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Chemical composition and mass size distribution of PM1 at an elevated site in central east China

机译:中国东部升高部位PM1的化学成分和质量分布

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Size-resolved aerosol chemical compositions were measured continuously for 1.5 years from June 2010 to January 2012 with an aerosol mass spectrometer (AMS) to characterize the mass and size distributions (MSDs) of major chemical components in submicron particles (approximately PM1) at Mountain Tai (Mt. Tai), an elevated site in central east China. The annual mean mass concentrations of organic, sulfate, nitrate, ammonium, and chloride were 11.2, 9.2, 7.2, 5.8, and 0.95 μg m?3, respectively, which are much higher than those at most mountain sites in the USA and Europe, but lower than those at the nearby surface rural sites in China. A clear seasonality was observed for all major components throughout the study, with low concentration in fall and high in summer, and is believed to be caused by seasonal variations in planetary boundary layer (PBL) height, near surface pollutant concentrations and regional transport processes. Air masses were classified into categories impacted by PBL, lower free troposphere (LFT), new particle formation (NPF), in-cloud processes, and polluted aerosols. Organics dominated the PM1 mass during the NPF episodes, while sulfate contributed most to PM1 in cloud events. The average MSDs of particles between 30 and 1000 nm during the entire study for organics, sulfate, nitrate, and ammonium were approximately log-normal with mass median diameters (MMDs) of 539, 585, 542, and 545 nm, respectively. These values are slightly larger than those observed at ground sites within the North China Plain (NCP), likely due to the relative aged and well-mixed aerosol masses at Mt. Tai. There were no obvious differences in MMDs during the PBL, LFT, in-cloud and polluted episodes, but smaller MMDs, especially for organics, were observed during the NPF events. During the PBL, NPF, and polluted episodes, organics accounted for major proportions at smaller modes, and reached 70% at 100–200 nm particles in the polluted events. In cloud episodes, inorganics contributed 70% to the whole size range dominated by sulfate, which contributed 40% to small particles (100–200 nm), while organics occupied 20%, indicating that sulfate is a critical chemical component in cloud formation. Seven clusters of air masses were classified based on 72 h back-trajectory analysis. The majority of the regionally dispersed aerosols were found to be contributed from short distance mixed aerosols, mostly originated from the south with organics and sulfate as major components. Air masses from long range transport always brought clean and dry aerosols which resulted in low concentrations at Mt. Tai. AMS-PMF (positive matrix factorization) was employed to resolve the subtype of organics. Oxygenic organics aerosols (OAs) occupied 49, 56, 51, and 41% of OAs in the four seasons respectively, demonstrating that most OA were oxidized in summer due to strong photochemical reactions. Biomass burning OAs (BBOAs) accounted for 34% of OA in summer, mainly from field burning of agriculture residues, and coal combustion OAs (CCOAs) accounted for 22% of OA in winter from heating.
机译:从2010年6月到2012年1月的尺寸分解的气溶胶化学成分用气溶胶质谱仪(AMS)在2010年6月至2012年1月开始测量1.5岁,以表征山地山丘脑颗粒(约PM1)中的主要化学成分的质量和尺寸分布(MSDS) (MT. TAI),中东华东地区的高架网站。有机,硫酸盐,硝酸盐,铵和氯的年平均质量浓度分别为11.2,9.2,7.2,5.8和0.95μgm≤3,高于美国和欧洲最多的山地地点的那些但低于中国附近的地表农村地区的地区。在整个研究中的所有主要组件中观察到清晰的季节性,夏季跌幅低,较低,被认为是由行星边界层(PBL)高度,近地表污染物浓度和区域运输过程中的季节变化引起的。空气群众被分类为PBL,下游离的对流层(LFT),新粒子形成(NPF),云内工艺和污染气溶胶的类别。有机物在NPF集中占主导地位PM1质量,而硫酸盐在云事件中向PM1贡献最多。在整个研究期间30至1000nm之间的平均颗粒MSDS,硫酸盐,硝酸铵和铵的全部研究分别与539,585,542和545nm的质量中值直径(MMD)近似。这些值略大于北中国平原(NCP)的地面位点观察的值,可能是由于Mt. Tai的相对老化和混合良好的气溶胶群体。在PBL,LFT,云和污染的发作期间,MMDS没有明显的差异,但在NPF事件期间观察到较小的MMD,特别是对于有机物。在PBL,NPF和污染的发作期间,有机物占较小模式的主要比例,并在污染事件中以100-200nm粒子达到70%。在云剧集中,无机贡献了70%,硫酸盐主导的整个尺寸范围贡献了40%至小颗粒(100-200nm),而有机体占用20%,表明硫酸盐是云形成的关键化学成分。基于72小时的返回轨迹分析,分类了七个空气群集。发现大多数区域分散的气溶胶是从短距离混合气溶胶的贡献,主要来自南部有机物和硫酸盐作为主要组分。远程运输的空气群众始终带来清洁干燥的气溶胶,导致Mt. Tai浓度低。 AMS-PMF(正基质分解)用于解决有机物的亚型。含氧有机物气溶胶(OAS)分别占用49,56,51和41%的OAS,分别在四季中展示,由于强烈的光化学反应,大多数OA在夏季被氧化。生物量燃烧OAS(BBOAS)占夏季的34%的OA,主要来自农业残留物的野外燃烧,煤炭燃烧OAS(CCOAS)占冬季加热中OA的22%。

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