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Trace elements in PM2.5 shed light on Saharan dust incursions over the Munich airshed in spring 2022† PM2.5 中的痕量元素揭示了 2022 年春季撒哈拉沙尘入侵慕尼黑上空的情况†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-08 DOI: 10.1039/D4EA00092G
Sara Padoan, Alessandro Zappi, Jan Bendl, Tanja Herrmann, Ajit Mudan, Carsten Neukirchen, Erika Brattich, Laura Tositti and Thomas Adam

The influence of a prolonged Saharan Dust event across Europe and specifically in Munich (Germany) in March 2022 was detected and analyzed in detail. The event arose from a sequence of Saharan Dust incursions intertwined with a stagnation in the regional circulation leading to the persistence of a mineral dust plume for several weeks over the region. Trace element and meteorological data were collected. Enrichment factors, size distribution analyses, and multivariate techniques such as Varimax and Self-Organizing Maps (SOM) were applied to highlight the influence of Saharan Dusts and to evaluate the pollution sources in Munich municipality. The overall results revealed how the Munich airshed was clearly affected by long-distance mineral dusts from the North African desert, that increased the concentrations of natural (e.g. Al, Mg, Ca) and anthropogenic (e.g. Sb, Mo, Pb) elements based on the different paths followed by the dusts. Moreover, the chemometric analyses revealed a range of well-defined local anthropogenic emission sources including road traffic, energy production by coal combustion (S and Se), traffic (Cu, Sb), and waste incineration (Zn).

检测并详细分析了 2022 年 3 月撒哈拉沙尘事件对整个欧洲,特别是对慕尼黑(德国)的影响。该事件源于一连串撒哈拉沙尘的入侵,与区域环流的停滞交织在一起,导致矿物尘羽在该地区上空持续数周。收集了痕量元素和气象数据。应用富集因子、粒度分布分析和多元技术(如 Varimax 和自组织图 (SOM))来突出撒哈拉沙尘的影响,并评估慕尼黑市的污染源。总体结果显示,慕尼黑空气流域明显受到来自北非沙漠的长距离矿物尘埃的影响,根据尘埃的不同路径,增加了天然(如 Al、Mg、Ca)和人为(如 Sb、Mo、Pb)元素的浓度。此外,化学计量学分析还揭示了一系列明确的当地人为排放源,包括道路交通、燃煤能源生产(S 和 Se)、交通(Cu、Sb)和垃圾焚烧(Zn)。
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引用次数: 0
Evaluating emissions and meteorological contributions to air quality trends in northern China based on measurements at a regional background station† 基于区域本底站的测量结果,评估排放和气象对中国北方空气质量趋势的影响†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-08 DOI: 10.1039/D4EA00070F
Weiwei Pu, Yingruo Li, Xiaowan Zhu, Xiangxue Liu, Di He, Fan Dong, Heng Guo, Guijie Zhao, Liyan Zhou, Shuangshuang Ge and Zhiqiang Ma

The contributions of meteorology and emissions to air pollutant trends are critical for air quality management, but they have not been fully analyzed, especially in the background area of northern China. Here, we used a machine learning technique to quantify the impacts of meteorological conditions and emissions on PM2.5, NO2, SO2, O3, and CO pollution during 2013–2021 and evaluated their contributions to Clean Air Action policies. The annual effect of the meteorology on PM2.5, NO2, SO2, and CO levels was dominated by the meteorological conditions during the cold season, while that of the O3 level largely depended on the meteorological conditions during the warm season. Meteorology-driven anomalies contributed −14.8 to 10.3%, −8.5 to 7.3%, −11 to 7.1%, −7.9 to 6.0%, and −7.4 to 7.3% to the annual mean concentrations of PM2.5, NO2, SO2, O3, and CO during the study period, respectively. The Clean Air Actions have led to a major improvement in the air quality at regional scale, with the reduction of 1.7 μg m−3 year−1, 0.2 μg m−3 year−1, 1.5 μg m−3 year−1, 0.7 μg m−3 year−1, and 0.03 mg m−3 year−1 for PM2.5, NO2, SO2, O3, and CO at background area, respectively, after meteorological correction. Although emissions dominated the long-term variations in pollutants, the meteorological conditions obviously played a positive role during the action periods for pollutants except for O3. Considering the notable effects of the meteorological conditions on air pollution and the interreaction between pollutants, a more comprehensive control strategy should be considered on a broader regional scale.

