Compositions and sources of organic acids in fine particles (PM2.5) over the Pearl River Delta region, south China

Organic acids as important constituents of organic aerosols not only influence the aerosols' hygroscopic property, but also enhance the formation of new particles and secondary organic aerosols. This study reported organic acids including C14–C32fatty acids, C4–C9dicarboxylic acids and aromatic acids in PM2.5collected during winter 2009 at six typical urban, suburban and rural sites in the Pearl River Delta region. Averaged concentrations of C14–C32fatty acids, aromatic acids and C4– C9 dicarboxylic acids were 157, 72.5 and 50.7 ng/m3, respectively. They totally accounted for 1.7% of measured organic carbon. C20–C32fatty acids mainly deriving from higher plant wax showed the highest concentration at the upwind rural site with more vegetation around, while C14–C18fatty acids were more abundant at urban and suburban sites, and dicarboxylic acids and aromatic acids except 1,4-phthalic acid peaked at the downwind rural site. Succinic and azelaic acid were the most abundant among C4–C9dicarboxylic acids, and 1,2-phthalic and 1,4-phthalic acid were dominant aromatic acids. Dicarboxylic acids and aromatic acids exhibited significant mutual correlations except for 1,4-phthalic acid, which was probably primarily emitted from combustion of solid wastes containing polyethylene terephthalate plastics. Spatial patterns and correlations with typical source tracers suggested that C14–C32fatty acids were mainly primary while dicarboxylic and aromatic acids were largely secondary. Principal component analysis resolved six sources including biomass burning, natural higher plant wax, two mixed anthropogenic and two secondary sources; further multiple linear regression revealed their contributions to individual organic acids. It turned out that more than 70% of C14–C18fatty acids were attributed to anthropogenic sources, about 50%–85% of the C20–C32fatty acids were attributed to natural sources, 80%–95% of dicarboxylic acids and 1,2-phthalic acid were secondary in contrast with that 81% of 1,4-phthalic acid was primary.     

Characteristics of atmospheric particles and heavy metals in winter in Chang-Zhu-Tan city clusters, China

To understand the pollution characteristics of atmospheric particles and heavy metals in winter in Chang-Zhu-Tan city clusters, China, total suspended particulate(TSP) and PM10samples were collected in cities of Changsha, Zhuzhou and Xiangtan from December 2011 to January 2012, and heavy metals of Cd, Pb, Cr, and As were analyzed. It shows that the average TSP concentration in Changsha, Zhuzhou and Xiangtan were(183 ± 73),(201 ± 84) and(190 ± 66) μg/m3respectively, and the average PM10 were(171 ± 82),(178 ± 65) and(179 ± 55) μg/m3respectively. The lowest TSP and PM10concentrations occurred at the background Shaping site of Changsha. The average ratio of ρ(PM10)/ρ(TSP) was 91.9%, ranging from 81.3% to 98.9%. Concerning heavy metals, in TSP samples, the concentration of Cr, As, Cd and Pb were 28.8–56.5, 18.1–76.3, 3.9–26.1 and 148.0–460.9 ng/m3, respectively, while in PM10samples, were 16.4–42.1, 15.5–67.9, 3.3–22.2 and 127.9–389.3 ng/m3, respectively. The enrichment factor of Cd was the highest, followed by Pb and As, while that of Cr was the lowest.     

杭州灰霾天气超细颗粒浓度分布特征

利用快速迁移率粒径谱仪(FMPS)对杭州2013年12月6～11日连续灰霾天气和灰霾消退过程超细颗粒进行监测,分析颗粒物浓度变化和粒径谱分布特征及其与气象的相关性.结果表明,颗粒物日变化特征为夜晚数浓度较高,凌晨数浓度开始降低,08:00和18:00上下班高峰期出现一个小峰值,体现出明显的交通源峰值,表明交通排放对大气污染影响较大.灰霾天气下颗粒物最高数浓度达到8.0×104cm-3.粒径谱呈双峰分布,峰值粒径分别为15 nm和100 nm,粒径在100 nm附近的粒子占大多数,粒子以爱根核模态和积聚模态为主,平均数量中位径CMD(count medium diameter)为85.89 nm.而在灰霾消退过程,颗粒物数浓度降低,峰值粒径向小粒径演变,粒径在100 nm附近的粒子逐渐减少,核模态粒子增多,大于积聚模态,平均CMD为58.64 nm.气象因素中能见度和风力与数浓度主要呈负相关,相关系数R分别为-0.225和-0.229,相对湿度与数浓度正相关,相关系数R为0.271,冬季大气比较稳定,水平温度与数浓度的相关性较小.研究灰霾天气数浓度分布和气象因素的综合影响对其形成机制及控制有重要意义.     

