Event-Based Atmospheric Precipitation Uncovers Significant Even and Odd Hg Isotope Anomalies Associated with the Circumpolar Vortex

Shengliu Yuan; Jiubin Chen; Holger Hintelmann

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Event-Based Atmospheric Precipitation Uncovers Significant Even and Odd Hg Isotope Anomalies Associated with the Circumpolar Vortex

机译：Event-Based Atmospheric Precipitation Uncovers Significant Even and Odd Hg Isotope Anomalies Associated with the Circumpolar Vortex

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The determination of the mass-independent fractionation of even Hg isotopes(even-MIF,Δ~(200)Hg) in atmospheric samples adds another intriguing feature to the Hg isotope system.Despite our lack of sufficient experimental verification and the momentary absence of a valid mechanism to explain its occurrence,even-MIF could be instrumental in understanding the cycle and deposition of atmospheric Hg.In contrast to slightly positive Δ~(200)Hg values(<0.30‰) frequently observed in most atmospheric samples,large Δ~(200)Hg values(up to 1.24‰) determined in precipitation from Peterborough(Ontario,Canada) stand out and could provide valuable information for the origin of the even-MIF mystery.We now report a systematic analysis of high-resolution rainfall and snowfall samples collected in winter during cold weather at Peterborough,Canada.Dissolved and particulate Hg both displayed large variations of odd-MIF(from-0.93‰ to 2.02‰ for Δ~(199)Hg),which may result from long-range transportation,as the negative odd-MIF in particulate Hg is likely a result of long-distance transport of arctic atmospheric Hg(II).Dissolved Hg revealed significant even-MIF values(from 0.25%c to 1.19‰ for Δ~(200)Hg) and a negative relationship between Δ~(200)Hg and Δ~(204)Hg,which provide further evidence for the previously proposed conceptual model of Δ~(200)Hg.Disconnected odd-MIF and even-MIF trends were detected in sequentially collected precipitation samples,which further suggests different sources or mechanisms for Δ~(199)Hg and Δ~(200)Hg.Particularly,the high Δ~(200)Hg values highlight the transport of stratospheric Hg through a polar vortex to the sampling region,stimulating further systematic investigation.The new Δ~(200)Hg data for particulate Hg add to existing information on atmospheric Hg(II) worldwide,suggesting a global distribution of Hg characterized by even-MIF in the atmosphere,and further constrain the model of atmospheric Hg deposition.

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《Environmental Science & Technology: ES&T》 |2022年第17期|12713-12722|共10页
作者
Shengliu Yuan; Jiubin Chen; Holger Hintelmann;
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作者单位

Chemistry Department,Trent University,Peterborough,Ontario K9J 7B8,Canada;

Institute of Surface-Earth System Science,Tianjin University,Tianjin 300072,People's Republic of China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
atmospheric Hg; mass-independent fractionation(MIF); troposphere and stratosphere; wet deposition; polar vortex;

Event-Based Atmospheric Precipitation Uncovers Significant Even and Odd Hg Isotope Anomalies Associated with the Circumpolar Vortex

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