气象和排放对空气污染物趋势的影响对于空气质量管理至关重要,但目前尚未对其进行全面分析,尤其是在中国北方的背景地区。在此,我们利用机器学习技术量化了 2013-2021 年气象条件和排放对 PM2.5、NO2、SO2、O3 和 CO 污染的影响,并评估了它们对清洁空气行动政策的贡献。气象对 PM2.5、NO2、SO2 和 CO 水平的年度影响主要受寒冷季节气象条件的影响,而对 O3 水平的影响则主要取决于温暖季节的气象条件。在研究期间,气象驱动的异常对 PM2.5、NO2、SO2、O3 和 CO 年平均浓度的影响分别为-14.8%至 10.3%、-8.5%至 7.3%、-11%至 7.1%、-7.9%至 6.0%和-7.4%至 7.3%。清洁空气行动大大改善了区域范围内的空气质量,经气象校正后,背景区域 PM2.5、NO2、SO2、O3 和 CO 的浓度分别降低了 1.7 μg m-3 年-1、0.2 μg m-3 年-1、1.5 μg m-3 年-1、0.7 μg m-3 年-1 和 0.03 mg m-3 年-1。虽然排放主导了污染物的长期变化,但除 O3 外,气象条件在污染物的作用期明显发挥了积极作用。考虑到气象条件对空气污染的显著影响以及污染物之间的相互影响,应在更广泛的区域范围内考虑更全面的控制策略。
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引用次数: 0
Determination of mass concentrations of airborne PET microplastics using liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS)† 使用液相色谱耦合串联质谱法(LC-MS/MS)†测定空气中PET微塑料的质量浓度
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-10-04 DOI: 10.1039/D4EA00047A
Durga Prasad Patnana and B. P. Chandra

Microplastics (MPs) have recently become a growing environmental pollution concern. MPs are easily transferred and ubiquitously found in ambient air. MPs in the air can act as carriers for several toxic pollutants, and exposure to MPs can lead to pulmonary diseases in humans. Polyethylene terephthalate (PET) is one of the most abundant MPs used in the manufacturing of various fibres and plastics. In this study, we present a method for the determination of mass concentrations of PET MPs in the airborne inhalable fraction of fine particulate matter (PM2.5) using liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS). Teflon and quartz fiber filters were tested for extraction efficiency in measuring the mass concentrations of airborne PET MPs. Teflon filters showed good recovery (80–120%) compared to quartz fiber filters. Using this method, a pilot study was carried out in Delhi, the national capital of India, and Mohali, a suburban city in the northwest Indo-Gangetic Plain (NWIGP), for the determination of mass concentrations of PET MPs present in airborne PM2.5. The observed maximum mass concentrations of PET MPs in airborne PM2.5 in Delhi and Mohali are 135.20 ng m−3 and 157.98 ng m−3, respectively.

