摘要
水溶性有机氮(WSON)在大气化学和气候变化中具有重要作用,目前鲜有针对WSON粒径分布的研究。本研究利用大流量采样器在2014年9月至2015年7月期间采集了广州市各个季节PM_(10)中不同粒径段(<0.49μm、0.49~0.95μm、0.95~1.5μm、1.5~3.0μm、3.0~7.2μm、7.2~10μm)大气颗粒物样品共100个,分析了其中的水溶性总氮(WSTN)、WSON以及水溶性无机氮(WSIN)含量。结果表明,各个粒径段中WSON的浓度呈现相似的季节变化特征,秋、冬季较高,春、夏季较低。WSON主要分布在细颗粒物上,PM_3中WSON的季节平均浓度在1.15~2.62μg/m~3范围内,占PM_(10)中WSON总量的63%~71%。WSON的粒径分布呈现单峰分布,主要富集在0.49~1.5μm粒径段。主成分分析/绝对主成分得分(PCA/APCS)分析表明,<0.49μm颗粒物上的WSON主要来源于本地化石燃料的燃烧排放;0.49~0.95μm颗粒物的WSON主要来源于建筑扬尘和光化学氧化二次生成过程;0.95~1.5μm颗粒物的WSON主要来源于光化学氧化二次生成过程。研究结果增加了目前对于WSON粒径分布特征和来源的认识。
Water-soluble organic nitrogen(WSON)plays an important role in atmospheric chemistry and climatic change.However,few studies have focused on WSON in size-segregated particles.In this study,size-segregated particle samples in the size ranges of<0.49μm,0.49–0.95μm,0.95–1.5μm,1.5–3.0μm,3.0–7.2μm,7.2–10μm were collected in Guangzhou,China from September 2014 to July 2015 by a high-volume sampler.Samples were analyzed for water-soluble total nitrogen(WSTN),WSON and and water-soluble inorganic ions(WSIN).The concentrations of WSON in each size range showed a similar seasonal trend with higher concentrations in autumn and winter and lower concentrations in spring and summer.The seasonal average concentrations of WSON in PM_3 ranged from 1.15 to 2.62μg/m~3,contributing to 63%–71%of the WSON in PM_(10).The concentrations of WSON in particles<3μm exhibited a unimodal distribution in four seasons,enriching in the 0.49–0.95μm particles.The principal component analysis(PCA)/absolute principal component scores(APCS)analysis showed that WSON can be mainly attributed to the burning of local fossil fuels in particles<0.49μm,to construction dust and photochemical oxidation leading to its secondary formation in 0.49–0.95μm particles;and to photochemical oxidation leading to secondary formation alone in 0.95–1.5μm particles.Our research improves our understanding of the environmental geochemical processes of organic nitrogen compounds.
引文
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