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耦合气象学、金属浓度和 Pb 同位素,对存档降水样本进行来源归因分析。

Coupling meteorology, metal concentrations, and Pb isotopes for source attribution in archived precipitation samples.

机构信息

Geological Sciences and Environmental Studies, Binghamton University, Binghamton, NY 13902, USA.

出版信息

Sci Total Environ. 2013 Mar 15;448:141-50. doi: 10.1016/j.scitotenv.2012.07.031. Epub 2012 Aug 14.

DOI:10.1016/j.scitotenv.2012.07.031
PMID:22901426
Abstract

A technique that couples lead (Pb) isotopes and multi-element concentrations with meteorological analysis was used to assess source contributions to precipitation samples at the Bondville, Illinois USA National Trends Network (NTN) site. Precipitation samples collected over a 16month period (July 1994-October 1995) at Bondville were parsed into six unique meteorological flow regimes using a minimum variance clustering technique on back trajectory endpoints. Pb isotope ratios and multi-element concentrations were measured using high resolution inductively coupled plasma-sector field mass spectrometry (ICP-SFMS) on the archived precipitation samples. Bondville is located in central Illinois, 250km downwind from smelters in southeast Missouri. The Mississippi Valley Type ore deposits in Missouri provided a unique multi-element and Pb isotope fingerprint for smelter emissions which could be contrasted to industrial emissions from the Chicago and Indianapolis urban areas (125km north and east, of Bondville respectively) and regional emissions from electric utility facilities. Differences in Pb isotopes and element concentrations in precipitation corresponded to flow regime. Industrial sources from urban areas, and thorogenic Pb from coal use, could be differentiated from smelter emissions from Missouri by coupling Pb isotopes with variations in element ratios and relative mass factors. Using a three endmember mixing model based on Pb isotope ratio differences, industrial processes in urban airsheds contributed 56±19%, smelters in southeast Missouri 26±13%, and coal combustion 18±7%, of the Pb in precipitation collected in Bondville in the mid-1990s.

摘要

采用一种将铅(Pb)同位素和多元素浓度与气象分析相结合的技术,评估了美国伊利诺伊州邦德维尔国家趋势网络(NTN)站点降水样本的来源贡献。利用最小方差聚类技术对后向轨迹端点进行划分,将 1994 年 7 月至 1995 年 10 月期间在邦德维尔采集的 16 个月降水样本分为 6 种独特的气象流型。使用高分辨率电感耦合等离子体质谱-扇形场质谱仪(ICP-SFMS)对存档降水样本进行 Pb 同位素比值和多元素浓度测量。邦德维尔位于伊利诺伊州中部,距离密苏里州东南部的冶炼厂约 250 公里。密西西比河谷型矿床为冶炼厂排放物提供了独特的多元素和 Pb 同位素特征,可以与来自芝加哥和印第安纳波利斯市区(分别位于邦德维尔以北和以东约 125 公里处)的工业排放物以及来自电力设施的区域排放物进行对比。降水的 Pb 同位素和元素浓度差异与流型相对应。来自城市地区的工业源和源自煤炭使用的钍源,可以通过将 Pb 同位素与元素比值和相对质量因子的变化相结合,与来自密苏里州的冶炼厂排放物区分开来。利用基于 Pb 同位素比值差异的三端元混合模型,城市大气中的工业过程贡献了 56±19%,来自密苏里州东南部的冶炼厂贡献了 26±13%,煤炭燃烧贡献了 18±7%,这些 Pb 是在 20 世纪 90 年代中期在邦德维尔采集的降水样本中所含的。

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