Methyl bromide (MeBr) is used increasingly as a biocidal fumigant, primarily in agricultural soils prior to planting ofcrops. This usage carries potential for stratospheric ozone reduction due to Br atom catalysis, depending on how much MeBr escapes from fumigated soils to the atmosphere and on details of atmospheric chemical reactions. We present direct field measurements of MeBr escape; 87% of the applied MeBr was emitted within 7 days after a commercial fumigation. Covering the field with plastic sheets retarded MeBr escape somewhat but first-day losses were still 40%; thicker sections of sheets were relatively more effective than thin sections. We also measured gaseous MeBr concentrations versus depth in the soil column; these profiles display diffusion-like evolution. In soil, MeBr is partitioned among gas, liquid, and adsorbed solid phases. The contribution of halons to the bromine flux, F., that enters the stratosphere is relatively well known (7.2 x 106 kg of Br per year in 1990) because the halons are totally synthetic, their industrial production and emission rates are known and they are inert in the troposphere (5, 6).The contribution from MeBr to F,, on the other hand, is poorly quantified at present. Natural sources, principally oceanic surface waters, are known to inject MeBr into surface air but are not well quantified (7,8). Currently, the global atmospheric content, B, of MeBr is 2 + 0.5 x 108 kg. If reaction with tropospheric OH radicals (7-9) is its major sink, the atmospheric residence time, T, for MeBr is 2 + 0.5 years. In an assumed quasi steady state, the total surface source = BIT or 0.6 to 1.7 x 108 kg/year (7)(8)(9). While muchThe publication costs of this article were defrayed in part by page charge payment. This article must therefore be hereby marked "advertisement" in accordance with 18 U.S.C. §1734 solely to indicate this fact.of the MeBr upward flux may be removed by tropospheric OH, thus limiting its contribution to F,, the amount that reaches the stratosphere may still exceed the contributions from CF3Br and CBrClF2.Concern arises over synthetic MeBr because its worldwide industrial usage has increased from 4.2 x 107 to 6.3 x 107 kg/year between 1984 and 1990; these figures exclude MeBr used as a chemical intermediate. Eighty percent of this usage is as an agricultural soil fumigant prior to planting (10). MeBr is a broad-spectrum fumigant biocide against arthropods, weeds, nematodes, fungi, and bacterial pests, apparently cost effective when applied to soils before planting; it is being used in many countries (10). Thus there is a significant and growing potential for atmospheric MeBr to increase, depending on the fraction of MeBr that escapes from soils during and after fumigations and on the size of the natural sources (7,8). In soils, MeBr may be removed by physical hydrolysis, adsorption to soil particles, and microbiological and transport processes (11,12). Moisture and organic matter in soils should enhance dissociation rates but it is very difficult to estimate h...
The treatment of agricultural soils with CH 3 Br (MeBr) has been suggested to be a significant source of atmospheric MeBr which is involved in stratospheric ozone loss. A field fumigation experiment showed that, after 7 days, 34 percent of the applied MeBr had escaped into the atmosphere. The remaining 66 percent should have caused an increase in bromide in the soil; soil bromide increased by an amount equal to 70 percent of the applied MeBr, consistent with the flux measurements to within 4 percent. Comparison with an earlier experiment in which the escape of MeBr to the atmosphere was greater showed that higher soil pH, organic content and soil moisture, and deeper, more uniform injection of MeBr may in combination reduce the escape of MeBr.
[1] Methyl halide gases are important sources of atmospheric inorganic halogen radicals. We measured methyl halide emissions from three rice fields over two full growing seasons. Rice paddy emissions of methyl chloride, methyl bromide and methyl iodide are insignificant until field flooding. Rice growth stage determines methyl bromide and methyl iodide emissions while methyl chloride emissions are comparable between planted and unplanted plots. Houston, Texas, and Maxwell, California, field integrated seasonal fluxes of methyl chloride, methyl bromide and methyl iodide are consistent (values range from 2.3 to 3.9, 0.8 to 1.1, and 28.1 to 62.0 mg m À2 , respectively) despite differences in multiple field parameters. We also examined field emission variability using 12 chamber placements. Methyl bromide and methyl iodide emissions within homogenous rice paddies require at least three replicates to determine field mean fluxes within 20%, and for methyl chloride emissions, over 10 replications per field are necessary.
[1] This paper investigates physiological and biochemical aspects of methyl halide production in rice plants over two growing seasons. Multiple separate mechanisms appear to be responsible for production of methyl halides in rice plant tissues. Evidence for multiple mechanisms is found in timing of peak emissions of methyl halides from rice, inconsistent effects of competitive inhibitors on methyl halide emissions, and large differences in methyl halide emission rates when compared to plant tissue halide concentrations. Other results show that chloride, bromide, and iodide ion concentrations in plant tissue appear to be regulated throughout the season, and observed changes in leaf tissue concentration cannot explain observed methyl halide emissions. The K m for methyl iodide formation in leaf tissue cell-free extract is 0.018 mM, suggesting a very efficient mechanism. Of the seven competitive inhibitors used, only thiol had a consistently strong effect on both methyl iodide and methyl bromide.
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