DOI: 10.1002/2014JD021915
论文题名: Volcanic sulfate aerosol formation in the troposphere
作者: Martin E. ; Bekki S. ; Ninin C. ; Bindeman I.
刊名: Journal of Geophysical Research Atmospheres
ISSN: 2169897X
出版年: 2014
卷: 119, 期: 22 起始页码: 12660
结束页码: 12673
语种: 英语
英文关键词: mass-independent fractionation
; O and S isotopes
; sulfate aerosols
; troposphere
; volcanic plume
Scopus关键词: catalysis
; gas phase reaction
; isotopic analysis
; Northern Hemisphere
; plume
; sulfate
; troposphere
; volcanic aerosol
; volcanic eruption
; Mexico [North America]
英文摘要: The isotopic composition of volcanic sulfate provides insights into the atmospheric chemical processing of volcanic plumes. First, mass-independent isotopic anomalies quantified by Δ17O and to a lesser extent Δ33S and Δ36S in sulfate depend on the relative importance of different oxidation mechanisms that generate sulfate aerosols. Second, the isotopic composition of sulfate (δ34S and δ18O) could be an indicator of fractionation (distillation/condensation) processes occurring in volcanic plumes. Here we present analyses of O- and S isotopic compositions of volcanic sulfate absorbed on very fresh volcanic ash from nine moderate historical eruptions in the Northern Hemisphere. Most of our volcanic sulfate samples, which are thought to have been generated in the troposphere or in the tropopause region, do not exhibit any significant mass-independent fractionation (MIF) isotopic anomalies, apart from those from an eruption of a Mexican volcano. Coupled to simple chemistry model calculations representative of the background atmosphere, our data set suggests that although H2O2 (a MIF-carrying oxidant) is thought to be by far the most efficient sulfur oxidant in the background atmosphere, it is probably quickly consumed in large dense tropospheric volcanic plumes. We estimate that in the troposphere, at least, more than 90% of volcanic secondary sulfate is not generated by MIF processes. Volcanic S-bearing gases, mostly SO2, appear to be oxidized through channels that do not generate significant isotopically mass-independent sulfate, possibly via OH in the gas phase and/or transition metal ion catalysis in the aqueous phase. It is also likely that some of the sulfates sampled were not entirely produced by atmospheric oxidation processes but came out directly from volcanoes without any MIF anomalies. ©2014. American Geophysical Union. All Rights Reserved. 资助项目: 14-CE33-0009-02-FOFAMIFS
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/63029
Appears in Collections: 影响、适应和脆弱性 气候减缓与适应
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作者单位: Sorbonne Universités, UPMC Université Paris 06, UMR 7193, Paris, France; CNRS, UMR 7193, ISTeP, Paris, France; Sorbonne Universités, UPMC Université Paris 06, Université Versailles St.-Quentin, Paris, France; Department of Geological Sciences, University of Oregon, Eugene, OR, United States
Recommended Citation:
Martin E.,Bekki S.,Ninin C.,et al. Volcanic sulfate aerosol formation in the troposphere[J]. Journal of Geophysical Research Atmospheres,2014-01-01,119(22)