School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, United Kingdom.
Proc Natl Acad Sci U S A. 2010 Apr 13;107(15):6594-9. doi: 10.1073/pnas.0913164107. Epub 2010 Apr 5.
Recent field observations have shown that the atmospheric plumes of quiescently degassing volcanoes are chemically very active, pointing to the role of chemical cycles involving halogen species and heterogeneous reactions on aerosol particles that have previously been unexplored for this type of volcanic plumes. Key features of these measurements can be reproduced by numerical models such as the one employed in this study. The model shows sustained high levels of reactive bromine in the plume, leading to extensive ozone destruction, that, depending on plume dispersal, can be maintained for several days. The very high concentrations of sulfur dioxide in the volcanic plume reduces the lifetime of the OH radical drastically, so that it is virtually absent in the volcanic plume. This would imply an increased lifetime of methane in volcanic plumes, unless reactive chlorine chemistry in the plume is strong enough to offset the lack of OH chemistry. A further effect of bromine chemistry in addition to ozone destruction shown by the model studies presented here, is the oxidation of mercury. This relates to mercury that has been coemitted with bromine from the volcano but also to background atmospheric mercury. The rapid oxidation of mercury implies a drastically reduced atmospheric lifetime of mercury so that the contribution of volcanic mercury to the atmospheric background might be less than previously thought. However, the implications, especially health and environmental effects due to deposition, might be substantial and warrant further studies, especially field measurements to test this hypothesis.
最近的实地观测表明,处于静止排气状态的火山的大气羽流在化学上非常活跃,这表明涉及卤素物种的化学循环以及气溶胶颗粒上的多相反应在以前对这种类型的火山羽流尚未得到探索。这些测量的关键特征可以通过数值模型来重现,例如本研究中使用的模型。该模型显示羽流中持续存在高水平的活性溴,导致广泛的臭氧破坏,这取决于羽流的扩散情况,臭氧破坏可持续数天。火山羽流中二氧化硫的浓度非常高,大大缩短了 OH 自由基的寿命,因此在火山羽流中几乎不存在 OH 自由基。这意味着甲烷在火山羽流中的寿命会延长,除非羽流中的活性氯化学物质足够强大,可以抵消 OH 化学物质的缺乏。除了这里展示的模型研究表明的臭氧破坏之外,溴化学物质还有另外一个作用,即汞的氧化。这与从火山共排放的溴和背景大气中的汞有关。汞的快速氧化意味着汞在大气中的寿命大大缩短,因此火山汞对大气背景的贡献可能比以前认为的要小。然而,其影响,特别是由于沉积造成的健康和环境影响,可能是巨大的,需要进一步的研究,特别是现场测量来验证这一假设。