Journal of Atmospheric Chemistry 25: 167-199, 1996. 167
© 1996 Kluwer Academic Publishers. Printed in the Netherlands.
Two-Dimensional Modelling of Some CFC
Replacement Compounds
OLIVER WILD,* OLIVER V. RATFIGAN,** RODERIC L. JONES,
JOHN A. PYLE and R. ANTHONY COX
Centre for Atmospheric Science, Department of Chemistry, University of Cambridge,
Cambridge CB2 I EW, U.K.
(Received: 2 November 1995; in final form: 17 June 1996)
Abstract. The Cambridge 2-D Eulerian model has been used to study the potential atmospheric
distributions and lifetimes of a number of CFC replacement compounds and their degradation prod-
ucts. The study has focused on I-IFC 134a and HCFCs 123, 141b and 142b and the major products
formed by their atmospheric degradation. The loss of these compounds and their products by hydrox-
yl radical attack, photolysis and in-cloud hydrolysis have been investigated. The study has shown
that HCFCs 141b and 142b have sufficiently long lifetimes to enter the stratosphere in significant
quantities, where degradation leads to an increase in the total stratospheric chlorine concentration.
The study has also highlighted areas where further experimental work would be valuable, in partic-
ular characterisation of the product channels for the degradation reactions and deter'ruinationof the
removal rates of the products in the aqueous phase.
Key words: CFC replacement compounds, distributions, tropospheric lifetimes, trifluoroacetic acid.
1. Introduction
Since their discovery in the late 1930s chlorofluorocarbons (CFCs) have been
used extensively both in industry and domestically as refrigerants, solvents and
propellants. Their physical properties and volatility make them ideal for these
purposes, and their chemically inert nature makes them safe for everyday use.
However, a number of studies over the past few years have indicated that the
heavy use of these compounds has been responsible for a significant build up of
chlorine in the lower stratosphere, and that this is one of the major factors in the
observed depletion of ozone in the polar lower stratosphere (Farman et aL, 1985;
SORG, 1993). A number of substitute compounds have been proposed with simi-
lar physical properties (WMO, 1989), but with little or no effect on stratospheric
chlorine or ozone levels. The most important of these are the hydrochlorofluorocar-
bons (HCFCs) and hydrofluorocarbons (HFCs). These compounds are preferable
to CFCs as they contain at least one hydrogen atom which is susceptible to hydrox-
yl attack in the troposphere, and consequently a smaller proportion reaches the
stratosphere. The HFCs are particularly important, as they do not contain chlorine,
* Now at: Earth System Science, University of California, Irvine CA 92697.
** Now at: Department of Chemistry, Boston College, Boston MA 02167.