微塑料(MPs)最近成为一个日益严重的环境污染问题。MPs很容易转移,并且在周围空气中无处不在。空气中的多聚体可作为几种有毒污染物的载体,暴露于多聚体可导致人类肺部疾病。聚对苯二甲酸乙二醇酯(PET)是用于制造各种纤维和塑料的最丰富的MPs之一。在这项研究中,我们提出了一种利用液相色谱-串联质谱(LC-MS/MS)测定空气中细颗粒物(PM2.5)可吸入部分中PET MPs质量浓度的方法。测试了聚四氟乙烯和石英纤维过滤器在测量空气中PET MPs质量浓度时的萃取效率。与石英纤维过滤器相比,聚四氟乙烯过滤器具有良好的回收率(80-120%)。利用该方法,在印度首都德里和印度-恒河平原(NWIGP)西北部的郊区城市莫哈里进行了一项试点研究,以确定空气中PM2.5中PET MPs的质量浓度。在德里和莫哈里观测到的空气中PM2.5中PET MPs的最大质量浓度分别为135.20 ng m - 3和157.98 ng m - 3。
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引用次数: 0
Kinetics of the reactions of the Criegee intermediate CH2OO with water vapour: experimental measurements as a function of temperature and global atmospheric modelling† 克里基中间体 CH2OO 与水蒸气反应的动力学:作为温度函数的实验测量结果和全球大气模型†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-30 DOI: 10.1039/D4EA00097H
Rachel E. Lade, Mark A. Blitz, Matthew Rowlinson, Mathew J. Evans, Paul W. Seakins and Daniel Stone
<p >The kinetics of reactions between the simplest Criegee intermediate, CH<small><sub>2</sub></small>OO, and water vapour have been investigated at temperatures between 262 and 353 K at a total pressure of 760 Torr using laser flash photolysis of CH<small><sub>2</sub></small>I<small><sub>2</sub></small>–O<small><sub>2</sub></small>–N<small><sub>2</sub></small>–H<small><sub>2</sub></small>O mixtures coupled with broadband time-resolved UV absorption spectroscopy. Results indicate that the reaction with water monomers represents a minor contribution to the total loss of CH<small><sub>2</sub></small>OO under the conditions employed in this work, with an estimated rate coefficient for CH<small><sub>2</sub></small>OO + H<small><sub>2</sub></small>O (R1) of (9.8 ± 5.9) × 10<small><sup>−17</sup></small> cm<small><sup>3</sup></small> molecule<small><sup>−1</sup></small> s<small><sup>−1</sup></small> at 298 K and a temperature dependence described by <em>k</em><small><sub>1</sub></small> = (3.2 ± 1.1) × 10<small><sup>−13</sup></small> exp(−(2410 ± 270)/<em>T</em>) cm<small><sup>3</sup></small> molecule<small><sup>−1</sup></small> s<small><sup>−1</sup></small>. The reaction of CH<small><sub>2</sub></small>OO with water dimers, CH<small><sub>2</sub></small>OO + (H<small><sub>2</sub></small>O)<small><sub>2</sub></small> (R2), dominates under the conditions employed in this work. The rate coefficient for R2 has been measured to be <em>k</em><small><sub>2</sub></small> = (9.5 ± 2.5) × 10<small><sup>−12</sup></small> cm<small><sup>3</sup></small> molecule<small><sup>−1</sup></small> s<small><sup>−1</sup></small> at 298 K, with a negative temperature dependence described by <em>k</em><small><sub>2</sub></small> = (2.85 ± 0.40) × 10<small><sup>−15</sup></small> exp((2420 ± 340)/<em>T</em>) cm<small><sup>3</sup></small> molecule<small><sup>−1</sup></small> s<small><sup>−1</sup></small>, where rate<small><sub>R2</sub></small> = <em>k</em><small><sub>2</sub></small>[CH<small><sub>2</sub></small>OO][(H<small><sub>2</sub></small>O)<small><sub>2</sub></small>]. For use in atmospheric models, we recommend description of the kinetics for R2 in terms of the product of the rate coefficient <em>k</em><small><sub>2</sub></small> and the equilibrium constant <em>K</em><small><sup>D</sup></small><small><sub>eq</sub></small> (<em>k</em><small><sub>2,eff</sub></small> = <em>k</em><small><sub>2</sub></small><em>K</em><small><sup>D</sup></small><small><sub>eq</sub></small>) for water dimer formation to allow the rate of reaction to be expressed in terms of water monomer concentration as rate<small><sub>R2</sub></small> = <em>k</em><small><sub>2,eff</sub></small>[CH<small><sub>2</sub></small>OO][H<small><sub>2</sub></small>O]<small><sup>2</sup></small> to avoid explicit calculation of dimer concentrations and impacts of differences in values of <em>K</em><small><sup>D</sup></small><small><sub>eq</sub></small> reported in the literature. Results from this work give <em>k</em><small
利用激光闪烁光解 CH2I2-O2-N2-H2O 混合物并结合宽带时间分辨紫外吸收光谱,研究了在 262 至 353 K 温度、760 托总压条件下最简单的克里基中间体 CH2OO 与水蒸气之间的反应动力学。结果表明,在本研究采用的条件下,与水单体的反应对 CH2OO 的总损失贡献不大,在 298 K 时,CH2OO + H2O (R1) 的估计速率系数为 (9.8 ± 5.9) × 10-17 cm3 分子-1 s-1,与温度的关系用 k1 = (3.2 ± 1.1) × 10-13 exp(-(2410 ± 270)/T) cm3 分子-1 s-1 描述。在本研究采用的条件下,CH2OO 与水二聚体的反应 CH2OO + (H2O)2 (R2) 占主导地位。在 298 K 时,R2 的速率系数为 k2 = (9.5 ± 2.5) × 10-12 cm3 分子-1 s-1,与温度的负相关关系为 k2 = (2.85 ± 0.40) × 10-15 exp((2420 ± 340)/T) cm3 分子-1 s-1,其中速率 R2 = k2[CH2OO][(H2O)2]。在大气模型中使用时,我们建议用水二聚体形成的速率系数 k2 与平衡常数 KDeq 的乘积(k2,eff = k2KDeq)来描述 R2 的动力学,以便用水单体浓度来表示反应速率,即速率 R2 = k2,eff[CH2OO][H2O]2,从而避免明确计算二聚体浓度和文献中报告的 KDeq 值差异的影响。这项工作的结果表明,在 298 K 时,k2,eff = (1.96 ± 0.51) × 10-32 cm6 molecule-2 s-1,温度依赖性描述为 k2,eff = (2.78 ± 0.28) × 10-38 exp((4010 ± 400)/T) cm6 molecule-2 s-1。在这项工作中,没有观察到 CH2OO 和三个水分子之间的反应有明显的影响,这可能是这项工作中使用的相对湿度(298 K 时高达 57%)的结果。使用全球化学传输模型 GEOS-Chem 对结果对大气的影响进行了研究。模型模拟表明,与水二聚体的反应主导了大气中 CH2OO 的损失,并限制了 CH2OO 其他反应的影响,与水二聚体的反应占对流层中 CH2OO 总损失的 98%。
