Cao Fang, Zhang Shi-Chun, Kawamura Kimitaka, Liu Xiaoyan, Yang Chi, Xu Zufei, Fan Meiyi, Zhang Wenqi, Bao Mengying, Chang Yunhua, Song Wenhuai, Liu Shoudong, Lee Xuhui, Li Jun, Zhang Gan, Zhang Yan-Lin
Yale-NUIST Center on Atmospheric Environment, Nanjing University of Information Science and Technology, Nanjing 10044, China; Key Laboratory of Meteorological Disaster Ministry of Education (KLME) & Joint International Research Laboratory of Climate and Environment Change (ILCEC) & Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters (CIC-FEMD), Nanjing University of Information Science and Technology, Nanjing 210044, China.
Northeast Institute of Geography and Agroecology, Chinese Academy of Sciences, 4888 Shengbei Road, Changchun 130102, China.
Environ Pollut. 2017 Dec;231(Pt 1):654-662. doi: 10.1016/j.envpol.2017.08.045. Epub 2017 Aug 29.
Fine particulate matter (PM2.5) samples were collected using a high-volume air sampler and pre-combusted quartz filters during May 2013 to January 2014 at a background rural site (4735 N, 13331 E) in Sanjiang Plain, Northeast China. A homologous series of dicarboxylic acids (C-C) and related compounds (oxoacids, α-dicarbonyls and fatty acids) were analyzed by using a gas chromatography (GC) and GC-MS method employing a dibutyl ester derivatization technique. Intensively open biomass-burning (BB) episodes during the harvest season in fall were characterized by high mass concentrations of PM2.5, dicarboxylic acids and levoglucosan. During the BB period, mass concentrations of dicarboxylic acids and related compounds were increased by up to >20 times with different factors for different organic compounds (i.e., succinic (C) acid > oxalic (C) acid > malonic (C) acid). High concentrations were also found for their possible precursors such as glyoxylic acid (ωC), 4-oxobutanoic acid, pyruvic acid, glyoxal, and methylglyoxal as well as fatty acids. Levoglucosan showed strong correlations with carbonaceous aerosols (OC, EC, WSOC) and dicarboxylic acids although such good correlations were not observed during non-biomass-burning seasons. Our results clearly demonstrate biomass burning emissions are very important contributors to dicarboxylic acids and related compounds. The selected ratios (e.g., C/C, maleic acid/fumaric acid, C/ωC, and C/levoglucosan) were used as tracers for secondary formation of organic aerosols and their aging process. Our results indicate that organic aerosols from biomass burning in this study are fresh without substantial aging or secondary production. The present chemical characteristics of organic compounds in biomass-burning emissions are very important for better understanding the impacts of biomass burning on the atmosphere aerosols.
2013年5月至2014年1月期间,在中国东北三江平原的一个农村背景站点(北纬47°35′,东经133°31′),使用大容量空气采样器和预燃烧石英滤膜采集了细颗粒物(PM2.5)样本。采用气相色谱(GC)和GC-MS方法,运用二丁酯衍生化技术,分析了一系列同系二元羧酸(C2-C12)及相关化合物(含氧酸、α-二羰基化合物和脂肪酸)。秋季收获季节强烈的露天生物质燃烧(BB)事件,其特征是PM2.5、二元羧酸和左旋葡聚糖的质量浓度很高。在BB期间,二元羧酸及相关化合物的质量浓度因不同有机化合物的不同因素而增加高达20倍以上(即琥珀酸(C4)>草酸(C2)>丙二酸(C3))。还发现其可能的前体如乙醛酸(ωC1)、4-氧代丁酸、丙酮酸、乙二醛和甲基乙二醛以及脂肪酸的浓度也很高。左旋葡聚糖与碳质气溶胶(OC、EC、WSOC)和二元羧酸显示出很强的相关性,尽管在非生物质燃烧季节未观察到这种良好的相关性。我们的结果清楚地表明,生物质燃烧排放是二元羧酸及相关化合物的非常重要的贡献源。所选的比率(例如,C2/C3、马来酸/富马酸、C2/ωC1和C2/左旋葡聚糖)被用作有机气溶胶二次形成及其老化过程的示踪剂。我们的结果表明,本研究中生物质燃烧产生的有机气溶胶是新鲜的,没有大量老化或二次生成。生物质燃烧排放中有机化合物的当前化学特征对于更好地理解生物质燃烧对大气气溶胶的影响非常重要。