有机气溶胶的来源与形成研究现状

介绍了有机气溶胶来源与形成的研究现状,从有机气溶胶的化学组成特征、一次有机气溶胶的来源和二次有机气溶胶的形成机制论述其研究进展.一次有机气溶胶主要来源于烹调油烟、机动车排放、生物质燃烧、工业或民用燃油锅炉释放出的有机物,还有道路扬尘、沥青、刹车尘、轮胎屑、室外香烟烟雾、以及高等植物蜡、细菌活动和草本植物等.大气中的半挥发性有机物可通过物理和化学吸附形成二次有机气溶胶,一些挥发性有机物可通过气相化学反应转化为低挥发性的物质并形成二次有机气溶胶,其主要前体物是芳香族化合物,如苯、甲苯、二甲苯,以及烯烃、烷烃、环烷烃、萜烯和生物排放的非饱和氧化物.     

Stable chlorine intramolecular kinetic isotope effects from the abiotic dehydrochlorination of DDT

INTENTION, GOAL, SCOPE, BACKGROUND: Identifying different sources and following reaction pathways of chlorinated organic contaminants in the environment can be challenging, especially when only their concentrations are available. Compound-specific stable chlorine measurements of some contaminants have recently been shown to provide additional information and an increased understanding of their biogeochemistry. These studies, however, have been generally limited to volatile molecules. OBJECTIVE: Here, the stable chlorine isotope ratios of the semi-volatile pesticide, 1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (DDT) were investigated. Specifically, the intramolecular stable chlorine isotopic compositions of DDT and the kinetic isotope effect (KIE) for the abiotic dehydrochlorination of DDT to 2,2-bis(p-chlorophenyl)-1,1-dichloroethene (DDE) were determined. METHODS: Selective chemical oxidation of DDT to dichlorobenzophenone (DCBP) and analysis of each compound was used to calculate the stable chlorine isotope ratios of the alkyl and aromatic chlorines in DDT. To determine the KIE for dehydrochlorination, DDT was reacted in a basic solution to yield DDE at 52 degrees C, 60 degrees C, and 72 degrees C for 3, 5, and 5 days, respectively. RESULTS AND DISCUSSION: Significant intramolecular stable chlorine isotopic differences were observed in one sample of DDT where the alkyl and aromatic delta 37Cl values were -5.76 +/- 0.45 and -2.21 +/- 0.24%@1000, respectively. Dehydrochlorination of DDT to DDE in basic solutions at 52, 60, and 70 degrees C resulted in a substantial intramolecular KIE where the alkyl chlorines of DDE shifted by approximately 3%@1000 relative to the alkyl chlorines in DDT. However, no temperature dependence was observed. The KIE, calculated by an iterative program, was 1.009. CONCLUSIONS: Intramolecular differences in the stable chlorine isotope ratios were observed in DDT and this is the first such finding. Dehydrochlorination of DDT yields a measurable and distinct intramolecular stable chlorine KIE. RECOMMENDATION AND OUTLOOK: The results of this study demonstrate the existence of significant intramolecular differences in chlorinated organic compounds. Many other chlorinated semi-volatile and volatile organic contaminants are synthesized from multiple sources of chlorine, and we recommend that similar studies be performed on many such molecules in order to attain a clear understanding of their intramolecular chlorine isotopic differences. The existence of a measurable KIE for the dehydrochlorination of DDT to DDE shows the potential strength of using isotopic measurements to investigate the biogeochemistry of these important compounds. For example, the isotopically depleted aqueous chloride produced by dehydrochlorination of DDT to DDE may be a useful tracer of these reactions in freshwater environments.     

Contaminants of Emerging Concern in Fish from Western U.S. and Alaskan National Parks — Spatial Distribution and Health Thresholds

Remote national parks of the western U.S. and Alaska are not immune to contaminants of emerging concern. Semivolatile organic compounds (SOCs) such as pesticides and PCBs can selectively deposit from the atmosphere at higher rates in cold, high‐elevation and high‐latitude sites, potentially increasing risk to these ecosystems. In the environment, SOCs magnify up food chains and are known to increase health risks such as cancer and reproductive impairment. One hundred twenty‐eight fish in 8 national parks in Alaska and the western U.S. were analyzed for contaminant concentrations, assessed by region, and compared to human and wildlife health thresholds. SOC concentrations from an additional 133 fish from a previous study were also included, for a total of 31 water bodies sampled. PCBs, endosulfan sulfate, and p,p′‐DDE were among the most frequently detected contaminants. Concentrations of historic‐use pesticides dieldrin, p,p′‐DDE, and/or chlordanes in fish exceeded USEPA guidelines for human subsistence fish consumers and wildlife (kingfisher) health thresholds at 13 of 14 parks. Average concentrations in fish ranged from 0.6‐280 ng/g lipid (0.02‐7.3 μg/g ww). Contaminant loading was highest in fish from Alaskan and Sierra Nevada parks. Historic compounds were highest in Alaskan parks, while current‐use pesticides were higher in the Rockies and Sierra Nevada. This study provides a rigorous analysis of CECs in fish from national parks and identifies regions at potential risk.     

