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).
{"title":"Trace elements in PM2.5 shed light on Saharan dust incursions over the Munich airshed in spring 2022†","authors":"Sara Padoan, Alessandro Zappi, Jan Bendl, Tanja Herrmann, Ajit Mudan, Carsten Neukirchen, Erika Brattich, Laura Tositti and Thomas Adam","doi":"10.1039/D4EA00092G","DOIUrl":"https://doi.org/10.1039/D4EA00092G","url":null,"abstract":"<p >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 (<em>e.g.</em> Al, Mg, Ca) and anthropogenic (<em>e.g.</em> 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).</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 11","pages":" 1266-1282"},"PeriodicalIF":2.8,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00092g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142595204","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}
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.
{"title":"Evaluating emissions and meteorological contributions to air quality trends in northern China based on measurements at a regional background station†","authors":"Weiwei Pu, Yingruo Li, Xiaowan Zhu, Xiangxue Liu, Di He, Fan Dong, Heng Guo, Guijie Zhao, Liyan Zhou, Shuangshuang Ge and Zhiqiang Ma","doi":"10.1039/D4EA00070F","DOIUrl":"https://doi.org/10.1039/D4EA00070F","url":null,"abstract":"<p >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 PM<small><sub>2.5</sub></small>, NO<small><sub>2</sub></small>, SO<small><sub>2</sub></small>, O<small><sub>3</sub></small>, and CO pollution during 2013–2021 and evaluated their contributions to Clean Air Action policies. The annual effect of the meteorology on PM<small><sub>2.5</sub></small>, NO<small><sub>2</sub></small>, SO<small><sub>2</sub></small>, and CO levels was dominated by the meteorological conditions during the cold season, while that of the O<small><sub>3</sub></small> 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 PM<small><sub>2.5</sub></small>, NO<small><sub>2</sub></small>, SO<small><sub>2</sub></small>, O<small><sub>3</sub></small>, 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<small><sup>−3</sup></small> year<small><sup>−1</sup></small>, 0.2 μg m<small><sup>−3</sup></small> year<small><sup>−1</sup></small>, 1.5 μg m<small><sup>−3</sup></small> year<small><sup>−1</sup></small>, 0.7 μg m<small><sup>−3</sup></small> year<small><sup>−1</sup></small>, and 0.03 mg m<small><sup>−3</sup></small> year<small><sup>−1</sup></small> for PM<small><sub>2.5</sub></small>, NO<small><sub>2</sub></small>, SO<small><sub>2</sub></small>, O<small><sub>3</sub></small>, 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 O<small><sub>3</sub></small>. 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.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 11","pages":" 1283-1293"},"PeriodicalIF":2.8,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00070f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142595205","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}
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。
{"title":"Determination of mass concentrations of airborne PET microplastics using liquid chromatography coupled to tandem mass spectrometry (LC-MS/MS)†","authors":"Durga Prasad Patnana and B. P. Chandra","doi":"10.1039/D4EA00047A","DOIUrl":"https://doi.org/10.1039/D4EA00047A","url":null,"abstract":"<p >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 (PM<small><sub>2.5</sub></small>) 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 PM<small><sub>2.5</sub></small>. The observed maximum mass concentrations of PET MPs in airborne PM<small><sub>2.5</sub></small> in Delhi and Mohali are 135.20 ng m<small><sup>−3</sup></small> and 157.98 ng m<small><sup>−3</sup></small>, respectively.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 12","pages":" 1352-1357"},"PeriodicalIF":2.8,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00047a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778036","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}
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
{"title":"Kinetics of the reactions of the Criegee intermediate CH2OO with water vapour: experimental measurements as a function of temperature and global atmospheric modelling†","authors":"Rachel E. Lade, Mark A. Blitz, Matthew Rowlinson, Mathew J. Evans, Paul W. Seakins and Daniel Stone","doi":"10.1039/D4EA00097H","DOIUrl":"https://doi.org/10.1039/D4EA00097H","url":null,"abstract":"<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","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}
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。
{"title":"Immersion ice nucleation of atmospherically relevant lipid particles†","authors":"Lincoln Mehndiratta, Audrey E. Lyp, Jonathan H. Slade and Vicki H. Grassian","doi":"10.1039/D4EA00066H","DOIUrl":"https://doi.org/10.1039/D4EA00066H","url":null,"abstract":"<p >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.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 11","pages":" 1239-1254"},"PeriodicalIF":2.8,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00066h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142595202","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}
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.