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Seakins and Daniel Stone","doi":"10.1039/D4EA00097H","DOIUrl":"https://doi.org/10.1039/D4EA00097H","url":null,"abstract":"&lt;p &gt;The kinetics of reactions between the simplest Criegee intermediate, CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO, and water vapour have been investigated at temperatures between 262 and 353 K at a total pressure of 760 Torr using laser flash photolysis of CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;I&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;–O&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;–N&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;–H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O mixtures coupled with broadband time-resolved UV absorption spectroscopy. Results indicate that the reaction with water monomers represents a minor contribution to the total loss of CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO under the conditions employed in this work, with an estimated rate coefficient for CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO + H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O (R1) of (9.8 ± 5.9) × 10&lt;small&gt;&lt;sup&gt;−17&lt;/sup&gt;&lt;/small&gt; cm&lt;small&gt;&lt;sup&gt;3&lt;/sup&gt;&lt;/small&gt; molecule&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; s&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; at 298 K and a temperature dependence described by &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;1&lt;/sub&gt;&lt;/small&gt; = (3.2 ± 1.1) × 10&lt;small&gt;&lt;sup&gt;−13&lt;/sup&gt;&lt;/small&gt; exp(−(2410 ± 270)/&lt;em&gt;T&lt;/em&gt;) cm&lt;small&gt;&lt;sup&gt;3&lt;/sup&gt;&lt;/small&gt; molecule&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; s&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt;. The reaction of CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO with water dimers, CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO + (H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O)&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; (R2), dominates under the conditions employed in this work. The rate coefficient for R2 has been measured to be &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; = (9.5 ± 2.5) × 10&lt;small&gt;&lt;sup&gt;−12&lt;/sup&gt;&lt;/small&gt; cm&lt;small&gt;&lt;sup&gt;3&lt;/sup&gt;&lt;/small&gt; molecule&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; s&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; at 298 K, with a negative temperature dependence described by &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; = (2.85 ± 0.40) × 10&lt;small&gt;&lt;sup&gt;−15&lt;/sup&gt;&lt;/small&gt; exp((2420 ± 340)/&lt;em&gt;T&lt;/em&gt;) cm&lt;small&gt;&lt;sup&gt;3&lt;/sup&gt;&lt;/small&gt; molecule&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; s&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt;, where rate&lt;small&gt;&lt;sub&gt;R2&lt;/sub&gt;&lt;/small&gt; = &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;[CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO][(H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O)&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;]. For use in atmospheric models, we recommend description of the kinetics for R2 in terms of the product of the rate coefficient &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; and the equilibrium constant &lt;em&gt;K&lt;/em&gt;&lt;small&gt;&lt;sup&gt;D&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;eq&lt;/sub&gt;&lt;/small&gt; (&lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2,eff&lt;/sub&gt;&lt;/small&gt; = &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;&lt;em&gt;K&lt;/em&gt;&lt;small&gt;&lt;sup&gt;D&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;eq&lt;/sub&gt;&lt;/small&gt;) for water dimer formation to allow the rate of reaction to be expressed in terms of water monomer concentration as rate&lt;small&gt;&lt;sub&gt;R2&lt;/sub&gt;&lt;/small&gt; = &lt;em&gt;k&lt;/em&gt;&lt;small&gt;&lt;sub&gt;2,eff&lt;/sub&gt;&lt;/small&gt;[CH&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;OO][H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O]&lt;small&gt;&lt;sup&gt;2&lt;/sup&gt;&lt;/small&gt; to avoid explicit calculation of dimer concentrations and impacts of differences in values of &lt;em&gt;K&lt;/em&gt;&lt;small&gt;&lt;sup&gt;D&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;eq&lt;/sub&gt;&lt;/small&gt; reported in the literature. Results from this work give &lt;em&gt;k&lt;/em&gt;&lt;small","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 11","pages":" 1294-1308"},"PeriodicalIF":2.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00097h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142595206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Immersion ice nucleation of atmospherically relevant lipid particles† 与大气相关的脂质颗粒的浸入式冰核形成†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-25 DOI: 10.1039/D4EA00066H
Lincoln Mehndiratta, Audrey E. Lyp, Jonathan H. Slade and Vicki H. Grassian

