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Processing of atmospheric polycyclic aromatic hydrocarbons by fog in an urban environment. 城市环境中雾对大气多环芳烃的处理。
Pub Date : 2012-10-26 Epub Date: 2012-09-12 DOI: 10.1039/c2em30336a
Franz S Ehrenhauser, Kalindi Khadapkar, Youliang Wang, James W Hutchings, Olivier Delhomme, Raghava R Kommalapati, Pierre Herckes, Mary J Wornat, Kalliat T Valsaraj

Polycyclic aromatic hydrocarbons (PAH) are ubiquitous pollutants in the atmosphere, predominantly known for their toxicity. Although there has been substantial work on the atmospheric degradation of PAH, little is known about how the presence of atmospheric droplets (e.g., a fog cloud) affects the fate of PAH. In order to assess the processing of PAH and their corresponding oxidation products during a fog event, two field-sampling campaigns in Fresno, CA and Davis, CA were conducted. The simultaneous evaluation of concentrations of the PAH and oxygenated polycyclic aromatic compounds (OPAC) in the gas phase, particulate matter and fog water droplets before, during and after fog allows for the characterization of transformative and transport processes in a fog cloud. By tracking the ratio of OPAC to PAH in the individual atmospheric phases, two major polycyclic aromatic compounds-processing pathways can be identified: (i) the dissolution of OPAC from particulate matter and (ii) the uptake and oxidation of PAH in the fog water droplets. Wet deposition steadily decreases the pollutant concentration in the fog cloud droplets during a fog event; however, uptake and concentration via evaporative water loss upon the dissipation of a fog cloud cause an increase in the atmospheric pollutant concentration.

多环芳烃(PAH)是大气中普遍存在的污染物,主要以其毒性而闻名。虽然在大气中多环芳烃的降解方面已经有了大量的工作,但人们对大气液滴(如雾云)的存在如何影响多环芳烃的命运知之甚少。为了评估多环芳烃及其相应的氧化产物在雾事件中的处理,在加利福尼亚州弗雷斯诺和加利福尼亚州戴维斯进行了两次实地采样活动。同时评估多环芳烃和氧合多环芳烃(OPAC)在雾前、雾中和雾后的气相、颗粒物和雾水滴中的浓度,可以表征雾云中的转化和传输过程。通过跟踪各大气相中OPAC与PAH的比例,可以确定两种主要的多环芳香族化合物处理途径:(i) OPAC从颗粒物中溶解;(ii)雾水滴对PAH的吸收和氧化。在雾事件中,湿沉降稳定地降低了雾云滴中的污染物浓度;然而,在雾云消散时,通过蒸发水分损失的吸收和浓缩导致大气污染物浓度的增加。
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引用次数: 36
Size dependent aqueous dispersibility of carboxylated multiwall carbon nanotubes. 羧化多壁碳纳米管的水分散性。
Pub Date : 2012-10-26 Epub Date: 2012-09-13 DOI: 10.1039/c2em30405h
Susana Addo Ntim, Ornthida Sae-Khow, Chintal Desai, Frank A Witzmann, Somenath Mitra

The size dependent colloidal behavior of aqueous dispersions of carboxylated multiwall carbon nanotubes (c-MWCNTs) is presented. The presence of carboxylic groups provided electrostatic stabilization in water, where the size affected agglomeration. While aspect ratio did not show any definite correlation, the hydrophobicity indices (HI), zeta potential and aggregation kinetics showed dependence on the length of the c-MWCNTs where the shorter c-MWCNTs showed significantly lower HI values, smaller particle aggregates, higher zeta potential values and higher critical coagulation concentrations (ccc) in the presence of electrolytes. Although the diameter of the short c-MWCNTs did not appear to influence their aggregation behavior, the longer c-MWCNTs showed a dependence on diameter where stability decreased with increasing CNT diameter.

