State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China; University of Chinese Academy of Sciences, Beijing 100049, China.
State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China.
Sci Total Environ. 2021 Mar 15;760:143935. doi: 10.1016/j.scitotenv.2020.143935. Epub 2020 Dec 5.
The source of fine particulate matter (PM) has been a longstanding subject of debate, the nitrogen-15 isotope (δN) has been used to identify the major sources of atmospheric nitrogen. In this study, PM samples (n = 361) were collected from September 2017 to August 2018 in the urban area of Guiyang (SW, China), to investigate the chemical composition and potential sources of PM. The results showed an average PM of 33.0 μg m ± 20.0 μg m. The concentration of PM was higher in Winter, lower in Summer. The major water resolved inorganic ions (WSIIs) were Ca, NH, Na, SO, NO, Cl. Nitrogen-containing aerosols (i.e., NO and NH) suddenly strengthened during the winter, when NO became the dominant contributor. Over the sampling period, the molar ratio of NH/(NO + 2 × SO) ranged from 0.1 to 0.9, thus indicating the full fixation of NH by existing NO and SO in PM. The annual value of NOR was 0.1 while rised to 0.5 in Winter. The variations of NOR (Nitrogen oxidation ratio) (0.1-0.5) values suggest that the secondary formation of NO occurred every season and was most influential during the winter. The total particulate nitrogen (TN) δN value of PM ranged from -5.9‰ to 25.3‰ over the year with annual mean of +11.8‰ ± 4.7‰, whereas it was between -5.9‰ and 14.3‰ during the winter with mean of 7.0‰ ± 3.8‰. A Bayesian isotope mixing model (Stable Isotope Analysis in R; SIAR) was applied to analyze the nitrogen sources. The modeling results showed that 29%, 21%, and 40% of TN in PM during the winter in Guiyang was due to nitrogen-emissions from coal combustion, vehicle exhausts, and biomass burning, respectively. Our results demonstrate that biomass burning was the main contributor to PM during the winter, 80% of the air mass comes from rural areas of Guizhou border, this transport process can increase the risk of particulate pollution in Guiyang.
细颗粒物(PM)的来源一直是一个长期存在的争论话题,氮-15 同位素(δN)已被用于识别大气氮的主要来源。本研究于 2017 年 9 月至 2018 年 8 月在贵阳市(西南,中国)城区采集了 PM 样本(n=361),以调查 PM 的化学组成和潜在来源。结果表明,PM 的平均浓度为 33.0μg/m ± 20.0μg/m。PM 浓度在冬季较高,夏季较低。主要的水解析出无机离子(WSIIs)是 Ca、NH、Na、SO、NO、Cl。含氮气溶胶(即 NO 和 NH)在冬季突然增强,此时 NO 成为主要贡献者。在采样期间,NH/(NO+2×SO)的摩尔比范围从 0.1 到 0.9,这表明 NH 已由 PM 中的现有 NO 和 SO 完全固定。NOR 的年值为 0.1,而在冬季升高到 0.5。NOR(氮氧化比)(0.1-0.5)值的变化表明,NO 的二次形成发生在每个季节,在冬季影响最大。PM 中总颗粒态氮(TN)δN 值全年范围为-5.9‰至 25.3‰,年平均值为+11.8‰±4.7‰,而冬季范围为-5.9‰至 14.3‰,平均值为 7.0‰±3.8‰。应用贝叶斯同位素混合模型(Stable Isotope Analysis in R;SIAR)分析氮源。建模结果表明,贵阳市冬季 PM 中 29%、21%和 40%的 TN 分别来自煤炭燃烧、车辆尾气和生物质燃烧的氮排放。我们的结果表明,生物质燃烧是冬季 PM 的主要贡献者,80%的气团来自贵州边境的农村地区,这种传输过程会增加贵阳市颗粒物污染的风险。