Ice nucleating particles (INPs) play a crucial role in freezing water droplets by acting as heterogeneous ice nuclei, influencing cloud phase state and climate dynamics. INPs from marine aerosol particles are particularly relevant. Saturated fatty alcohols and acids have been identified in sea spray aerosols (SSA). In this study, we employ a micro-Raman spectrometer integrated with an environmental cell to control relative humidity and temperature and measure the ice nucleation activity of individual lipid particles, including fatty alcohols and fatty acids of varying chain lengths. For fatty acids, we observe little IN activity for these lipid particles as they freeze close to the temperature found for homogeneous freezing. For fatty alcohols, we demonstrate that freezing temperatures depend on the carbon chain length, with longer chains leading to warmer ice nucleating temperatures. Although this result qualitatively agrees with existing literature, we observe that the ice nucleating temperatures of these lipid particles differ from the freezing temperatures measured for fatty alcohol monolayers at the air/water interface for large water droplets. To better understand these differences, we further investigate the effects of droplet size as well as phase state by theoretically determining the wet viscosity on freezing. Our results, taken together, suggest that for fatty alcohol particles, freezing occurs at the lipid particle/water interface. Overall, our findings highlight the influence of lipid chain length, droplet size, and phase state on ice nucleation for lipid particles.

冰核粒子(INPs)通过充当异质冰核在水滴冻结过程中发挥着至关重要的作用,影响着云相状态和气候动力学。来自海洋气溶胶颗粒的 INPs 尤其具有相关性。在海雾气溶胶(SSA)中发现了饱和脂肪醇和酸。在这项研究中,我们利用微拉曼光谱仪与环境电池集成来控制相对湿度和温度,并测量单个脂质颗粒的冰核活性,包括不同链长的脂肪醇和脂肪酸。对于脂肪酸,我们观察到这些脂质微粒几乎没有 IN 活性,因为它们的冻结温度接近均匀冻结时的温度。对于脂肪醇,我们证明冻结温度取决于碳链长度,碳链越长,冰核温度越高。虽然这一结果与现有文献的定性结果一致,但我们观察到这些脂质颗粒的冰核温度与脂肪醇单层在大水滴的空气/水界面上测得的冻结温度不同。为了更好地理解这些差异,我们通过理论测定冻结时的湿粘度,进一步研究了水滴大小和相态的影响。我们的研究结果表明,对于脂肪醇颗粒来说,冻结发生在脂质颗粒/水的界面上。总之,我们的研究结果凸显了脂质链长、液滴大小和相态对脂质颗粒冰核形成的影响。
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引用次数: 0
Particle number size distribution evaluation of Plantower PMS5003 low-cost PM sensors – a field experiment† Plantower PMS5003 低成本可吸入颗粒物传感器的粒度分布评估--现场实验†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-24 DOI: 10.1039/D4EA00086B
Alexandre Caseiro, Seán Schmitz and Erika von Schneidemesser

