修正的铅锶同位素混合模型定量解析大气PM_(2.5)的来源
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摘要
本文在2014年3月至2015年1月采集了泉州市城区5个采样点的大气PM_(2.5)样品,并同步采集泉州市主要大气PM_(2.5)潜在污染源样品.采用电感耦合等离子质谱(ICP-MS)和热电离质谱(TIMS)分析样品中铅、锶含量及铅、锶同位素的组成,利用铅、锶二元同位素示踪了大气PM_(2.5)的污染来源.结果表明,泉州市大气PM_(2.5)主要来自建筑尘、交通源、燃煤尘、垃圾焚烧厂飞灰和土壤扬尘.通过对传统的同位素混合模型计算方法的修正,尝试解决"二元同位素混合模型"无法定量解析3个以上PM_(2.5)潜在污染源的问题.根据修正的同位素混合模型计算采样期间大气各个PM_(2.5)潜在污染源的平均贡献率,分别为建筑尘(23.3%～35.4%)、交通源(22.4%～52.9%)、燃煤尘(10.1%～24.1%)、垃圾焚烧飞灰(2.1%～4.8%)和土壤扬尘(2.1%～14.5%),表明该修正方法具有一定的应用价值.
Atmospheric PM_(2.5) samples from five sampling stations in the urban area of Quanzhou were obtained between March 2014 and January 2015. Samples of major potential sources for atmospheric PM_(2.5) of Quanzhou were collected simultaneously. Inductively coupled plasma mass spectrometry(ICP-MS) and thermal ionization mass spectrometry(TIMS) were employed to analyse contents and isotopic compositions of lead and strontium of the samples. Clumped isotopes of lead and strontium were used to track the sources for atmospheric PM_(2.5). The results reveal that atmospheric PM_(2.5) of Quanzhou mainly originates from construction, traffic, coal combustion, incineration plants, and soil dust. The calculation method by the traditional isotope mixing model was corrected to solve the problemthat the "clumped isotope mixing model" cannot quantitatively resolve three or more potential PM_(2.5) sources. Accordingto the corrected isotope mixing model, the average contribution of each potential atmospheric PM_(2.5) source during the sampling period was determined. The contributions of construction, traffic, coal combustion, incineration plants, andsoil dust are 23.3%–35.4%, 22.4%–52.9%, 10.1%–24.1%, 2.1%–4.8%, and 2.1%–14.5%, respectively. This indicates that the corrected model is applicable in certain cases.
Atmospheric PM_(2.5) samples from five sampling stations in the urban area of Quanzhou were obtained between March 2014 and January 2015. Samples of major potential sources for atmospheric PM_(2.5) of Quanzhou were collected simultaneously. Inductively coupled plasma mass spectrometry(ICP-MS) and thermal ionization mass spectrometry(TIMS) were employed to analyse contents and isotopic compositions of lead and strontium of the samples. Clumped isotopes of lead and strontium were used to track the sources for atmospheric PM_(2.5). The results reveal that atmospheric PM_(2.5) of Quanzhou mainly originates from construction, traffic, coal combustion, incineration plants, and soil dust. The calculation method by the traditional isotope mixing model was corrected to solve the problemthat the "clumped isotope mixing model" cannot quantitatively resolve three or more potential PM_(2.5) sources. Accordingto the corrected isotope mixing model, the average contribution of each potential atmospheric PM_(2.5) source during the sampling period was determined. The contributions of construction, traffic, coal combustion, incineration plants, andsoil dust are 23.3%–35.4%, 22.4%–52.9%, 10.1%–24.1%, 2.1%–4.8%, and 2.1%–14.5%, respectively. This indicates that the corrected model is applicable in certain cases.
引文
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2 Wu Y,Chen J.Studies Trace Elements Health,2009,26:65-67(in Chinese)[武永锋,陈建华.微量元素与健康研究,2009,26:65-67]
3 Chow TJ.Nature,1970,225:295-296
4 Hurst RW,Terry ED.Eng Goel,1981,3:363-367
5 Lee CSL,Li XD,Zhang G,Li J,Ding AJ,Wang T.Atmos Environ,2007,41:432-447
6 Widory D,Liu X,Dong S.Atmos Environ,2010,44:3679-3687
7 Zhao Y,Yu R,Hu G,Lin X,Liu X.Particuology,2017,32:95-102
8 Cai J,Wang J,Zhang Y,Tian H,Zhu C,Gross DS,Hu M,Hao J,He K,Wang S,Zheng M.Environ Pollut,2017,226:30-40
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