长三角地区全氟温室气体本底特征及来源

采用位于长三角地区的临安区域大气本底站罐采样获得的全氟温室气体（PFCs、SF₆、NF₃、SO₂F₂）浓度,分析2011~2020年该地区大气中全氟温室气体的浓度分布特征和变化趋势.结果显示,临安站绝大部分全氟温室气体的浓度均呈现逐年升高的变化趋势,至2020年长三角地区全氟温室气体本底浓度分别达到（86.30±0.52）×10^-12（CF₄）、（5.03±0.00）×10^-12（C₂F₆）、（0.70±0.01）×10^-12（C₃F₈）、（1.82±0.00）×10^-12（c-C₄F₈）、（10.44±0.01）×10^-12（SF₆）、（2.36±0.04）×10^-12（NF₃）、（2.61±0.05）×10^-12（SO₂F₂）.长三角地区大部分全氟温室气体的本底浓度与全球本底值接近.通过对临安站全氟温室气体污染浓度的潜在源贡献作用（PSCF）和浓度权重轨迹（CWT）分析显示,临安站全氟化碳PFCs （CF₄、C₄F₁₀、C₂F₆、C₃F₈、c-C₄F₈）的潜在源区主要包括山东、江苏、安徽、上海、浙江中北部和江西东北部地区,NF₃、SF₆、SO₂F₂的潜在源区则集中在江苏中南部、上海、浙北地区.     

Degradation of duloxetine: Identification of transformation products by UHPLC-ESI(+)-HRMS/MS, in silico toxicity and wastewater analysis

Duloxetine (DUL), an antidepressant drug, has been detected in surface water and wastewater effluents, however, there is little information on the formation of its transformation products (TPs). In this work, hydrolysis, photodegradation (UV irradiation) and chlorination experiments were performed on spiked distillated water, under controlled experimental conditions to simulate abiotic processes that can occur in the environment and wastewater treatment plants (WWTPs). Eleven TPs, nine from reaction with UV light and two from chlorine contact, were formed and detected by ultra-high performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry, and nine of them had their chemical structures elucidated upon analyses of their fragmentation patterns in MS/MS spectra. The formation and degradation of the TPs were observed. The parent compound was completely degraded after 30?min in photodegradation and after 24?hr in chlorination. Almost all TPs were completely degraded in the experiments. The ecotoxicity and mutagenicity of the TPs were predicted based on several in silico models and it was found that a few of these products presented more ecotoxicity than DUL itself and six TPs showed positive mutagenicity. Finally, wastewater samples were analyzed and DUL and one TP, possibly formed by chlorination process, were detected in the effluent, which showed that WWTP not only did not remove DUL, but also formed a TP.     

Characterization of particulate matter from diesel passenger cars tested on chassis dynamometers

Emission characterization of particle number as well as particle mass from three diesel passenger cars equipped with diesel particulate filter(DPF), diesel oxidation catalyst(DOC)and exhaust gas recirculation(EGR) under the vehicle driving cycles and regulatory cycle.Total particle number emissions(PNEs) decreased gradually during speed-up of vehicle from 17.3 to 97.3 km/hr. As the average vehicle speed increases, the size-segregated peak of particle number concentration shifts to smaller size ranges of particles. The correlation analysis with various particulate components such as particle number concentration(PNC),ultrafine particle number concentration(UFPNC) and particulate matter(PM) mass was conducted to compare gaseous compounds(CO, CO_2, HC and NOx). The UFPNC and PM were not only emitted highly in Seoul during severe traffic jam conditions, but also have good correlation with hydrocarbons and NOxinfluencing high potential on secondary aerosol generation. The effect of the dilution temperature on total PNC under the New European Driving Cycle(NEDC), was slightly higher than the dilution ratio. In addition, the nuclei mode(DP: ≤ 13 nm) was confirmed to be more sensitive to the dilution temperature rather than other particle size ranges. Comparison with particle composition between vehicle speed cycles and regulatory cycle showed that sulfate was slightly increased at regulatory cycle, while other components were relatively similar. During cold start test, semivolatile nucleation particles were increased due to effect of cold environment. Research on particle formation dependent on dilution conditions of diesel passenger cars under the NEDC is important to verify impact on vehicular traffic and secondary aerosol formation in Seoul.     

浙江北部一次爆发式发展重度大气污染的气象特点和成因

基于全国空气质量指数和PM_(2.5)监测、常规气象观测、浙江省6种主要大气污染物和自动气象监测、宁波镇海激光雷达、美国国家环境预报中心GDAS和欧洲中期天气预报中心ERA-interim再分析等多种资料,对2017年12月30日―2018年1月1日浙江北部一次爆发式发展大气污染事件气象特点及成因进行分析,应用HYSPLIT4模式进行粒子后向轨迹分析.结果表明:PM_(10)和PM_(2.5)质量浓度在浙江省表现出明显的爆发性增长和自西北向东南传输的特征,污染程度自浙北向浙中、浙南逐渐减轻,重度污染时浙北大范围出现2000 m以下的重度霾,污染粒子主要来自上游的安徽和江苏省.大气污染爆发式发展与冷空气有关,1000 m以下边界层内冷空气偏弱,但足以将盛行风改变为西北风,是污染物粒子输送的动力条件,污染粒子集中在该层内,层内没有下沉运动,因此水平风场对污染事件爆发有决定性作用;1000 m以上层次冷平流表现明显,且伴有下沉运动,抑制了边界层粒子的垂直扩散,对污染事件的发展和维持有间接影响.激光雷达的消光系数变化不仅与污染物粒子浓度变化有关,还与气象条件密切相关.污染物粒子质量浓度通量散度的变化对预报粒子浓度的增减有较好的参考作用.     