The use of low-cost sensors (LCS) for the evaluation of the ambient pollution by particulate matter (PM) has grown and become significant for the scientific community in the past few years. However promising this novel technology is, the characterization of their limitations is still not satisfactory. Reports in the scientific literature rely on calibration, which implies the physical (or geographical) co-location of the LCS with reference in situ (or remote, e.g. onboard satellite platforms) instrumentation. However, calibration is not always feasible, and even when feasible, the validity of the developed relationship, even in similar settings, is subject to large uncertainties. In the present work, the performance of a popular LCS for PM, the Plantower PMS5003, is investigated. The LCS performs particle counts, which is the physical quantity that is input to the black-box model of the manufacturer to compute the ambient PM mass, which is output to the operator. The particle counts of LCS Plantower PMS5003 units were compared to those of the co-located research-grade Grimm EDM-164 monitor. The results show that humidity possibly has a reduced influence on the performance, but the performance can better be constrained, however spanning more than one order of magnitude in terms of agreement ratio, by functions of the actual particle count itself. In view of these results, further development in the field of LCS for PM monitoring should focus on improvements of the physical design of the devices, in order to enhance the sizing of the particles. The use of the actual Plantower PMS5003 models should be limited to the monitoring of PM mass in the smaller size bins.

在过去几年里,使用低成本传感器(LCS)来评估环境颗粒物(PM)污染的情况越来越多,对科学界来说意义重大。尽管这项新技术前景广阔,但对其局限性的描述仍不尽人意。科学文献中的报告依赖于校准,这意味着将 LCS 与参考原地(或远程,如卫星平台上)仪器物理(或地理)同地定位。然而,校准并不总是可行的,即使可行,所建立关系的有效性,即使在类似的环境中,也会受到很大的不确定性影响。在本研究中,对一种常用的可吸入颗粒物 LCS(Plantower PMS5003)的性能进行了调查。该 LCS 可进行颗粒计数,这是输入到制造商黑盒模型中的物理量,用于计算环境 PM 质量,并将其输出给操作员。将 LCS Plantower PMS5003 设备的颗粒计数与同处的研究级 Grimm EDM-164 监测器的颗粒计数进行了比较。结果表明,湿度对性能的影响可能较小,但通过实际颗粒计数本身的功能,可以更好地限制性能,但在一致性比方面,差距超过一个数量级。鉴于这些结果,用于可吸入颗粒物监测的 LCS 领域的进一步发展应侧重于改进设备的物理设计,以提高颗粒的大小。实际使用的 Plantower PMS5003 型号应仅限于监测较小粒径范围内的可吸入颗粒物质量。
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引用次数: 0
Ozone formation potential related to the release of volatile organic compounds (VOCs) and nitrogen oxide (NOX) from a typical industrial park in the Pearl River Delta† 与珠江三角洲典型工业园区释放的挥发性有机化合物(VOCs)和氮氧化物(NOX)有关的臭氧形成潜力†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-20 DOI: 10.1039/D4EA00091A
Taicheng An, Jiajia Li, Qinhao Lin and Guiying Li

Ozone (O3) pollution has been recognized as the major air pollution in the Pearl River Delta (PRD) region, South China. Understanding O3 formation sensitive to volatile organic compound (VOC)- and nitrogen oxide (NOX)-limited regimes is a key step for alleviating O3 pollution. Herein, measurements of VOCs, NOX and O3 were simultaneously performed at multi sampling sites in an industrial park of the PRD region during June, 2020. VOCs/NOX ratios ranged from 0.5 to 5.7, suggesting that the O3 formation was in the VOC-limited regime in the industrial park. The estimated O3 formation potential (OFP) of VOCs showed that alkenes and aromatic hydrocarbons from motor vehicles and industrial sources contributed to 40% and 39% of the O3 formation, respectively, in the industrial park. However, a low O3 level (<50 ppb) was observed in the region where high OFP values (>194 ppb) were estimated. Further analysis found that the concentration of NOx (25 ± 10 ppb) in the high O3 region was lower than that (36 ± 6 ppb) in the low O3 region, mostly due to the titration reaction of NO and O3 to form NO2, therefore leading to the consumption of O3. This result implies that NOX control was not conducive to the O3 pollution in the study region. Thus, O3 pollution control in the study region should be taken into consideration in terms of the effect of NOX titration and control of VOC emissions.