介绍了羧化多壁碳纳米管(c-MWCNTs)水分散体的粒径依赖性胶体行为。羧基的存在在水中提供了静电稳定性,其中尺寸影响团聚。虽然宽高比没有显示出任何明确的相关性,但疏水性指数(HI)、zeta电位和聚集动力学与c-MWCNTs的长度有关,其中较短的c-MWCNTs在电解质存在下具有较低的HI值、较小的颗粒聚集、较高的zeta电位值和较高的临界凝血浓度(ccc)。虽然短c-MWCNTs的直径似乎不影响它们的聚集行为,但较长的c-MWCNTs表现出对直径的依赖,其稳定性随着碳纳米管直径的增加而下降。
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引用次数: 22
Gold mining impact on riverine heavy metal transport in a sparsely monitored region: the upper Lake Baikal Basin case. 少监测地区金矿开采对河流重金属运输的影响:贝加尔湖上游流域案例。
Pub Date : 2012-10-26 Epub Date: 2012-09-13 DOI: 10.1039/c2em30643c
Josefin Thorslund, Jerker Jarsjö, Sergey R Chalov, Ekaterina V Belozerova

Mining and ore excavation can cause the acidification and heavy metal pollution of downstream water systems. It can be difficult to assess the load contributions from individual mining areas, which is commonly required for environmental impact assessments. In the current study, we quantified the net impact of the unmonitored mining activities in the Zaamar Goldfield (Mongolia) on heavy metal transport in the downstream Tuul River-Selenga River-Lake Baikal water systems. We also noted that the Zaamar site shares the conditions of limited monitoring with many rapidly developing regions of the world. The heavy metal concentrations and flow data were obtained from historical measurement campaigns, long-term monitoring, and a novel field campaign. The results indicate that natural mass flows of heavy metals in dissolved form increased by an order of magnitude because of mining. Prevailing alkaline conditions in the vicinity of Zaamar can limit the dissolution, maintaining the on-site concentrations below health-risk based guideline values. However, suspended river concentrations are much higher than the dissolved concentrations. The placer gold mining at the Zaamar site has increased the total riverine mass flows of Al, As, Cu, Fe, Mn, Pb and Zn by 44.300, 30.1, 65.7, 47.800, 1.480, 76.0 and 65.0 tonnes per year respectively. We suggest that local to regional transformation and enrichment processes in combination with suspended sediment transport from numerous existing upstream mining areas contribute to high concentrations of dissolved heavy metals in downstream parts of the Selenga River, including its delta area at Lake Baikal. Furthermore, single hydrological events can increase the suspended load concentrations by at least one order of magnitude. Overall, the Selenga River Basin, which drains into Lake Baikal, should be recognised as one of the world's most impacted areas with regard to heavy metal loads, and it contributes to 1% and 3% of the world flux of dissolved Fe and Pb, respectively.

采矿和矿石挖掘会造成下游水系酸化和重金属污染。评估个别矿区的负荷贡献可能很困难,这通常是环境影响评估所需要的。在本研究中,我们量化了Zaamar金矿(蒙古)不受监测的采矿活动对下游图勒河-色楞嘎河-贝加尔湖水系重金属运输的净影响。我们还注意到,扎马尔场址与世界上许多迅速发展的地区一样,都有有限监测的条件。重金属浓度和流量数据是通过历史测量活动、长期监测和一项新的现场活动获得的。结果表明,由于开采,溶解态重金属自然质量流量增加了一个数量级。Zaamar附近普遍存在的碱性条件可以限制溶解,使现场浓度保持在基于健康风险的指导值以下。然而,悬浮的河流浓度远高于溶解的浓度。Zaamar矿区砂金开采使Al、As、Cu、Fe、Mn、Pb和Zn的河流总流量分别增加了44.300、30.1、65.7、47.800、1.480、76.0和65.0吨/年。我们认为,局部到区域的转变和富集过程,加上来自众多现有上游矿区的悬浮沉积物运输,导致色楞格河下游地区(包括贝加尔湖三角洲地区)溶解重金属浓度很高。此外,单个水文事件可以使悬浮荷载浓度增加至少一个数量级。总体而言,流入贝加尔湖的色楞格河流域应该被认为是世界上受重金属负荷影响最严重的地区之一,它分别占世界溶解铁和铅通量的1%和3%。
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引用次数: 92
Apparatus for in situ monitoring of copper in coastal waters. 沿海水域中铜的现场监测装置。
Pub Date : 2012-10-26 Epub Date: 2012-09-17 DOI: 10.1039/c2em30460k
Conrad S Chapman, Richard D Cooke, Pascal Salaün, Constant M G van den Berg