鼎湖山PM2.5 中水溶性离子浓度特征分析

为研究珠江三角洲背景区域大气气溶胶中水溶性离子的特征及其来源,于2007年1月～2008年12月,在鼎湖山利用大流量滤膜采样器采集PM2.5样品,并用离子色谱(IC)分析其中的水溶性离子成分含量.结果表明,PM2.5中总水溶性离子年平均浓度为(36.3±16.4)μg.m-3.其中,3种主要离子SO24-、NH4+和NO3-占总离子浓度的89%;夏季受到来自海洋气团的影响,Na+和Cl-相关性明显增强,相关系数R2为0.91;NO3-/SO24-的平均值为0.32,表明固定源对鼎湖山地区污染的贡献更大;PM2.5中Σ阳离子电荷/Σ阴离子电荷的变化范围为0.44～2.59,平均值是1.03,水溶性离子电荷基本平衡.     

瓦斯浓度区间预测的灰色聚类与高斯过程模型

为有效分析矿井瓦斯监测数据,以实现准确、可靠的瓦斯浓度预测,基于灰色关联聚类分析与高斯过程回归模型,研究瓦斯浓度时间序列分析与预测的方法。以预测有效度为预测精度的评估指标来动态确定重构瓦斯浓度时间序列样本空间的维数;应用灰色关联分析方法将瓦斯浓度时间序列划分成若干样本集,将其中具有关联特征的样本作为虚拟变量进行预测以消除因随机、不确定因素干扰而引起的预测误差;应用高斯过程回归模型实现瓦斯浓度区间预测,将预测结果表示成一个具有较高可信度的取值区间,以此表达对未来一段时间内瓦斯浓度动态变化情况的预测。实例分析表明:预测结果准确、可靠,能够较好地反映瓦斯浓度的实际变化状况。     

基于HHT方法的矿井瓦斯体积分数预测

为有效分析煤矿瓦斯监测数据以实现较准确的瓦斯浓度预测,研究应用希尔伯特-黄变换(HHT)方法进行瓦斯浓度时间序列分析与预测的方法。应用经验模态分解(EMD)方法将瓦斯浓度时间序列分解成不同频率的固有模态函数(IMF)分量的叠加,以获取瓦斯浓度时间序列的瞬时特征;通过Hilbert变换求得各IMF分量的瞬时频率,依据各IMF分量瞬时频率的均值将分解得到的IMF划分成较高频和低频2类新的分量,选取适合于各分量特征的预测模型分别进行预测,以消除局部随机性对预测精度的影响,结合自回归(AR)、径向基函数(RBF)神经网络和支持向量机(SVM)3种预测模型实现瓦斯浓度预测。实例分析表明:应用该方法所得预测结果比较准确,降低了预测复杂度,提高了预测精度。     

可燃气体空间置换限值研究

在全面解析三元组分图构成要素和含义的基础上,分析可燃物质设备投用和停用过程中惰化置换的机理和浓度限值。可燃气体空间置换限值包括设备投用惰化置换时氧气的最高容许浓度(ISOC)和设备停用惰化置换时可燃气体的最高容许浓度(OSFC),二者可由试验和公式计算2种方式获得。与目前惰化置换时通常参照的限制氧浓度(LOC)、燃烧下限(LFL)等参数相比,ISOC和OSFC值可以更准确地表征惰化置换时临界浓度的意义。通过对部分可燃物质的ISOC和OSFC试验值及计算值进行对比分析,证明以LOC为依据计算出的ISOC和OSFC值与试验值具有更高的符合性;指出目前国内惰化置换浓度控制值采用统一规定值这一方式的不足;证明合理利用LFL,LOCI,SOC,OSFC等参数开展可燃气体密闭空间置换限值研究的科学合理性。     

基于通量守恒原理的水质监测非统计不确定性研究

水环境动态监测过程中,结果存在非统计不确定性.以北京市密云水库曹家路小流域安达木河部分汇流河段为研究对象,结合水质和流量数据,分析了单次监测中水质存在的偶然误差下限值,去除其粗大值,以其均值表征动态监测过程中的非统计不确定性.由于研究的汇流河段尺度小,水流经过时间短,迁移转化过程可以忽略,建立的基于通量守恒原理的非统计...     

北京密闭式垃圾清洁站内外大气监测与安全距离

以北京海淀区为例,对密闭式垃圾清洁站的分布及内外部的大气状况进行了监测并运用大气扩散模型探讨了垃圾清洁站的安全防护距离.结果表明:海淀区垃圾清洁站的分布不均衡;所有垃圾清洁站内外的大气污染物中,H2S、NH3、S02、N02、二硫化碳、苯乙烯、TSP、CO等指标均符合中国相关排放标准;转运站内部三甲胺、甲硫醇、甲硫醚、...