Wind-blown dust can affect the acidity of all particles, impacting a series of related chemical processes. In this work, we use a wind-blown dust emissions model along with the hybrid version of aerosol dynamics in the PMCAMx chemical transport model to quantify the effects of dust on size-resolved aerosol pH over the U.S during February and July 2017 as a function of altitude. The version of the model used can capture the most important range of pH values (less than 5), while particles that are more alkaline than this threshold are assumed to have pH equal to 5. Our simulations indicate that wind-blown dust can increase ground level PM1 pH up to 1 unit during wintertime and up to 3.5 units during summertime in the western U.S. For PM1−2.5, the corresponding increases are higher during wintertime (up to 1.5 units) and a little lower during summertime (up to 3 units) compared to PM1. For coarse particles (PM2.5−5 and PM5−10), the impact of wind-blown dust is predicted to be lower since in most areas the corresponding pH is already quite high due to the presence of dust from anthropogenic activities (e.g., agriculture, resuspension due to traffic). The impact of wind-blown dust on aerosol acidity decreases with altitude for PM1 mainly because of the reduction of aerosol water. On the other hand, for PM1−2.5, the predicted effect increases with altitude due to the lower pH at higher altitudes. PM1 and PM1−2.5 acidity can be affected significantly by wind-blown dust for both simulated periods impacting at the same time secondary aerosol formation, emissions control strategies, solubility of metals, and nitrogen deposition.
{"title":"Effects of wind-blown dust emissions on size-resolved aerosol acidity over the US","authors":"Stylianos Kakavas , Evangelia Siouti , Athanasios Nenes , Spyros N. Pandis","doi":"10.1016/j.atmosenv.2025.121056","DOIUrl":"10.1016/j.atmosenv.2025.121056","url":null,"abstract":"<div><div>Wind-blown dust can affect the acidity of all particles, impacting a series of related chemical processes. In this work, we use a wind-blown dust emissions model along with the hybrid version of aerosol dynamics in the PMCAMx chemical transport model to quantify the effects of dust on size-resolved aerosol pH over the U.S during February and July 2017 as a function of altitude. The version of the model used can capture the most important range of pH values (less than 5), while particles that are more alkaline than this threshold are assumed to have pH equal to 5. Our simulations indicate that wind-blown dust can increase ground level PM<sub>1</sub> pH up to 1 unit during wintertime and up to 3.5 units during summertime in the western U.S. For PM<sub>1−2.5</sub>, the corresponding increases are higher during wintertime (up to 1.5 units) and a little lower during summertime (up to 3 units) compared to PM<sub>1</sub>. For coarse particles (PM<sub>2.5−5</sub> and PM<sub>5−10</sub>), the impact of wind-blown dust is predicted to be lower since in most areas the corresponding pH is already quite high due to the presence of dust from anthropogenic activities (e.g., agriculture, resuspension due to traffic). The impact of wind-blown dust on aerosol acidity decreases with altitude for PM<sub>1</sub> mainly because of the reduction of aerosol water. On the other hand, for PM<sub>1−2.5</sub>, the predicted effect increases with altitude due to the lower pH at higher altitudes. PM<sub>1</sub> and PM<sub>1−2.5</sub> acidity can be affected significantly by wind-blown dust for both simulated periods impacting at the same time secondary aerosol formation, emissions control strategies, solubility of metals, and nitrogen deposition.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"345 ","pages":"Article 121056"},"PeriodicalIF":4.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143277104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-20DOI: 10.1016/j.atmosenv.2025.121058
Prachi Goyal, Sunil Gulia, S.K. Goyal
The application of diverse methods/tools (satellite data, ground-based monitoring and dispersion modelling) for quantitative assessment of air pollution has created a critical challenge for policymakers, in understating the actual stubble burning contribution in North Indian states including Punjab, Haryana, Delhi and western Uttar Pradesh. Considering the variations in monitoring sites, quantified emissions, satellite data resolutions, parameterization schemes, meteorology and/or adopted models, huge differences in the source contribution are reported. Considering these ambiguities, the present study is an attempt to review the studies revealing actual paddy stubble burning contribution to air quality of Delhi conducted year 2015 onwards; one year before the severe episodic smog event of November 2016. A total of 114 articles were searched using different keywords for subsequent in-depth analysis. The biomass burning share was broadly studied for winter, summer and post-monsoon seasons. Further, to understand the season-specific nature of the paddy stubble burning activity, the analysis was restricted to post-monsoon months. A co-occurrence keyword network analysis was performed based on which biomass/stubble burning related studies were divided into three clusters based on i) source apportionment using receptor modeling, ii) satellite data (AOD values coupled with ground-based observation and wind back trajectory and, iii) regional scale chemical transport modeling approach. Some studies were generalized displaying correlation patterns, some used only fire count data and correlated with AOD while some used either satellite data or regional scale models. Learning from the gap analysis of the reviewed studies led to the development of an integrated assessment protocol to quantify the stubble-burning contribution in the region.