Apparatus is designed and tested to determine metals in situ in seawater. Voltammetry with a vibrating gold microwire electrode (VGME) is combined with a battery powered potentiostat and a processor board and is tested for in situ monitoring of copper (Cu) in coastal waters. The VGME was combined with solid state reference and counter electrodes to make a single vibrating probe which was rated up to a depth of 40 m. The measuring mode for Cu was square-wave anodic stripping voltammetry whilst dissolved oxygen (DO) was monitored by a linear sweep scan in a negative potential direction. The working electrode was reactivated between measurements using a suitable potential sequence. The novelties of this work are the field-testing of apparatus incorporating a VGME for copper monitoring, which eliminates the need for pumping and reagents, but has sufficient sensitivity for low ambient levels of copper, and the use of a novel potential sequence to stabilise the response over a long time period. The apparatus has a measuring time of about 6 weeks and a measuring frequency of 12 h(-1). Measurement is reagent-free and power use is low as no pump is required. Experiments are carried out to test the stability of response of the system at various temperatures and its robustness with respect to long-term copper monitoring. Preliminary data were obtained during autonomous deployment over several weeks on a buoy in the Irish Sea. Vertical movement of the buoy caused individual measurements to have a variability of about 15%. It was found that longer term variability of the electrode could be minimised by normalisation of the Cu response over that of DO as the response was related to diffusion through the electrode surface which was similarly affected. The detected fraction of Cu (labile Cu) amounted to 1.5-4 nM during different deployments at a total Cu concentration of ∼10 nM. The same ratio was found by voltammetry in samples taken to the laboratory. The new apparatus has demonstrated that metals in coastal waters can be monitored at trace level, much facilitating the monitoring of outfalls and local water contamination. Because of its sensitivity the apparatus would be of use in estuarine as well as coastal waters, with the aim of monitoring intermittent variability in the copper concentration.

设计并试验了海水中金属原位测定装置。伏安法与振动金微丝电极(VGME)结合电池供电的恒电位器和处理器板,用于沿海水域铜(Cu)的原位监测。VGME与固态参考电极和反电极相结合,制成一个额定深度为40 m的振动探头。铜的测量方式采用方波阳极溶出伏安法,溶解氧(DO)采用负电位方向线性扫描法监测。在测量之间使用合适的电位序列重新激活工作电极。这项工作的新颖之处在于现场测试了包含用于铜监测的VGME设备,这消除了对泵浦和试剂的需要,但对低环境铜水平具有足够的灵敏度,并且使用了新的电位序列来稳定长时间的响应。该仪器的测量时间约为6周,测量频率为12小时(-1)。测量是无试剂和电力使用低,因为不需要泵。实验测试了系统在不同温度下的响应稳定性及其对铜长期监测的鲁棒性。初步数据是在爱尔兰海的一个浮标上自主部署的几个星期中获得的。浮标的垂直运动导致单个测量值的可变性约为15%。研究发现,电极的长期可变性可以通过将Cu响应归一化而不是DO响应的归一化来最小化,因为响应与通过电极表面的扩散有关,这也受到了类似的影响。在Cu总浓度为~ 10 nM的不同部署下,检测到的Cu(不稳定Cu)分数为1.5-4 nM。在送到实验室的样品中,伏安法也发现了同样的比例。新的仪器已经证明,沿海水域的金属可以在痕量水平上进行监测,大大促进了对排放物和当地水污染的监测。由于其灵敏度,该仪器将用于河口和沿海水域,目的是监测铜浓度的间歇性变化。
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引用次数: 6
Comments on "assessment of prenatal mercury exposure in a predominantly Caribbean immigrant community in Brooklyn, NY". 关于“纽约布鲁克林一个主要加勒比移民社区产前汞暴露评估”的评论。
Pub Date : 2012-10-26 Epub Date: 2012-09-06 DOI: 10.1039/c2em30475a
Arnold Wendroff
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引用次数: 1
Calcium- and ammonium ion-modification of zeolite amendments affects the metal-uptake of Hieracium piloselloides in a dose-dependent way. 沸石改性剂的钙铵离子改性对毛蕊草的金属吸收率有剂量依赖性。
Pub Date : 2012-10-26 Epub Date: 2012-08-17 DOI: 10.1039/c2em30301a
Anca Peter, Leonard Mihaly-Cozmuta, Anca Mihaly-Cozmuta, Camelia Nicula, Emil Indrea, Hlanganani Tutu