模拟烹饪油烟的粒径分布与扩散

烹饪油烟颗粒物粒径分布与扩散特性研究有助于解析其对室内空气质量和居民健康的影响,采用电子低压撞击器(ELPI)实时监测了油烟机开启和关闭状态下,模拟烹饪油烟发生处和3 m外位置处,0.03~10μm范围内油烟颗粒数浓度和质量浓度随粒径分布.油烟颗粒主要以655 nm以下的细颗粒为主.油烟机能够显著降低室内油烟浓度,开启油烟机后,油烟发生处颗粒数浓度从2.8×106个·cm-3降低到2.3×105个·cm-3,PM2.5(空气动力学直径≤2.5μm的颗粒)质量浓度从85.9 mg·m-3降低到6.2 mg·m-3.油烟机对PM10的净化效率高于PM2.5.油烟迅速从发生处扩散到3 m外,无通风状态下,总颗粒数浓度衰减达65%,PM2.5质量浓度衰减达75%.计算流体动力学(CFD)模拟了油烟机对油烟PM2.5质量浓度场扩散分布影响.红外摄像仪监测了油烟温度场分布扩散,以扇形向外扩散,伴随着油烟温度梯度降低.     

EDTA优化纳米Pd/Fe对2,4-D的催化脱氯研究

采用EDTA优化纳米Pd/Fe催化脱氯水中2,4-二氯苯氧乙酸(2,4-D),并考察了EDTA投加浓度、pH、钯化率、温度等因素对2,4-D还原的影响.结果表明,EDTA的加入络合了纳米Pd/Fe在催化脱氯过程中生成的铁离子,抑制纳米Pd/Fe颗粒表面钝化层的形成,提高了体系的反应活性.适宜的EDTA浓度、低pH、高钯化率、低温等有利于2,4-D的还原脱氯.当EDTA浓度为25.0 mmol·L-1,纳米铁含量为1.0 g·L-1,初始pH=4.3、钯化率为0.5%,温度为25.0℃,搅拌速率为200 r·min~(-1)时,反应50 min,10.0 mg·L-1的2,4-D去除率及苯氧乙酸(PA)生成率均达到100%.     

Fe3O4/TiO2-H2O2非均相类Fenton体系对3，4-二氯三氟甲苯的降解

用Fe_3O_4/Ti O_2-H_2O_2体系对3,4-二氯三氟甲苯(3,4-DCBTE)进行降解反应研究,同时考察了pH值、催化剂投加量、H_2O_2投加量、温度等因素对3,4-DCBTE降解效率的影响.实验结果表明,Fe_3O_4/Ti O_2-H_2O_2非均相类Fenton体系对3,4-二氯三氟甲苯的处理效果极佳;并且在H_2O_2投加量为45.0 mg·L~(-1)、Fe_3O_4/TiO_2的物质的量比为1∶1、pH=3.0、温度为40.0℃的条件下反应效果最佳,去除率高达99.1%.同时从实验结果可以看出,pH在2.0~7.0范围内该体系对3,4-二氯三氟甲苯均有降解效果,说明该体系相比于传统的Fenton体系有较宽的pH适用范围.目标污染物的降解符合一级反应动力学,其发生反应所需的活化能为36.9 k J·mol~(-1).     

Sorption of polycyclic aromatic hydrocarbons (PAHs) to carbonaceous materials in a river floodplain soil

We report on sorption isotherm of phenanthrene (Phe) for river floodplain soil associated with carbonaceous materials, with particular attention being devoted to the natural loading of Phe. Our sorption experiments with original soil samples, size, and density sub-fractions showed that the light fraction had the highest sorption capacity comparable to low rank coals. In addition, the light fraction contributed most for the sorption of Phe in total soil samples. K_oc values for all fractions were in the same range, thus indicating that coal and coal-derived particles in all samples are responsible for the enhanced sorption for Phe. Sorption was strongly nonlinear and the combined partitioning and pore-filling model gave a better fit than the Freundlich sorption model. In addition, the spiked PAHs did not show the same behavior as the naturally aged ones, therefore the accessibility of indigenous background organic contaminants was reduced when coal and coal-derived particles are associated with the soils.     

