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Chlorine-catalysed Pyrolysis of 1,2-Dichloroethane. Part 1.- Experimental Results and Proposed Mechanism

DOI: 10.1039/f19827800657

Source and publish data:

Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases p. 657 - 676 (1982)

Update date:2022-08-29

Topics:

Authors:

Ashmore, Philip G.Ashmore, Philip G.

Gardner, John W.Gardner, John W.

Owen, Anthony J.Owen, Anthony J.

Smith, BarbaraSmith, Barbara

Sutton, Philip R.Sutton, Philip R.

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Article abstract of DOI:10.1039/f19827800657

Experimental studies of the pyrolysis and chlorination of 1,2-C2H4Cl2 in the presence of small proportions of chlorine, or of chlorine plus nitric oxide, confirm that the main propagating steps between 520 and 620 K are .The initial rates (d/dt)0 and (d/dt)0-decrease together as the vessels age, but k2/k3=γ remains constant at constant pDCE. γ increases as pDCE is increased, or if inert gases are added, as expected from unimolecular behaviour of k2, and the Arrhenius parameters of γ increase together as pDCE is increased. γ(p) is evaluated for several ranges of pDCE at five temperatures to allow study of k2(p) by unimolecular theory in Part 2.The addition of VC lowers (d/dt)0 through reaction (-2), and the results are used to evaluate k-2/k1; k-2 is also pressure-dependent.In vessels with fresh surfaces, d(VC)/dt is proportional to pDCExp0.5Cl for low pCl and is independent of added inert gases; in aged vessels, the order in pDCE becomes 0.62, very close to the dependence of γ(p) on pDCE.Calculations of .>0 and .>0 from the observed rates and rate constants point to an initiation step and termination by the reverse reaction in fresh-surfaced vessels, where S is a surface site; with aged surfaces, the results point to the same initiation step combined with termination by especially at lower temperatures.

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