基于FBM法追踪秦皇岛海域赤潮迁移扩散

在Delft3D-FLOW模型模拟水动力的基础上,基于FBM粒子追踪法建立和验证赤潮迁移扩散模型.模拟了秦皇岛海域潮流和风生流,分析了风生流对赤潮迁移扩散的作用,对比分析了FBM法、拉格朗日法和常规布朗运动法在赤潮迁移扩散模拟中的特性,测试了模型Hurst指数的敏感性并得出其在赤潮模拟中的合理取值范围.主要结论为：①秦皇岛海域的赤潮主要随潮流的涨落而往复移动,一个涨落潮周期内赤潮的净迁移距离较小;②秦皇岛海域夏季潮流较弱,但风对赤潮迁移具有一定影响,易产生东北向风生流,导致赤潮更易往东北方向迁移;③Hurst指数较明显地影响粒子云的扩散范围,Hurst指数取0.80±0.03能比较真实地模拟秦皇岛海域赤潮的迁移扩散;④FBM法可模拟赤潮的non-Fickian扩散现象,使其模拟的粒子云扩散范围和分布形状明显优于拉格朗日法和常规布朗运动法.     

Key features of new particle formation events at background sites in China and their influence on cloud condensation nuclei

New particle formation (NPF) event at multi rural sites in China Identifying the characteristics of NPF event Comparing NPF event between clean and polluted conditions Quantifying contribution to the cloud condensation nuclei Implication of climate and air quality Long-term continuous measurements of particle number size distributions with mobility diameter sizes ranging from 3 to 800 nm were performed to study new particle formation (NPF) events at Shangdianzi (SDZ), Mt. Tai (TS), and Lin’an (LAN) stations representing the background atmospheric conditions in the North China Plain (NCP), Central East China (CEC), and Yangtze River Delta (YRD) regions, respectively. The mean formation rate of 3-nm particles was 6.3, 3.7, and 5.8 cm⁻³·s⁻¹, and the mean particle growth rate was 3.6, 6.0, and 6.2 nm·h⁻¹ at SDZ, TS, and LAN, respectively. The NPF event characteristics at the three sites indicate that there may be a stronger source of low volatile vapors and higher condensational sink of pre-existing particles in the YRD region. The formation rate of NPF events at these sites, as well as the condensation sink, is approximately 10 times higher than some results reported at rural/urban sites in western countries. However, the growth rates appear to be 1–2 times higher. Approximately 12%–17% of all NPF events with nucleated particles grow to a climate-relevant size (>50 nm). These kinds of NPF events were normally observed with higher growth rate than the other NPF cases. Generally, the cloud condensation nuclei (CCN) number concentration can be enhanced by approximately a factor of 2–6 on these event days. The mean value of the enhancement factor is lowest at LAN (2–3) and highest at SDZ (~4). NPF events have also been found to have greater impact on CCN production in China at the regional scale than in the other background sites worldwide.     

西安市大气颗粒物数浓度分布及典型天气条件特征变化

利用2013年3月到2014年12月期间西安市大气中0.25～32μm颗粒物监测数据和同期气象参数、散射消光系数等数据,分析了大气颗粒物数浓度分布及典型天气条件下变化特征.结果表明:采样期间西安市大气颗粒物平均数浓度为206.27个/cm3, 99%以上为<1μm的颗粒物数.大气颗粒物数浓度冬季最高,其次为秋、夏和春季,分别为267.66、231.31、141.82和135.77个/cm3.四季的数浓度低值均出现在18:00左右,之后数浓度上升,且晚上高于白天,冬季6:00左右达到峰值,夏季的昼夜差最小,秋季最大.春夏秋冬的大气颗粒物数浓度与散射消光系数的Pearson相关系数分别为0.756、0.702、0.411、0.377.大气颗粒物数浓度在沙尘天气发生前、中、后会升高、下降和再下降,霾天气出现前、后会升高和下降;高温干燥天气下,大气颗粒物数浓度相对较低;降雨对大气颗粒物的清除作用明显,但降雨后大气颗粒物数浓度又很快回升.     