{"title":"Particle number size distribution evaluation of Plantower PMS5003 low-cost PM sensors – a field experiment†","authors":"Alexandre Caseiro, Seán Schmitz and Erika von Schneidemesser","doi":"10.1039/D4EA00086B","DOIUrl":"https://doi.org/10.1039/D4EA00086B","url":null,"abstract":"<p >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 <em>in situ</em> (or remote, <em>e.g.</em> 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.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 10","pages":" 1183-1194"},"PeriodicalIF":2.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00086b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142397523","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}
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.
{"title":"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†","authors":"Taicheng An, Jiajia Li, Qinhao Lin and Guiying Li","doi":"10.1039/D4EA00091A","DOIUrl":"https://doi.org/10.1039/D4EA00091A","url":null,"abstract":"<p >Ozone (O<small><sub>3</sub></small>) pollution has been recognized as the major air pollution in the Pearl River Delta (PRD) region, South China. Understanding O<small><sub>3</sub></small> formation sensitive to volatile organic compound (VOC)- and nitrogen oxide (NO<small><sub>X</sub></small>)-limited regimes is a key step for alleviating O<small><sub>3</sub></small> pollution. Herein, measurements of VOCs, NO<small><sub>X</sub></small> and O<small><sub>3</sub></small> were simultaneously performed at multi sampling sites in an industrial park of the PRD region during June, 2020. VOCs/NO<small><sub>X</sub></small> ratios ranged from 0.5 to 5.7, suggesting that the O<small><sub>3</sub></small> formation was in the VOC-limited regime in the industrial park. The estimated O<small><sub>3</sub></small> formation potential (OFP) of VOCs showed that alkenes and aromatic hydrocarbons from motor vehicles and industrial sources contributed to 40% and 39% of the O<small><sub>3</sub></small> formation, respectively, in the industrial park. However, a low O<small><sub>3</sub></small> 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 O<small><sub>3</sub></small> region was lower than that (36 ± 6 ppb) in the low O<small><sub>3</sub></small> region, mostly due to the titration reaction of NO and O<small><sub>3</sub></small> to form NO<small><sub>2</sub></small>, therefore leading to the consumption of O<small><sub>3</sub></small>. This result implies that NO<small><sub>X</sub></small> control was not conducive to the O<small><sub>3</sub></small> pollution in the study region. Thus, O<small><sub>3</sub></small> pollution control in the study region should be taken into consideration in terms of the effect of NO<small><sub>X</sub></small> titration and control of VOC emissions.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 11","pages":" 1229-1238"},"PeriodicalIF":2.8,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00091a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142595201","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}
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。
{"title":"Impact of atmospheric water-soluble iron on α-pinene-derived SOA formation and transformation in the presence of aqueous droplets†","authors":"Sabine Lüchtrath, Sven Klemer, Clément Dubois, Christian George and Andreas Held","doi":"10.1039/D4EA00095A","DOIUrl":"https://doi.org/10.1039/D4EA00095A","url":null,"abstract":"<p >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 (C<small><sub>17</sub></small>H<small><sub>26</sub></small>O<small><sub>8</sub></small>) ester which ages through oxidation <em>via</em> 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 (C<small><sub>19</sub></small>H<small><sub>30</sub></small>O<small><sub>5</sub></small>) in the acidic sample affected by Fenton's chemistry was detected which is suggested to be formed <em>via</em> 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.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 11","pages":" 1218-1228"},"PeriodicalIF":2.8,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00095a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142595200","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}
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.
{"title":"Characterization of atmospheric microplastics in Hangzhou, a megacity of the Yangtze river delta, China†","authors":"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","doi":"10.1039/D4EA00069B","DOIUrl":"https://doi.org/10.1039/D4EA00069B","url":null,"abstract":"<p >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 m<small><sup>3</sup></small>, with an annual mean of 3.2 ± 0.5 particles per m<small><sup>3</sup></small>. The dry deposition rate of atmospheric MPs ranged from 441.18–3181.8 particles per m<small><sup>2</sup></small> per day, with an annual mean of 1387.8 ± 237.7 particles per m<small><sup>2</sup></small> 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.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 10","pages":" 1161-1169"},"PeriodicalIF":2.8,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00069b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142397521","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}
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.
{"title":"Increasing the Earth's albedo: the Köhler equation at sea","authors":"J. I. Katz","doi":"10.1039/D4EA00073K","DOIUrl":"https://doi.org/10.1039/D4EA00073K","url":null,"abstract":"<p >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.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 10","pages":" 1157-1160"},"PeriodicalIF":2.8,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00073k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142397520","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}