respectively, what are the minimum wavelengths needed to break these bonds? Comment on the relevance with respect to why (1) organoiodine compounds have such short lifetimes in the troposphere and (2) the lifetimes of organoiodine compounds are shorter than those of the analogous organobromine compounds.

2. CH3Br reacts with OH with a room temperature rate constant of 2.9 X 10"14 cm3 molecule"1 s"1.

(a) What is the lifetime of methyl bromide with respect to reaction with OH at a global mean concentration of 5 X 105 radicals cm"3?

(b) Colman et al. (1998) report an atmospheric lifetime of 0.8 + 0.1 years for methyl bromide. Since it is also taken up by soils and oceans, what must the lifetime with respect to uptake by soils and oceans be?

(c) If the global mean OH concentration is really 1 X 106 radicals cm"3, what must the lifetime be with respect to uptake by soils and oceans?

3. Keim et al. (1996) have shown that there is a significant reduction in NO and increase in NO and CIO in a layer above the tropopause that has increased aerosol surface areas (Fig. 12.31). They attribute this to increased heterogeneous reactions of C10N02 on particles to form HN03 and active chlorine.

(a) Estimate the ratio of the rates of C10N02 loss and HN03 production in going from an altitude of ff km below the aerosol layer where the particle surface area is ~4 /xm2 cm"3 to 13 km where the surface area is ~20 /xm2 cm"3. Assume the temperature and C10N02 concentrations remain approximately constant over this altitude range.

(b) Estimate the ratio of the lifetimes for C10N02 with respect to heterogeneous hydrolysis in going from 14 km above the aerosol layer to 13 km, at the top of the layer. Assume the reaction probability is 10"3 for the particle composition at 14 km but increases to 0.1 at 13 km due to the increased water content of these particles in the aerosol layer. Use Fig. 12.31 to estimate the change in particle surface area from 14 to 13 km and assume the temperature at both altitudes is approximately 210 K. Does this support the conclusion of Keim et al. (1996) that activation on particles is a reasonable explanation for their observations?

4. McKinney et al. (1997) report measurements of CIO and BrO in a chemically perturbed region of the stratosphere over Sweden. They observe that the production of BrO with decreasing solar zenith angle is so rapid that it implies the bromine atom source is very photolabile, likely BrCl, rather than BrONOz. Using data from Chapters 3 and 4, calculate the lifetimes of BrCl and Br0N02 at a solar zenith angle of 86° to estimate how much faster BrCl photolysis would be compared to Br0N02 at 25 km. Assume the earth-sun distance correction factor is 1.0.

5. If the aerosol surface area in the McKinney et al. studies in Problem 4 was 5 fxm2 cm"3, what would the lifetime be for Br0N02 with respect to hydrolysis on particles? Take a temperature of 200 K and assume a reaction probability of 0.8 (Table 12.8) and that the reaction is not diffusion-limited. Compare this to the lifetime with respect to photolysis calculated in Problem 4.

6. The hydrolysis of Br0N02 does not generate active bromine directly, but rather HOBr, which must then photolyze to OH + Br. Calculate the lifetime of HOBr with respect to photolysis at a solar zenith angle of 86° and an altitude of 25 km. Assume the earth-sun distance correction factor is 1.0. Is the hydrolysis of Br0N02 or the photolysis of HOBr the rate-determining step?


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Koike, M., Y. Kondo, W. A. Matthews, P. V. Johnston, and K. Yamazaki

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