{"title":"Critical review of air pollution contribution in Delhi due to paddy stubble burning in North Indian States","authors":"Prachi Goyal, Sunil Gulia, S.K. Goyal","doi":"10.1016/j.atmosenv.2025.121058","DOIUrl":"10.1016/j.atmosenv.2025.121058","url":null,"abstract":"<div><div>The application of diverse methods/tools (satellite data, ground-based monitoring and dispersion modelling) for quantitative assessment of air pollution has created a critical challenge for policymakers, in understating the actual stubble burning contribution in North Indian states including Punjab, Haryana, Delhi and western Uttar Pradesh. Considering the variations in monitoring sites, quantified emissions, satellite data resolutions, parameterization schemes, meteorology and/or adopted models, huge differences in the source contribution are reported. Considering these ambiguities, the present study is an attempt to review the studies revealing actual paddy stubble burning contribution to air quality of Delhi conducted year 2015 onwards; one year before the severe episodic smog event of November 2016. A total of 114 articles were searched using different keywords for subsequent in-depth analysis. The biomass burning share was broadly studied for winter, summer and post-monsoon seasons. Further, to understand the season-specific nature of the paddy stubble burning activity, the analysis was restricted to post-monsoon months. A co-occurrence keyword network analysis was performed based on which biomass/stubble burning related studies were divided into three clusters based on i) source apportionment using receptor modeling, ii) satellite data (AOD values coupled with ground-based observation and wind back trajectory and, iii) regional scale chemical transport modeling approach. Some studies were generalized displaying correlation patterns, some used only fire count data and correlated with AOD while some used either satellite data or regional scale models. Learning from the gap analysis of the reviewed studies led to the development of an integrated assessment protocol to quantify the stubble-burning contribution in the region.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"346 ","pages":"Article 121058"},"PeriodicalIF":4.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143317426","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-20DOI: 10.1016/j.atmosenv.2025.121053
Hye-Ji Lee , Hyo-Won Lee , Sung-Won Park , Ji-Won Jeon , Pyung-Rae Kim , Kyung-Hwan Kwak , Young-Ji Han , Thomas M. Holsen , Seung-Ha Lee , Hyun-Gu Jung , Seung-Hwan Cha , Jung-Min Park , Myung-Soo Yoo
Organic matter is often the largest contributor to PM2.5, but its emission sources and formation pathways are very diverse, making it challenging to identify the causes of high concentration episodes. In this study, four groups of organic compounds that contribute to PM2.5, including sugars, dicarboxylic acids (DA), fatty acids (FA), and pinonic acid (PNA) were measured in a medium-sized residential city in South Korea during three seasons, where high PM2.5 concentration episodes often occur. The average concentrations of PM2.5 and total quantified organic matter (∑17 qOM) was 21 ± 12 μg m−3 and 391 ± 183 ng m−3, respectively. The concentration of ∑sugars was higher during the colder seasons compared to the warm season (32 ± 18 ng m−3, 240 ± 109 ng m−3, and 231 ± 105 ng m−3 in the warm, transition, and cold seasons, respectively). In contrast, ∑DAs exhibited the opposite seasonal trend (234 ± 164 ng m−3, 114 ± 103 ng m−3, and 140 ± 103 ng m−3 in the warm, transition, and cold seasons, respectively). The contribution of ∑FA to qOM was relatively consistent (13.1% in warm season to 15.6% in colder seasons). PNA, a biogenic secondary organic aerosol tracer, had a significantly higher concentration during the warm season (16 ± 13 ng m−3 in warm season vs. 3 ± 3 ng m−3 in colder seasons). A strong correlation between ∑sugars and ∑FAs (r = 0.72) was observed only in the transition season, when crop residue burning was determined to be important. Unsaturated FAs were likely to be efficiently aged during the cold season since the ratio of C18:0 to C18:1, a tracer for the age of aerosol, increased. DAs were generally dominant in the warm season, but also significantly increased during most high PM2.5 concentration episodes (HCEs; 306 ± 199 ng m−3), which primarily occurred in the colder season. During HCEs appearing in colder season, the ratio of malonic acid (C3) to succinic acid (C4), a tracer for photochemical aging of air masses, also increased, suggesting that the secondary aerosol formation and aerosol aging significantly enhanced PM2.5 concentration.
