引用本文:闫磊,黄银芝,高松,等.杭州湾北岸36种挥发性有机物污染特征及来源解析[J].环境科学研究,2020,33(3):536-546.
YAN Lei,HUANG Yinzhi,GAO Song,et al.Pollution Characteristics and Source Analysis of 36 Volatile Organic Compounds on the North Coast of Hangzhou Bay[J].Research of Environmental Sciences,2020,33(3):536-546.]
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杭州湾北岸36种挥发性有机物污染特征及来源解析
闫磊1,2,3, 黄银芝1,2,3, 高松4, 修光利1,2,3
1. 华东理工大学, 国家环境保护化工过程环境风险评价与控制重点实验室, 上海 200237;2. 华东理工大学, 上海市环境保护化学污染物环境标准与风险管理重点实验室, 上海 200237;3. 上海污染控制与生态安全研究院, 上海 200237;4. 上海市环境监测中心, 上海 200235
摘要:
为研究杭州湾北岸VOCs(挥发性有机物)的浓度水平、组成特征、反应活性和潜在来源,采用GC-FID在线监测系统对杭州湾北岸环境大气中的36种VOCs开展了为期1 a(2017年12月-2018年11月)的连续观测,采用LOH(VOCs的·OH消耗速率)和OFP(O3生成潜势)2种方法估算了大气VOCs的反应活性,并利用PMF(正定矩阵因子分解)和CPF(条件概率函数)模型分析其来源.结果表明:①φ(VOCs)小时平均值在冬季(26.47×10-9)最高,夏季(9.76×10-9)最低;全年φ(VOCs)小时平均值为21.24×10-9,其中烷烃、烯烃+炔烃、芳香烃、卤代烃的贡献率分别为33.24%、34.13%、15.63%、17.00%;φ(烷烃)、φ(芳香烃)和φ(卤代烃)呈较明显的昼夜变化特征,φ(烯烃)和φ(炔烃)无明显昼夜变化趋势.②大气VOCs的总LOH和OFP分别为9.39 s-1和220.57 μg/m3KOH(·OH反应速率常数)和MIR(最大增量反应活性)系数的平均值分别为17.34×10-12 cm3/(molecule·s)和3.31;KOH和MIR系数的平均值分别与间/对-二甲苯的KOH和乙苯的MIR系数接近,表明大气VOCs的化学反应活性较强;VOCs关键活性物种为异戊二烯、乙烯、丙烯、甲苯、二甲苯和顺-2-丁烯.③特征物种相关性分析表明,杭州湾北岸大气存在老化现象,异戊烷和正戊烷受煤燃烧源影响较大,二甲苯和乙苯受溶剂排放源影响较大,甲苯和苯除受机动车尾气影响外,还受其他排放源影响.④PMF和CPF模型来源分析表明,大气VOCs主要来自石化工业源、燃料挥发源、生物质燃烧和煤燃烧源、机动车排放源和溶剂使用源,其中,机动车排放源主要来自西北方向,其他源主要来自西北、西和西南方向.研究显示,杭州湾北岸大气VOCs来源复杂,受周边工业区的影响较大.
关键词:  挥发性有机物  反应活性  PMF模型  来源解析
DOI:10.13198/j.issn.1001-6929.2019.05.26
分类号:X513
基金项目:国家重点研发计划项目(No.2016YFC0200502);上海市环境监测中心项目(No.SEMC-SHXM-00-20180402-0079);上海市环境保护局项目(No.沪环科[2018]11号)
Pollution Characteristics and Source Analysis of 36 Volatile Organic Compounds on the North Coast of Hangzhou Bay
YAN Lei1,2,3, HUANG Yinzhi1,2,3, GAO Song4, XIU Guangli1,2,3
1. State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237, China;2. Shanghai Environmental Protection Key Laboratory on Environmental Standard and Risk Management of Chemical Pollutants, East China University of Science and Technology, Shanghai 200237, China;3. Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200237, China;4. Shanghai Environmental Monitoring Center, Shanghai 200235, China
Abstract:
To study the concentration, composition, reactivity and source of ambient VOCs (volatile organic compounds) on the north coast of Hangzhou Bay, 36 ambient VOCs species were measured continuously for a year by online gas chromatography with flame ionization detection systems (GC-FID) from December 2017 to November 2018. LOH (·OH radical loss rate) and OFP (ozone formation potential) were used to estimate the reactivity of ambient VOCs, and the PMF (positive matrix factorization) model and CPF (conditional probability function) model were used to analyze the potential sources of VOCs. The results showed that:(1) The hourly average of ambient φ(VOCs) was the highest in winter (26.47×10-9) and lowest in summer (9.76×10-9). The hourly average of φ(VOCs) was 21.24×10-9 during the sampling period, of which alkanes, alkenes and alkynes, aromatics, and halohydrocarbons accounted for 33.24%, 34.13%, 15.63%, and 17.00%, respectively. Alkanes, aromatics and halohydrocarbons showed obvious diurnal pattern, while there was no obvious diurnal variation for alkenes and alkynes. (2) The total LOH and OFP of the ambient VOCs were 9.39 s-1 and 220.57 μg/m3, respectively, with the average KOH (·OH radical loss rate constant) and MIR (maximum O3 incremental reactivity) coefficient of 17.34×10-12 cm3/(molecule·s) and 3.31, respectively, which was close to the KOH of m, p-xylene and the MIR coefficient of ethylbenzene, respectively. The results indicated that the ambient VOCs had relatively high chemical reactivity. The key reactive species were isoprene, ethene, propene, toluene, xylene and cis-2-butene. (3) The correlation analysis of the specific VOCs species showed that the plumes were aged, iso-pentane and n-pentane were more likely affected by coal combustion, while xylene and ethylbenzene were greatly affected by organic solvent emissions. Apart from vehicle exhaust, toluene and benzene were also affected by other emission sources. (4) The source apportionment identified by PMF and CPF model showed that the ambient VOCs were mainly from petrochemical industry, fuel volatilization, biomass and coal burning, vehicular emissions and organic solvent usage. Vehicle emissions were mainly from the northwest direction, while other sources mainly were from the northwest, west and southwest. The research showed that the sources of the ambient VOCs on the north coast of Hangzhou Bay were complex and greatly influenced by the nearby industrial parks.
Key words:  volatile organic compounds  reactivity  positive matrix factorization model  source analysis