臭氧(O3)污染已被认为是华南珠江三角洲(PRD)地区的主要空气污染。了解 O3 的形成对挥发性有机化合物(VOC)和氮氧化物(NOX)限制机制的敏感性是缓解 O3 污染的关键一步。在此,我们于 2020 年 6 月在珠三角地区一个工业园区的多个采样点同时测量了挥发性有机化合物、氮氧化物和臭氧。VOCs/NOX 比率介于 0.5 至 5.7 之间,表明该工业园区的 O3 形成受 VOC 限制。挥发性有机化合物的 O3 形成潜能估计值(OFP)显示,机动车和工业源产生的烯烃和芳香烃分别占工业园区 O3 形成的 40% 和 39%。然而,在估算出高 OFP 值(194 ppb)的区域,观测到的 O3 水平较低(50 ppb)。进一步分析发现,高 O3 区域的 NOx 浓度(25 ± 10 ppb)低于低 O3 区域的 NOx 浓度(36 ± 6 ppb),这主要是由于 NO 与 O3 发生滴定反应生成 NO2,从而导致 O3 的消耗。这一结果意味着 NOX 控制不利于研究区域的 O3 污染。因此,研究区域的 O3 污染控制应考虑 NOX 滴定和控制 VOC 排放的效果。
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引用次数: 0
Impact of atmospheric water-soluble iron on α-pinene-derived SOA formation and transformation in the presence of aqueous droplets† 大气中的水溶性铁对α-蒎烯衍生的 SOA 在水滴存在下的形成和转化的影响†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-14 DOI: 10.1039/D4EA00095A
Sabine Lüchtrath, Sven Klemer, Clément Dubois, Christian George and Andreas Held

The impact of water-soluble atmospheric iron on formation, growth and aging of secondary organic aerosol (SOA) is a controversial subject in the literature. Iron chemistry drives Fenton reactions in the aqueous phase which is dependent on pH. Flow reactor experiments in the dark and under humid conditions were conducted to investigate systematically the influence of ferrous iron in the aqueous phase on α-pinene SOA by online physical analysis and offline high-resolution mass spectrometry. During the experiments increased SOA formation under conditions favorable for dark Fenton chemistry in the aqueous phase was observed. Furthermore, samples with an acidified and iron-containing aqueous phase showed a degradation of pinyl-diaterpenyl (C17H26O8) ester which ages through oxidation via OH radicals and can thus be evidence for ongoing degradation processes of high molecular weight molecules by iron chemistry. Moreover, higher abundance of dimer MW338 (C19H30O5) in the acidic sample affected by Fenton's chemistry was detected which is suggested to be formed via acid catalysis indicating competing acidity-driven reactions influencing SOA formation. Therefore, this study provides insight into the impact of aqueous phase iron on SOA formation and transformation under simulated natural conditions.

水溶性大气铁对二次有机气溶胶(SOA)的形成、增长和老化的影响是文献中一个有争议的主题。铁的化学性质会驱动水相中的芬顿反应,而芬顿反应则取决于 pH 值。我们在黑暗和潮湿的条件下进行了流动反应器实验,通过在线物理分析和离线高分辨率质谱分析,系统地研究了水相中的亚铁对α-蒎烯 SOA 的影响。在实验过程中,观察到在有利于水相中暗芬顿化学反应的条件下,SOA 的形成有所增加。此外,酸化和含铁水相中的样品显示出蒎基-二萜(C17H26O8)酯的降解,这种降解是通过羟基自由基氧化老化的,因此可以证明铁化学作用正在对高分子量分子进行降解。此外,在受 Fenton 化学作用影响的酸性样品中检测到了较多的二聚体 MW338(C19H30O5),这表明二聚体是通过酸催化形成的,表明酸性驱动的竞争反应影响了 SOA 的形成。因此,这项研究有助于深入了解在模拟自然条件下,水相铁对 SOA 形成和转化的影响。
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引用次数: 0
Characterization of atmospheric microplastics in Hangzhou, a megacity of the Yangtze river delta, China† 中国长江三角洲特大城市杭州大气中微塑料的特征†。
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-08-23 DOI: 10.1039/D4EA00069B
Liang Xu, Jiefeng Li, Shushen Yang, Zhenyang Li, Yan Liu, Yifan Zhao, Dantong Liu, Admir Créso Targino, Zhonghua Zheng, Mingzhou Yu, Peng Xu, Yele Sun and Weijun Li