{"title":"Characteristics of elevated PM2.5 events driven by enhanced organic compound concentrations in a South Korean residential city","authors":"Hye-Ji Lee , Hyo-Won Lee , Sung-Won Park , Ji-Won Jeon , Pyung-Rae Kim , Kyung-Hwan Kwak , Young-Ji Han , Thomas M. Holsen , Seung-Ha Lee , Hyun-Gu Jung , Seung-Hwan Cha , Jung-Min Park , Myung-Soo Yoo","doi":"10.1016/j.atmosenv.2025.121053","DOIUrl":"10.1016/j.atmosenv.2025.121053","url":null,"abstract":"<div><div>Organic matter is often the largest contributor to PM<sub>2.5</sub>, but its emission sources and formation pathways are very diverse, making it challenging to identify the causes of high concentration episodes. In this study, four groups of organic compounds that contribute to PM<sub>2.5</sub>, including sugars, dicarboxylic acids (DA), fatty acids (FA), and pinonic acid (PNA) were measured in a medium-sized residential city in South Korea during three seasons, where high PM<sub>2.5</sub> concentration episodes often occur. The average concentrations of PM<sub>2.5</sub> and total quantified organic matter (∑17 qOM) was 21 ± 12 μg m<sup>−3</sup> and 391 ± 183 ng m<sup>−3</sup>, respectively. The concentration of ∑sugars was higher during the colder seasons compared to the warm season (32 ± 18 ng m<sup>−3</sup>, 240 ± 109 ng m<sup>−3</sup>, and 231 ± 105 ng m<sup>−3</sup> in the warm, transition, and cold seasons, respectively). In contrast, ∑DAs exhibited the opposite seasonal trend (234 ± 164 ng m<sup>−3</sup>, 114 ± 103 ng m<sup>−3</sup>, and 140 ± 103 ng m<sup>−3</sup> in the warm, transition, and cold seasons, respectively). The contribution of ∑FA to qOM was relatively consistent (13.1% in warm season to 15.6% in colder seasons). PNA, a biogenic secondary organic aerosol tracer, had a significantly higher concentration during the warm season (16 ± 13 ng m<sup>−3</sup> in warm season vs. 3 ± 3 ng m<sup>−3</sup> in colder seasons). A strong correlation between ∑sugars and ∑FAs (r = 0.72) was observed only in the transition season, when crop residue burning was determined to be important. Unsaturated FAs were likely to be efficiently aged during the cold season since the ratio of C<sub>18:0</sub> to C<sub>18:1</sub>, a tracer for the age of aerosol, increased. DAs were generally dominant in the warm season, but also significantly increased during most high PM<sub>2.5</sub> concentration episodes (HCEs; 306 ± 199 ng m<sup>−3</sup>), which primarily occurred in the colder season. During HCEs appearing in colder season, the ratio of malonic acid (C<sub>3</sub>) to succinic acid (C<sub>4</sub>), a tracer for photochemical aging of air masses, also increased, suggesting that the secondary aerosol formation and aerosol aging significantly enhanced PM<sub>2.5</sub> concentration.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"345 ","pages":"Article 121053"},"PeriodicalIF":4.2,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143277170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-13DOI: 10.1016/j.atmosenv.2025.121050
Suzana Sopčić, Ivana Jakovljević, Zdravka Sever Štrukil, Ivan Bešlić
This study examines the levels and seasonal changes of organic compounds in terms of carbohydrates and polycyclic aromatic hydrocarbons (PAHs) in PM10 collected at a rural site near the Plitvice Lake National Park (Croatia) to determine their source in airborne particles. Mass concentrations of PM10 particles were higher during the summer compared to the winter season (14 ± 5.3 μg m−3 and 6 ± 3.4 μg m−3, respectively). Such seasonal variation is unusual for this part of Europe, where the winters are harsh and biomass for domestic heating is most common. The analysis of carbohydrates in PM10 revealed the presence of anhydrosugars, sugar alcohols, and monosaccharides throughout the sampling period. Anhydrosugars were the most dominant compounds despite the season. The highest average mass concentrations of 124.1 ± 100.06 ng m−3, 8.0 ± 5.55 ng m−3, and 7.0 ± 7.62 ng m−3 for levoglucosan (LG), mannosan (MNS), and galactosan (GA), respectively, were reached in the winter season. Sugar alcohols were most pronounced during the summer, while the levels of monosaccharides contributed evenly through autumn and summer. The levels of PAHs were higher during winter and lowest during the summer season. Their concentrations in PM10 were at least one order of magnitude smaller compared to carbohydrate concentrations. The highest average mass concentration was observed for benzo(b)fluoranthene (BbF) in spring (0.126 ± 0.068 ng m−3), pyrene (Pyr) in summer (0.038 ± 0.013 ng m−3), benzo(ghi)perylene (BghiP) in autumn (0.153 ± 0.107 ng m−3) and BbF in winter (0.283 ± 0.259 ng m−3). The annual average mass concentration of BaP was 0.086 ± 0.1028 ng m−3, which is lower than the European Union (EU) directive target value of 1 ng m−3. To determine the sources of organic compounds in airborne particles, different multi-statistical techniques were used; Spearman correlation, factor analysis, principal Component Analysis (PCA), as well as diagnostic ratio method, revealing the seasonal dynamics of various sources. The reason for these changes can be found in different human and nature activities in the rural background area. Data analyses indicated that in the spring season, there were mixed sources, including traffic, emissions from domestic heating or the combustion of grass/agricultural waste, and biogenic aerosols. In the summer, the dominant sources were biogenic emissions related to fungi spores and degraded material, biomass burning, and traffic. Vehicular emissions and biogenic sources were likely dominant at Plitvice Lakes during autumn, whereas domestic heating was the dominant source in the studied area during winter.
{"title":"Source identification of carbohydrates and polycyclic aromatic hydrocarbons in a rural area near the Plitvice Lakes National Park, Croatia","authors":"Suzana Sopčić, Ivana Jakovljević, Zdravka Sever Štrukil, Ivan Bešlić","doi":"10.1016/j.atmosenv.2025.121050","DOIUrl":"10.1016/j.atmosenv.2025.121050","url":null,"abstract":"<div><div>This study examines the levels and seasonal changes of organic compounds in terms of carbohydrates and polycyclic aromatic hydrocarbons (PAHs) in PM<sub>10</sub> collected at a rural site near the Plitvice Lake National Park (Croatia) to determine their source in airborne particles. Mass concentrations of PM<sub>10</sub> particles were higher during the summer compared to the winter season (14 ± 5.3 μg m<sup>−3</sup> and 6 ± 3.4 μg m<sup>−3</sup>, respectively). Such seasonal variation is unusual for this part of Europe, where the winters are harsh and biomass for domestic heating is most common. The analysis of carbohydrates in PM<sub>10</sub> revealed the presence of anhydrosugars, sugar alcohols, and monosaccharides throughout the sampling period. Anhydrosugars were the most dominant compounds despite the season. The highest average mass concentrations of 124.1 ± 100.06 ng m<sup>−3</sup>, 8.0 ± 5.55 ng m<sup>−3</sup>, and 7.0 ± 7.62 ng m<sup>−3</sup> for levoglucosan (LG), mannosan (MNS), and galactosan (GA), respectively, were reached in the winter season. Sugar alcohols were most pronounced during the summer, while the levels of monosaccharides contributed evenly through autumn and summer. The levels of PAHs were higher during winter and lowest during the summer season. Their concentrations in PM<sub>10</sub> were at least one order of magnitude smaller compared to carbohydrate concentrations. The highest average mass concentration was observed for benzo(b)fluoranthene (BbF) in spring (0.126 ± 0.068 ng m<sup>−3</sup>), pyrene (Pyr) in summer (0.038 ± 0.013 ng m<sup>−3</sup>), benzo(ghi)perylene (BghiP) in autumn (0.153 ± 0.107 ng m<sup>−3</sup>) and BbF in winter (0.283 ± 0.259 ng m<sup>−3</sup>). The annual average mass concentration of BaP was 0.086 ± 0.1028 ng m<sup>−3</sup>, which is lower than the European Union (EU) directive target value of 1 ng m<sup>−3</sup>. To determine the sources of organic compounds in airborne particles, different multi-statistical techniques were used; Spearman correlation, factor analysis, principal Component Analysis (PCA), as well as diagnostic ratio method, revealing the seasonal dynamics of various sources. The reason for these changes can be found in different human and nature activities in the rural background area. Data analyses indicated that in the spring season, there were mixed sources, including traffic, emissions from domestic heating or the combustion of grass/agricultural waste, and biogenic aerosols. In the summer, the dominant sources were biogenic emissions related to fungi spores and degraded material, biomass burning, and traffic. Vehicular emissions and biogenic sources were likely dominant at Plitvice Lakes during autumn, whereas domestic heating was the dominant source in the studied area during winter.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"345 ","pages":"Article 121050"},"PeriodicalIF":4.2,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143277271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-13DOI: 10.1016/j.atmosenv.2025.121047
D.A. Carnelos , M. Poca , E. Jobbagy , G. Piñeiro