The role of natural zeolite and of two types of modified zeolite (with ammonium and with calcium ions) in reducing the accumulation of ions of heavy metals in roots and leaves of Hieracium piloselloides grown on tailing ponds was investigated. The variation of the content of zeolite (5% w/w and 10% w/w) is another parameter that significantly and positively affects the accumulation of the metal ions in Hieracium piloselloides. The results showed that zeolite used as an amendment in the soil in tailing ponds significantly reduces the accumulation of heavy metal ions in Hieracium piloselloides. The highest concentrations of heavy metals were accumulated in plants grown on soil without zeolite, being followed by the plants grown on the substrate with natural zeolite. Moreover, the translocation factors of heavy metal ions uptake in roots and leaves grown on substrates with modified zeolites are lower than those calculated for the organs grown on the substrate amended with natural zeolite. This behaviour has demonstrated the positive effect of those changes of zeolite amendments in the potential phytoremediation practice.

研究了天然沸石和两种改性沸石(含铵和钙离子)对尾矿库生长的毛叶Hieracium piloselloides根和叶中重金属离子积累的影响。沸石含量的变化(5% w/w和10% w/w)是影响毛叶猴耳草中金属离子积累的另一个显著且积极的参数。结果表明,在尾矿库土壤中添加沸石改进剂可显著降低毛叶猴体内重金属离子的积累。在不含沸石的土壤上生长的植物重金属积累浓度最高,其次是在含天然沸石的基质上生长的植物。此外,在改性沸石基质上生长的根和叶的重金属离子吸收转运因子低于在天然沸石基质上生长的器官。这种行为证明了沸石改性剂的这些变化在潜在的植物修复实践中的积极作用。
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引用次数: 29
Levels and distribution of hexabromocyclododecane (HBCD) in environmental samples near manufacturing facilities in Laizhou Bay area, East China. 莱州湾地区生产设施附近环境样品中六溴环十二烷(HBCD)的含量及分布
Pub Date : 2012-10-26 Epub Date: 2012-08-17 DOI: 10.1039/c2em30231d
Honghua Li, Qinghua Zhang, Pu Wang, Yingming Li, Jianxia Lv, Weihai Chen, Dawei Geng, Yawei Wang, Thanh Wang, Guibin Jiang

A total of 55 samples including soil, sediment, plants (cypress, reed and seepweed) and aquatic species were collected at locations around hexabromocyclododecane (HBCD) manufacturing facilities in Laizhou Bay area, East China. HBCD was determined at concentrations ranging between 0.88 and 6901 ng g(-1) dry weight (dw), 2.93-1029 ng g(-1) dw, 8.88-160241 ng g(-1) dw, and 7.09-815 ng g(-1) lipid weight (lw), respectively. Significant negative correlations (r(2) = 0.54, p = 0.006) were observed between HBCD concentrations in soils and the distance from the manufacturing facility, and the concentrations became constant when the distance was >4 km. The calculation results on the bioaccumulation factors (BAFs) suggested that HBCD may be accumulated in plants. Tissue-specific bioaccumulation of HBCD diastereoisomers was found in aquatic species. For example, in crabs the highest concentrations of HBCD (815 ng g(-1) lw for female and 446 ng g(-1) lw for male) were observed in the gill. Besides the gill, α-HBCD was more preferentially accumulated in the spermary and ovary, while β- and γ-HBCD were more accumulated in the muscle. A similar distribution was also observed in roe and muscle of goby fish.