黄山大气气溶胶新粒子生长特性观测分析

利用2012年9月22日~10月28日黄山地区大气气溶胶、二氧化硫和臭氧观测数据,结合气象数据,分析气溶胶新粒子的生成-增长特征.分析发现,在33个有效观测日中,有新粒子生成-增长的观测日占总数的18.2%,其中晴天的发生频率为37.5%,新粒子生成-增长都开始于晴天上午,与无新粒子观测日相比,太阳辐射量、风速、SO2及O3浓度较高,环境温度和相对湿度较低.气溶胶新粒子的增长具有由小及大的特点,核模态气溶胶粒子(10~20nm)数浓度最先增加,爱根核模态粒子(20~50nm)数浓度随着时间推移逐渐增大,但浓度峰值依次下降,平均增长率为3.58nm/h. SO2浓度先于核模态气溶胶数浓度到达峰值,其氧化后的产物H2SO4为新粒子的核化提供前体物,并且参与新粒子的增长过程,当SO2浓度较低时,不会发生新粒子生长事件.     

正丁醇对柴油机颗粒组分与形貌特征的影响

为探讨柴油机燃用正丁醇-柴油混合燃料降低颗粒排放的机理,采用热重分析仪与场发射扫描电子显微镜,重点对正丁醇-柴油混合燃料燃烧的颗粒形貌特征进行研究,分析了颗粒的组分、微观结构以及粒径分布随w(正丁醇)的变化规律. 结果表明:正丁醇-柴油混合燃料燃烧的颗粒呈团簇状结构,随着w(正丁醇)的增加,团聚程度逐渐提高,排列结构更加紧密;颗粒的粒径逐渐减小,柴油、B5、B10〔B5、B10是指w(正丁醇)分别为5%、10%的正丁醇-柴油混合燃料〕燃烧的颗粒平均粒径分别为1.43、0.85、0.52 μm;颗粒中的主要成分为碳烟,其质量分数约为60%,随着w(正丁醇)的增加,碳烟和可溶有机物组分的质量分数有所增加,硫酸盐、金属等不易挥发组分以及金属元素的质量分数逐渐减少. 研究显示,添加正丁醇,可促进颗粒转化、改善颗粒的氧化过程,使颗粒向小粒径方向移动;由于颗粒中可溶有机物组分含量增加,因此提高了颗粒在碰撞过程中凝并的概率,致使颗粒的团聚程度增加.      

Effects of molecular weight and concentration of carboxymethyl cellulose on morphology of hydroxyapatite nanoparticles as prepared with one-step wet chemical method

Nano-sized apatite particles (nAP) synthesized with carboxymethyl cellulose (CMC) have shown great application potentials in in situ heavy metal remediation. However, differences in CMC’s properties effects on the size of nAP produced are not well understood. In this paper, two types of CMC, with respective molecular weights (MW) of ～120000 and ～240000 Dalton or respective polymerization degrees of 500 (CMC-500) and 1050 (CMC-1050), were studied in a concentration range of 0.05%–0.5% (w/w) for nAP synthesis. Morphology of the particles was characterized with transmission electron microscopy (TEM). Results showed that 0.05% CMC-500 solution gave an average particle size of 148.7±134.9 nm, 0.25% CMC-500 solution produced particles of 21.8±20.4 nm, and, 0.5% CMC-500 solution contained particles of 15.8±7.7 nm. In comparison, 0.05% CMC-1050 solution produced nanoparticles of 6.8±3.2 nm, 0.25% CMC-1050 produced smaller nAP of 4.3±3.2 nm, and 0.5% CMC-1050 synthesized the smallest nanoparticles in this study, with an average diameter of 3.0±2.1 nm. Chemical composition of the products was identified with X-ray diffraction (XRD) as pure hydroxyapatite. Interactions between nAP and CMC were discussed with help of attenuated total reflection Fourier transform infrared (ATRFTIR) spectroscopic data. This study showed that CMC at higher concentration as well as higher MW facilitated to produce finer nanoparticles, showing that nAP size could be manipulated by selecting appropriate CMC MW and/or applying appropriate CMC concentration.     

四川乡村点新粒子生成特征及其对云凝结核数浓度的贡献

为揭示成渝地区大气复合污染成因,选择乡村点资阳站的冬季,实测了颗粒物数浓度及其粒径谱分布、云凝结核(CCN),在二氧化硫、光解速率(JO1D)实测值基础上估算了新粒子生成的重要前体物气态硫酸的浓度.2012年12月5日到2013年1月5日观测期间,3~582nm颗粒物数浓度水平较高,平均值为(16072±9713)cm-3.颗粒物数谱分布呈现以积聚模态为主体的特征,占总颗粒物数浓度的46%,此比值高于我国北京、上海、广州等城市和珠江三角洲及长江三角洲的乡村点和背景点.在较高颗粒物凝结汇(CS)水平下[(4.3±3.6)×10-2s-1],甄别出7次新粒子生成(NPF)事件,占观测天数的23%.NPF事件发生时,颗粒物生成速率与增长速率分别为(5.2±1.4)cm-3s-1,(3.6±2.5)nm/h. NPF事件对CCN数浓度有明显贡献,NPF发生后CCN数浓度平均增长19%.     