Semivolatile organic compounds, organochlorine pesticides and heavy metals in sediments and risk assessment in Huaihe River of China

The concentrations of semivolatile organic compounds, organochlorine pesticides and heavy metals in sediments from Jiangsu reach of Huaihe River, China, were presented. The organic compounds were extracted by acetone： n-hexane using a Soxhlet apparatus and concentrations were performed using HP6890 gas chromatography coupled by FID and ECD detector. The total contents of 8 heavy metals by inductively coupled plasma atomic emission spectrometry or cold-vapor/atomic absorption spectrometry were developed. 30 semivolatile organic compounds were detected, including substituted benzenes, phenols, phthalates and polycyclic aromatic hydrocarbons, from 0.01 to 3.01 mg/kg. 16 organochlorine pesticides were almost detected and from 0.010 to 2.339 μg/kg. Concentrations of major metals were 50 mg/kg or less, mean level of mercury was only 0.055 mg/kg. Compared to sediment quality guidelines （SQGs）, concentrations of some semivolatilc organic compounds were high enough to cause possible toxic effects to living resources. The organochlorine pesticides presented relatively low, lower than threshold effect concentrations （TECs）, harmful effects on sediment-dwelling organisms were not expected. Chromium posed probable toxic effects to the living resources, other heavy metals had no threat temporarily according to SQGs.     

克拉玛依城市土壤的环境磁学特征研究

对克拉玛依市土壤环境磁学特征进行研究,并探讨土壤磁性增强的机制。结果表明:低频质量磁化率(χLF)在不同用地上依次表现为:交通运输用地>商业用地>林地>公共设施用地>未建设用地>居住用地。交通运输用地、公共设施用地较居住用地、非建设用地的土壤以低矫顽力的亚铁磁性矿物含量较高和少量不完全反铁磁性矿物,且磁性颗粒以多畴(MD)颗粒为主,含少量的单畴(SP)颗粒和稳定单畴(SSD)颗粒,与交通运输用地、公共设施用地受到汽车尾气和其他人为活动产生的污染物中含有大量的粗颗粒亚铁磁性矿物密切相关。     

Long-range transport potential of semivolatile organic chemicals in coupled air-water systems

Ongoing deliberations on the regulation of semivolatile organic chemicals require the assessment of chemical transport in atmospheric and marine systems. The characteristic travel distance was proposed as a measure for the transport potential in air and water. However, the existing definition treats the transport processes separately. It is shown that combined transport in coupled air-ocean systems can accelerate the overall transport into remote regions. Concentration ratios in air and water change with distance from sources depending on the initial concentration ratio and on the difference between the transport velocities. A measure is suggested facilitating the chemical screening with respect to transport potentials in such air-ocean systems. A case study for alpha and gamma-hexachlorocyclohexane shows that the suggested measure qualitatively reveals the transport potentials of these chemicals and exemplifies possible concentration patterns.     

大气总悬浮颗粒物中半挥发性有机污染物的测定

采用超声萃取技术提取大气总悬浮颗粒物(TSP)采样膜中的半挥发性有机污染物(SVOC),浓缩净化后,将1μL试样注入气相色谱质谱仪(GC/MS)进行定性定量分析.研究了大气中64种半挥发有机污染物,包括苯酚类、苯胺类、硝基芳香烃类、多环芳烃类和酞酸酯类物质的回收率、精密度和检测限.实验表明,方法操作简便,净化效果好,且部分测定指标优于美国环境标准方法EPA8270c.     

长江口水体中半挥发性有机污染物的分布特征

采用气相色谱法分析了长江口水体中64种半挥发性有机污染物(SVOCs)的含量,共检出其中的50种SVOCs,主要包括多环芳烃类、酚类、酯类、卤代烃类、取代苯类和醚类.其中属于我国优先控制污染物的有16种,属于美国优先控制污染物的有42种,属于我国《地表水环境质量标准》(GB3838-2002)控制的有10种.长江口水体中SVOCs的空间分布表明,南港附近城市排放的工业废水和生活污水是影响水体中SVOCs含量的重要因素之一,表现为排污口附近水域各类SVOCs含量均较高.水体中2,4－二硝基甲苯和六氯丁二烯的检出值超过了中国地表水环境质量标准限值,其最大值分别超标3.32和2.07倍.      

挥发及半挥发有机物污染场地蒸汽抽提修复技术原理与影响因素

土壤蒸汽抽提技术(soil vapor extraction,SVE)因其对挥发性/半挥发性有机物污染土壤治理的有效性、经济性和环境友好性,被广泛用于该类有机物污染土壤的修复.本文介绍了SVE技术的基本原理和工程技术实施的基本步骤,并且讨论了影响SVE修复技术的因素和3种SVE强化技术,最后概述了我国对SVE技术的研究...