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Ozone Depletion in Tropospheric Volcanic Plumes: From Halogen-Poor to Halogen-Rich Emissions

机译:对流层火山羽中的臭氧消耗:从贫卤素到富卤素排放

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Volcanic halogen emissions to the troposphere undergo a rapid plume chemistry that destroys ozone. Quantifying the impact of volcanic halogens on tropospheric ozone is challenging, only a few observations exist. This study presents measurements of ozone in volcanic plumes from Kīlauea (HI, USA), a low halogen emitter. The results are combined with published data from high halogen emitters (Mt Etna, Italy; Mt Redoubt, AK, USA) to identify controls on plume processes. Ozone was measured during periods of relatively sustained Kīlauea plume exposure, using an Aeroqual instrument deployed alongside Multi-Gas SO 2 and H 2 S sensors. Interferences were accounted for in data post-processing. The volcanic H 2 S/SO 2 molar ratio was quantified as 0.03. At Halema‘uma‘u crater-rim, ozone was close to ambient in the emission plume (at 10 ppmv SO 2 ). Measurements in grounding plume (at 5 ppmv SO 2 ) about 10 km downwind of Pu‘u ‘ō‘ō showed just slight ozone depletion. These Kīlauea observations contrast with substantial ozone depletion reported at Mt Etna and Mt Redoubt. Analysis of the combined data from these three volcanoes identifies the emitted Br/S as a strong but non-linear control on the rate of ozone depletion. Model simulations of the volcanic plume chemistry highlight that the proportion of HBr converted into reactive bromine is a key control on the efficiency of ozone depletion. This underlines the importance of chemistry in the very near-source plume on the fate and atmospheric impacts of volcanic emissions to the troposphere.
机译:进入对流层的火山卤素排放会经历快速的羽状化学反应,从而破坏臭氧。量化火山卤素对对流层臭氧的影响具有挑战性,只有很少的发现。这项研究提供了来自低卤素发射器Kīlauea(美国HI)的火山羽中臭氧的测量结果。将结果与来自高卤素发射器(意大利埃特纳火山;美国阿拉巴马州Mt Redoubt)的公开数据相结合,以确定羽流过程的控制方法。使用部署在Multi-Gas SO 2和H 2 S传感器旁边的Aeroqual仪器,在相对持续的Kīlauea羽流暴露期间测量了臭氧。在数据后处理中考虑了干扰。火山H 2 S / SO 2摩尔比定量为0.03。在Halemaʻuma’u火山口边缘,排放羽流中的臭氧接近环境(SO 2为10 ppmv时)。在Pu'u‘ō’ō顺风向约10公里处的地面羽状流(在5 ppmv SO 2处)的测量结果显示,臭氧消耗量很小。这些基拉韦厄的观测与埃特纳火山和Redoubt山报告的大量臭氧消耗形成对比。对这三个火山的综合数据的分析表明,所排放的Br / S是对臭氧消耗速率的强有力但非线性的控制。火山羽化学的模型模拟表明,HBr转化成活性溴的比例是控制臭氧消耗效率的关键控制因素。这强调了在近源羽流中化学作用对火山向对流层排放的命运和大气影响的重要性。

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