Fe-Ni-TiO2/AC粒子电极的制备及可见光光电催化协同降解RhB

制备Fe-Ni-TiO2/AC粒子电极,应用于可见光助三维电极/电Fenton(Vis-3D/EF)光电催化体系中,以RhB为目标污染物,研究了可见光光电催化对RhB的协同降解.实验优化了Fe-Ni-TiO2/AC粒子电极的制备条件,并与活性炭粒子电极、活性炭负载TiO2粒子电极在Vis-3D/EF体系中的光电催化性能进行对比,结果表明:TiO2浸渍液浓度为2g/L,Fe-Ni掺杂比为5:5,Fe:Ni:TiO2物质的量比为0.5:0.5:100的条件下制备的粒子电极在Vis-3D/EF体系中表现出最优的光电催化性能,60min对RhB的去除率达92.58%,优于活性炭粒子电极和活性炭负载TiO2粒子电极.自制粒子电极在Vis-3D/EF体系比在3D/EF体系对RhB的去除率提高29.46%,表现出明显的光催化和三维电极/电Fenton协同处理效果,协同指数为1.18,说明了自制粒子电极应用在Vis-3D/EF组合技术中,实现对RhB的可见光光电协同降解是可行的.     

典型电子垃圾拆解区二噁英污染特征、相分配及暴露风险

选取南方某典型电子垃圾拆解区不同作业区为研究对象,重点研究了拆解地大气中二噁英的污染特征、气相-颗粒相分配及呼吸暴露风险。通过对5个采样点（包括1个背景点）的研究发现,电子垃圾拆解作业区颗粒相ΣPCDD/Fs的质量浓度为：20.64-56.14 pg·m^-3,毒性当量为：I-TEQ 0.293-1.490 pg·m^-3;气相ΣPCDD/Fs的质量浓度为：3.861-19.29 pg·m^-3,毒性当量为：I-TEQ 0.384-2.150 pg·m^-3。背景点大气中二噁英浓度相对较低,颗粒相和气相样品中质量浓度值分别为：3.734 pg·m^-3和2.637 pg·m^-3,毒性当量仅为I-TEQ 0.176-0.267 pg·m^-3;要明显低于电子垃圾拆解区。基于污染物气相-颗粒相分配系数与蒸汽压的关系对二噁英的气-固分配行为研究显示,除了拆解混合作业区有较好的分配系数（-0.64）外,其它监测点位二噁英的气-固平衡状态较弱（-0.27--0.03）,更多的是以低分子量的单体化合物赋存于气相样品中。对拆解区二噁英呼吸暴露风险研究结果表明,儿童呼吸暴露风险要高于成年人;同时无论是儿童还是成年人,其二噁英的呼吸暴露量均要高于国内外城市报道的二噁英人体呼吸暴露量,说明本次监测的电子垃圾拆解区存在的潜在健康风险不容忽视。     

Investigation on sampling artifacts of particle associated PAHs using ozone denuder systems

Polycyclic aromatic hydrocarbons （PAHs） are complex organic compounds which are identified as significant carcinogenic to human health. PAHs （mainly in particle phase） are susceptible to atmospheric oxidant gases, especially ozone, nitrogen oxides （NOx）, hydroxyl radical （OH）, and could be degraded on filters during sampling process, leading to an underestimation of ambient PAH concentrations. The goal of this work was to investigate particle associated PAHs sampling artifacts caused by ozone in summer of Beijing. Comparative sampling systems were operated simultaneously during the whole campaign, one with activated carbon ozone denuder, the other being set as conventional sampling system. Activated carbon denuder was testified to be highly efficient to eliminate ozone from air stream. In general, nine particle-bound PAHs observed from conventional sampler were all lower than those from ozone denuder system. The total PAHs （particle phase） concentration was averagely underestimated by 35.9% in conventional sampling procedure. Benzo[a]pyrene （BaP） had the highest percentage of mass loss. founded to have influences Ambient temperature was on PAHs sampling artifacts. High temperature can increase loss of particle associated PAHs during sampling.