Improvement of an efficient separation method for chemicals in diesel exhaust particles: analysis for nitrophenols

GOAL, SCOPE, AND BACKGROUND: Diesel exhaust is believed to consist of thousands of organic constituents and is a major cause of urban pollution. We recently reported that a systematic separation procedure involving successive solvent extractions, followed by repeated column chromatography, resulted in the isolation of vasodilatory active nitrophenols. These findings indicated that the estimation of the amount of nitrophenols in the environment is important to evaluate their effect on human health. The isolation procedure, however, involved successive solvent extractions followed by tedious, repeated chromatography, resulting in poor fractionation and in a significant loss of accuracy and reliability. Therefore, it was crucial to develop an alternative, efficient, and reliable analytical method. Here, we describe a facile and efficient acid-base extraction procedure for the analysis of nitrophenols. MATERIALS AND METHODS: Diesel exhaust particles (DEP) were collected from the exhaust of a 4JB1-type engine (ISUZU Automobile Co., Tokyo, Japan). Gas chromatography-mass spectrometry (GC-MS) analysis was performed with a GCMS-QP2010 instrument (Shimadzu, Kyoto, Japan). RESULTS: A solution of DEP in 1-butanol was extracted with aqueous NaOH to afford a nitrophenol-rich oily extract. The resulting oil was methylated with trimethylsilyldiazomethane and subsequently subjected to GC-MS analysis, revealing that 4-nitrophenol, 3-methyl-4-nitrophenol, 2-methyl-4-nitrophenol, and 4-nitro-3-phenylphenol were present in significantly higher concentrations than those reported previously. DISCUSSION: Simple acid-base extraction followed by the direct analysis of the resulting extract by GC-MS gave only broad peaks of nitrophenols with a poor detection limit, while the GC-MS analysis of the sample pretreated with (trimethylsilyl)diazomethane gave satisfactorily clear chromatograms with sharp peaks and with a significantly lowered detection limit (0.5 ng/ml, approximately 100 times). CONCLUSION: The present method involving an acid-base extraction, in situ derivatization, and GC-MS analysis has shown to be a simple, efficient, and reliable method for the isolation and identification of the chemical substances in DEP.     

Spatial & temporal variations of PM10 and particle number concentrations in urban air

The size of particles in urban air varies over four orders of magnitude (from 0.001 μm to 10 μm in diameter). In many cities only particle mass concentrations (PM10, i.e. particles <10 μm diameter) is measured. In this paper we analyze how differences in emissions, background concentrations and meteorology affect the temporal and spatial distribution of PM10 and total particle number concentrations (PNC) based on measurements and dispersion modeling in Stockholm, Sweden. PNC at densely trafficked kerbside locations are dominated by ultrafine particles (<0.1 μm diameter) due to vehicle exhaust emissions as verified by high correlation with NOx. But PNC contribute only marginally to PM10, due to the small size of exhaust particles. Instead wear of the road surface is an important factor for the highest PM10 concentrations observed. In Stockholm, road wear increases drastically due to the use of studded tires and traction sand on streets during winter; up to 90% of the locally emitted PM10 may be due to road abrasion. PM10 emissions and concentrations, but not PNC, at kerbside are controlled by road moisture. Annual mean urban background PM10 levels are relatively uniformly distributed over the city, due to the importance of long range transport. For PNC local sources often dominate the concentrations resulting in large temporal and spatial gradients in the concentrations. Despite these differences in the origin of PM10 and PNC, the spatial gradients of annual mean concentrations due to local sources are of equal magnitude due to the common source, namely traffic. Thus, people in different areas experiencing a factor of 2 different annual PM10 exposure due to local sources will also experience a factor of 2 different exposure in terms of PNC. This implies that health impact studies based solely on spatial differences in annual exposure to PM10 may not separate differences in health effects due to ultrafine and coarse particles. On the other hand, health effect assessments based on time series exposure analysis of PM10 and PNC, should be able to observe differences in health effects of ultrafine particles versus coarse particles.     

300MW燃煤锅炉机组超细颗粒聚并器的实验研究

为了解决燃煤锅炉烟气中超细颗粒难以脱除的问题,基于流体动力学原理设计了一种超细颗粒聚并器,并在300 MW燃煤锅炉机组电除尘器的前置烟道中进行了实验研究。结果表明,聚并器内部存在超细颗粒之间以及超细颗粒与大颗粒之间的相互聚集行为,从而使超细颗粒数量显著减少。例如,对于粒径在2.65和10.48μm以下的颗粒,其体积比例在聚并器出口分别减少了56.7%和62.3%,在电除尘器出口的粉尘浓度减少了26.34 mg/Nm3,这表明,基于流体动力学原理的聚并器对超细颗粒的聚并作用明显,具有良好的应用前景。