在莱州湾地区六溴环十二烷(HBCD)生产设施周围采集了土壤、沉积物、植物(柏树、芦苇和海杂草)和水生物种等55个样本。测定HBCD浓度范围分别为0.88 ~ 6901 ng g(-1)干重(dw)、2.93 ~ 1029 ng g(-1) dw、8.88 ~ 160241 ng g(-1) dw和7.09 ~ 815 ng g(-1)脂重(lw)。土壤中HBCD浓度与工厂距离呈显著负相关(r(2) = 0.54, p = 0.006),当工厂距离>4 km时,土壤中HBCD浓度趋于稳定。生物积累因子(baf)的计算结果表明,HBCD可能在植物体内积累。在水生物种中发现了HBCD非对映异构体的组织特异性生物积累。例如,在蟹的鳃中观察到最高的HBCD浓度(雌性为815 ng g(-1) lw,雄性为446 ng g(-1) lw)。除鳃外,α-HBCD更倾向于在精子和卵巢中积累,β-和γ-HBCD更多地在肌肉中积累。虾虎鱼的鱼子和肌肉也有类似的分布。
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引用次数: 42
Using Py-GC/MS to fingerprint additives associated with paper mill effluent toxicity episodes. 采用液相色谱/质谱法测定造纸厂废水毒性事件相关添加剂的指纹图谱。
Pub Date : 2012-10-26 Epub Date: 2012-08-28 DOI: 10.1039/c2em30359k
B Bruce Sithole, Jorge Pimentel, Sharon Gibbons, Chu Watanabe

Understanding the cause of effluent toxicity is an important requirement for its prevention, remediation and return to compliance. One component of the strategy entails identification and fingerprinting of additives or components in additives that may be the cause of the toxicity episodes. A number of additives used in pulp and papermaking are polymeric compounds that are suspect in effluent toxicity. Their analysis and detection is difficult as they are not amenable to analysis by normal techniques applicable to mill effluents such as gas chromatography. Py-GC/MS is a powerful analytical technique that can be used to fingerprint these additives. The presence of the additives is confirmed by fingerprint pyrograms of the additives (or components in the formulations of the additives) in conjunction with mass spectrometry. The technique has been used to fingerprint and quantify polymeric additives associated with mill effluent toxicity episodes.

了解废水毒性的原因是其预防、补救和恢复合规的重要要求。该策略的一个组成部分需要对可能引起毒性事件的添加剂或添加剂中的成分进行鉴定和指纹识别。在纸浆和造纸中使用的一些添加剂是聚合物化合物,在废水毒性方面有嫌疑。它们的分析和检测是困难的,因为它们不适合用气相色谱法等适用于工厂废水的常规技术进行分析。Py-GC/MS是一种功能强大的分析技术,可用于这些添加剂的指纹图谱。添加剂的存在通过结合质谱法的添加剂(或添加剂配方中的成分)的指纹热像图来确认。该技术已用于指纹和量化与工厂废水毒性事件相关的聚合物添加剂。
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引用次数: 2
Lifetime of combustion-generated environmentally persistent free radicals on Zn(II)O and other transition metal oxides. Zn(II)O 和其他过渡金属氧化物上燃烧产生的环境持久性自由基的寿命。
Pub Date : 2012-10-26 Epub Date: 2012-09-18 DOI: 10.1039/c2em30545c
Eric Vejerano, Slawo Lomnicki, Barry Dellinger