Microplastics (MPs) have become a key environmental issue over the last few decades. However, while previous studies have mainly focused on aquatic MP pollution, research on atmospheric MPs remains limited. To expand our knowledge of atmospheric MPs, we collected atmospheric samples using active and dry deposition techniques during one year in an urban environment in the megacity of Hangzhou, China. MPs were identified in the samples using a range of analytical and optical techniques. The concentrations of MPs on the filters collected using active sampling ranged from 0.37–8.9 particles per m3, with an annual mean of 3.2 ± 0.5 particles per m3. The dry deposition rate of atmospheric MPs ranged from 441.18–3181.8 particles per m2 per day, with an annual mean of 1387.8 ± 237.7 particles per m2 per day. Fiber MPs were the most predominant type while a few film-type MPs were identified. Raman microspectrometer analysis identified that tires (27.0% of MPs) and polyethylene terephthalate (PET, 19.7% of MPs) were the dominant MP types. Finally, we estimated that the annual dry deposition rate of MPs in the Hangzhou urban area was 16.9 ± 2.9 tons. Exploring the abundance and deposition of MPs helps to evaluate their potential threat to human health or aquatic ecology, which finally contributes to development of MP control measures.

过去几十年来,微塑料(MPs)已成为一个关键的环境问题。然而,以往的研究主要集中在水生 MP 污染方面,对大气中 MP 的研究仍然有限。为了扩大我们对大气中 MPs 的了解,我们在中国杭州特大城市的城市环境中使用主动沉积和干沉积技术收集了一年的大气样本。我们使用一系列分析和光学技术对样本中的多溴联苯进行了鉴定。使用主动采样收集的过滤器上的多溴联苯醚浓度范围为每立方米 0.37-8.9 个颗粒,年平均值为每立方米 3.2 ± 0.5 个颗粒。大气中多颗粒物的干沉降率为每天每平方米 441.18-3181.8 个颗粒,年平均值为每天每平方米 1387.8 ± 237.7 个颗粒。最主要的颗粒类型是纤维 MPs,同时也发现了一些薄膜型 MPs。拉曼光谱仪分析表明,轮胎(占 MPs 的 27.0%)和聚对苯二甲酸乙二酯(PET,占 MPs 的 19.7%)是主要的 MP 类型。最后,我们估计杭州城区每年的干物质沉积率为 16.9 ± 2.9 吨。探索多溴联苯醚的丰度和沉积情况有助于评估其对人类健康或水生生态的潜在威胁,最终有助于制定多溴联苯醚控制措施。
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引用次数: 0
Increasing the Earth's albedo: the Köhler equation at sea 增加地球的反照率:海上的科勒方程
IF 2.8 Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-08-23 DOI: 10.1039/D4EA00073K
J. I. Katz

Increasing marine haze and clouds has been considered as a possible means of increasing the Earth's albedo. This would reduce solar heating and global warming, counteracting the effects of the anthropogenic increase in greenhouse gases. One proposed method of doing so would inject small droplets of seawater or condensation nuclei into the marine boundary layer, creating artificial haze and cloud. The equilibrium size of such droplets is described by the Köhler equation that includes the vapor pressure reduction attributable to the solute according to Raoult's law and the vapor pressure increase of a small droplet as a result of surface tension according to Kelvin. Here we apply this classic result to small droplets in the marine boundary layer, where the partial pressure of water vapor is less than the equilibrium vapor pressure because it is in equilibrium with the saline ocean. We calculate the equilibrium size of a droplet containing dissolved ions and find that the radius of a droplet of seawater shrinks greatly before it achieves equilibrium.

增加海洋雾霾和云层被认为是增加地球反照率的一种可能手段。这将减少太阳辐射热和全球变暖,抵消温室气体人为增加的影响。其中一种拟议的方法是向海洋边界层注入海水小液滴或凝结核,制造人造雾霾和云层。这种液滴的平衡大小由科勒方程描述,其中包括根据拉乌尔定律由溶质引起的蒸汽压降低和根据开尔文定律由表面张力引起的小液滴蒸汽压升高。在这里,我们将这一经典结果应用于海洋边界层中的小水滴,在海洋边界层中,水蒸气分压小于平衡水蒸气压,因为它与含盐海洋处于平衡状态。我们计算了含有溶解离子的水滴的平衡尺寸,发现海水水滴的半径在达到平衡之前会大大缩小。
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引用次数: 0
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Environmental science: atmospheres
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