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Title: Contributions from inner and outer shell electron energies to reaction heats for C/sub 1/, C/sub 2/, and C/sub 3/ hydrocarbons

Journal Article · · Int. J. Quant. Chem.; (United States)
 [1]; ;
  1. Univ. of Pennsylvania, Philadelphia

The expectation energy values E/sub k/, V/sub ee/, V/sub nn/, V/sub en/, and E/sub T/ have been calculated for H/sub 2/ and the C/sub 1/, C/sub 2/, and C/sub 3/ hydrocarbons using a (9,5) basis set and the experimental geometries. Treating the theoretical reaction heat, ..delta..E/sub T/, as the resultant of the nuclear repulsion term, ..delta..V/sub nn/, and the net electron energy term, ..delta..E/sub elec/ = ..delta..E/sub k/ + ..delta..V/sub ee/ + ..delta..V/sub en/, the contribution of inner and outer shell electron energies to ..delta..E/sub elec/, and hence to ..delta..E/sub T/, has been calculated for a large number of hydrocarbon reactions by evaluating the Coulson--Neilson energies eta/sub i/, where eta/sub i/ = E/sub elec/. For the vast majority of reactions, 67/84, the change in inner shell electron energy, (..delta sigma..eta/sub i/)/sub inner/, accounts for more than 10% of ..delta..E/sub elec/, in many cases being as high as 20-35%. Furthermore, in addition to these cases in which the change in inner shell electron energy serves to augment (significantly) the change in outer shell electron energy, there are other cases in which the change in inner shell electron energy either exceeds in magnitude the change in outer shell energy, or is even opposite in sign, indicative of inner and outer shell electrons acting contrariwise. Inner shell electron energies contribute to the reaction heats because they are structure dependent, like the more familiar orbital energies epsilon, but the dependence is of a different kind.

OSTI ID:
6092017
Journal Information:
Int. J. Quant. Chem.; (United States), Vol. 15:4
Country of Publication:
United States
Language:
English