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Kinetics of Cl atom reactions with C sub 2 H sub 6 , C sub 2 H sub 5 , and C sub 2 H sub 4. Rates of disproportionation and recombination of ethyl radicals

Journal Article · · Journal of the American Chemical Society; (USA)
DOI:https://doi.org/10.1021/ja00159a020· OSTI ID:6835118
;  [1]
  1. Univ. of Southern California, Los Angeles (USA)

The kinetics of Cl atom reaction with ethane at 298 K were studied with the very low pressure reactor (VLPR). In the very early stages of reaction, with (Cl) > (C{sub 2}H{sub 6}), there is a very fast and irreversible reaction (1), producing HCl + C{sub 2}H{sub 5} followed by a slightly slower reaction (2) of Cl with C{sub 2}H{sub 5} to produce HCl + C{sub 2}H{sub 4}. An extremely slow reaction (4) of Cl with C{sub 2}H{sub 4} to form HCl + C{sub 2}H{sub 3} can also be seen followed by a much faster reaction (5) of Cl with C{sub 2}H{sub 3} to form HCl + C{sub 2}H{sub 2}. After 50% Cl conversion when (Cl) < (C{sub 2}H{sub 6}), only reactions 1 and 3 (the disproportionation of C{sub 2}H{sub 5}) are important. By studying the reaction over large ranges of concentration of both Cl and C{sub 2}H{sub 6}, it is possible to obtain all rate constants except for (5) with good accuracy (cm{sup 3}/molecule {times} s {times} 10{sup 11}): k{sub 1} = 6.10 {plus minus} 0.11, k{sub 2} = 1.21 {plus minus}0.04, k {sub 3} = 0.227 {plus minus}0.006, k{sub 4} = 0.050 {plus minus}0.002. Reaction 2 occurs via an initial recombination that is rate determining and can be described by the recently modified Gorin model for recombination. Ethyl radical disproportionation (3) is well described by a contact-transition-state model. From k{sub 3} and the known ratio for disproportionation to recombination of 0.14 {plus minus}0.01, the rate of recombination of ethyl radical at 298 K is calculated as k{sub r} = (1.62 {plus minus}0.14) {times} 10{sup {minus}11} cm{sup 3}/molecule {times} s = (9.7 {plus minus}.8) {times} 10{sup 9} L/mol {times} s.

OSTI ID:
6835118
Journal Information:
Journal of the American Chemical Society; (USA), Journal Name: Journal of the American Chemical Society; (USA) Vol. 112:3; ISSN 0002-7863; ISSN JACSA
Country of Publication:
United States
Language:
English