
United States
Language:
English