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Kinetics of the reaction of CCl sub 3 + Br sub 2 and thermochemistry of CCl sub 3 radical and cation

Journal Article · · Journal of Physical Chemistry; (United States)
DOI:https://doi.org/10.1021/j100164a043· OSTI ID:5890244
;  [1]; ; ;  [2]
  1. National Inst. of Standards and Technology, Gaithersburg, MD (United States)
  2. Catholic Univ. of America, Washington, DC (United States)

The rate constant of the CCl{sub 3} + Br{sub 2} {yields} CCl{sub 3}Br + Br reaction was determined as a function of temperature between 300 and 532 K and fit to an Arrhenius expression: k{sub 1} (L mol{sup {minus}1} s{sup {minus}1}) = (1.8 {plus minus} 0.4) {times} 10{sup 8} exp(({minus}1.43 {plus minus} 0.29) kcal mol{sup {minus}1}/RT). The reaction was studied in a tubular flow reactor by using laser photolysis to produce the CCl{sub 3} reactant and photoionization mass spectrometry to monitor CCl{sub 3} in time-resolved experiments. Previously published kinetic data were reevaluated to obtain k{sup {minus}1}, the rate constant for the reverse reaction, and recent spectroscopic data were used to calculate accurate entropies and heat capacities. The values of k{sub {minus}1}, k{sub 1}, and these calculated thermodynamic properties were used in a third law determination to obtain {Delta}H{degree}{sub f,298.15}(CCl{sub 3}) = 17.0 {plus minus} 0.6 kcal mol{sup {minus}1} and {Delta}H{degree}{sub f,0}(CCl{sub 3}) = 16.7 {plus minus} 0.6 kcal mol{sup {minus}1}. This information was combined with spectroscopic data on CCl{sub 3}{sup +} to obtain {Delta}H{degree}{sub f,298.15}(CCl{sub 3}{sup +}) = 205.2 {plus minus} 0.6 kcal mol{sup {minus}1} and {Delta}H{degree}{sub f,0}(CCl{sub 3}{sup +}) = 203.7 {plus minus} 0.6 kcal mol{sup {minus}1}. Bond energies of several relevant compounds and tables of thermodynamic functions for CCl{sub 3} and CCl{sub 3}{sup +} are presented. An improved heat of formation for the CCl{sub 3}O{sub 2} radical, {Delta}H{degree}{sub f,298.15}(CCl{sub 3}O{sub 2}) = 2.7 {plus minus} 1.1 kcal mol{sup {minus}1}, is also reported.

OSTI ID:
5890244
Journal Information:
Journal of Physical Chemistry; (United States), Journal Name: Journal of Physical Chemistry; (United States) Vol. 95:11; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English

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