Previous studies indicated that Environmentally Persistent Free Radicals (EPFRs) are formed in the post-flame, cool zone of combustion. They result from the chemisorption of gas-phase products of incomplete combustion (particularly hydroxyl- and chlorine-substituted aromatics) on Cu(II)O, Fe(III)(2)O(3), and Ni(II)O domains of particulate matter (fly ash or soot particles). This study reports our detailed laboratory investigation on the lifetime of EPFRs on Zn(II)O/silica surface. Similarly, as in the case of other transition metals, chemisorption of the adsorbate on the Zn(II)O surface and subsequent transfer of electron from the adsorbate to the metal forms a surface-bound EPFR and a reduced metal ion center. The EPFRs are stabilized by their interaction with the metal oxide domain surface. The half-lives of EPFRs formed on Zn(II)O domains were the longest observed among the transition metal oxides studied and ranged from 3 to 73 days. These half-lives were an order of magnitude longer than those formed on nickel and iron oxides, and were 2 orders of magnitude longer compared to the EPFRs on copper oxide which have half-lives only on the order of hours. The longest-lived radicals on Zn(II)O correspond to the persistency in ambient air particles of almost a year. The half-life of EPFRs was found to correlate with the standard reduction potential of the associated metal.

以往的研究表明,环境持久性自由基(EPFR)是在燃烧后的火焰冷却区形成的。它们是由不完全燃烧的气相产物(特别是羟基和氯代芳烃)在颗粒物质(飞灰或烟尘颗粒)的 Cu(II)O、Fe(III)(2)O(3) 和 Ni(II)O 域上的化学吸附作用产生的。本研究报告了我们对 Zn(II)O/二氧化硅表面上 EPFR 的寿命进行的详细实验室调查。与其他过渡金属的情况类似,吸附物在 Zn(II)O 表面的化学吸附以及随后电子从吸附物转移到金属上形成了表面结合的 EPFR 和还原的金属离子中心。EPFR 通过与金属氧化物畴表面的相互作用而得到稳定。在所研究的过渡金属氧化物中,Zn(II)O 域上形成的 EPFR 的半衰期最长,从 3 天到 73 天不等。这些半衰期比在镍和铁氧化物上形成的 EPFR 长一个数量级,比在氧化铜上形成的 EPFR 长两个数量级,后者的半衰期只有几个小时。Zn(II)O 上最长寿的自由基在环境空气颗粒中的持续时间几乎为一年。发现 EPFR 的半衰期与相关金属的标准还原电位有关。
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引用次数: 0
Sedimentary loadings and ecological significance of polycyclic aromatic hydrocarbons in a typical mariculture zone of South China. 华南典型海水养殖区多环芳烃沉积负荷及其生态意义
Pub Date : 2012-10-26 Epub Date: 2012-08-17 DOI: 10.1039/c2em30292f
Huan-Yun Yu, Lian-Jun Bao, Charles S Wong, Yuanan Hu, Eddy Y Zeng

Two sediment cores were collected from Hailing Bay located in a typical mariculture zone of Guangdong Province, South China, and analyzed for polycyclic aromatic hydrocarbons (PAHs). The concentrations of the sum of 27 PAHs ranged from 62 to 1200 ng g(-1) dry wt, and sediment in the study area was considered to be moderately polluted by PAHs. Source diagnostics based on PAH composition and principal component analysis suggested that PAHs in the study area were mainly derived from petroleum combustion, with discharge of PAHs from fishing boats as an important source. Ecological risk assessment results indicate that PAHs in sediment of the present study currently have minimal adverse effect on the mariculture environment. Comparison of sedimentary inventory of PAHs in the fish harbor of the study area with those in the Pearl River Estuary and the coastal Bohai Bay indicate that the sediment has become an important reservoir of PAHs.

在广东海岭湾采集了2个沉积物岩心,分析了沉积物中多环芳烃(PAHs)的含量。27种多环芳烃的浓度总和在62 ~ 1200 ng g(-1) dry wt之间,研究区沉积物受多环芳烃污染程度为中度。基于多环芳烃组成和主成分分析的多环芳烃源诊断表明,研究区多环芳烃主要来源于石油燃烧,渔船排放的多环芳烃是重要来源。生态风险评价结果表明,目前研究沉积物中多环芳烃对海水养殖环境的不利影响最小。研究区鱼港沉积物中PAHs的清查结果与珠江口和渤海湾沿岸沉积物中PAHs清查结果的比较表明,该沉积物已成为PAHs的重要储集层。
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引用次数: 9
期刊
Journal of Environmental Monitoring
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