Regional patterns and sources of wet atmospheric deposition are an important aspect of biogeochemical cycling. The isotopic composition of wet atmospheric deposition samples can serve as a characteristic marker, dependent on local geographical and meteorological factors, providing valuable information about the spatial and temporal origins of rainwater and its chemical load. This study aimed to characterize the δ18O and δ2H isotopic composition of rainfall events to evaluate the relative contribution of different possible origins of precipitated moisture and its relationship with the potential origin of ions (Na+, Cl−, Mg2+, SO42−, Ca2+, K+, NO3− and NH4+) in wet atmospheric deposition samples collected from four sites within the Río de la Plata basin region in South America during 2007. Our results revealed significant variability in the isotopic and ionic concentrations among different rainfall events at each site (temporal variability overwhelmed spatial variability). Most ions appeared to share a common origin with the moisture that carried them before deposition. The isotopic values of δ18O and δ2H were primarily influenced by the distance from the ocean, the origin of humidity sources, and, to a lesser extent, the magnitude of rainfall. The average deuterium excess values (10.95‰) suggested that a substantial portion of the rainfall during the study period originated in the Atlantic Ocean rather than from recycling from the Amazon basin. Events with more negative δ18O-values (i.e. more depleted events) appeared to be predominantly oceanic, characterized by higher amounts of Na+, Cl− and Mg2+. Conversely, events with more positive δ18O-values (i.e. more enriched events) exhibited increased concentrations of terrestrial ions, including K+, NO3− and NH4+, indicating an inland moisture source. No clear association was found for SO42− and Ca2+ and rainfall isotopic composition. Hysplit back trajectory analyses showed that air masses traveling across the ocean contain higher amounts of marine ions like Na+ and Cl−. Conversely, air masses transported across the continent incorporated higher amounts of ions with terrestrial origins, such as NO3− and NH4+.Our findings suggest a tight coupling between moisture, ion sources and air mass trajectories in the Río de la Plata basin region.
{"title":"Characterizing moisture origins and ionic contributions in wet deposition samples from the Río de la Plata basin","authors":"D.A. Carnelos , M. Poca , E. Jobbagy , G. Piñeiro","doi":"10.1016/j.atmosenv.2025.121047","DOIUrl":"10.1016/j.atmosenv.2025.121047","url":null,"abstract":"<div><div>Regional patterns and sources of wet atmospheric deposition are an important aspect of biogeochemical cycling. The isotopic composition of wet atmospheric deposition samples can serve as a characteristic marker, dependent on local geographical and meteorological factors, providing valuable information about the spatial and temporal origins of rainwater and its chemical load. This study aimed to characterize the δ<sup>18</sup>O and δ<sup>2</sup>H isotopic composition of rainfall events to evaluate the relative contribution of different possible origins of precipitated moisture and its relationship with the potential origin of ions (Na<sup>+</sup>, Cl<sup>−</sup>, Mg<sup>2+</sup>, SO<sub>4</sub><sup>2−</sup>, Ca<sup>2+</sup>, K<sup>+</sup>, NO<sub>3</sub><sup>−</sup> and NH<sub>4</sub><sup>+</sup>) in wet atmospheric deposition samples collected from four sites within the Río de la Plata basin region in South America during 2007. Our results revealed significant variability in the isotopic and ionic concentrations among different rainfall events at each site (temporal variability overwhelmed spatial variability). Most ions appeared to share a common origin with the moisture that carried them before deposition. The isotopic values of δ<sup>18</sup>O and δ<sup>2</sup>H were primarily influenced by the distance from the ocean, the origin of humidity sources, and, to a lesser extent, the magnitude of rainfall. The average deuterium excess values (10.95‰) suggested that a substantial portion of the rainfall during the study period originated in the Atlantic Ocean rather than from recycling from the Amazon basin. Events with more negative δ<sup>18</sup>O-values (i.e. more depleted events) appeared to be predominantly oceanic, characterized by higher amounts of Na<sup>+</sup>, Cl<sup>−</sup> and Mg<sup>2+</sup>. Conversely, events with more positive δ<sup>18</sup>O-values (i.e. more enriched events) exhibited increased concentrations of terrestrial ions, including K<sup>+</sup>, NO<sub>3</sub><sup>−</sup> and NH<sub>4</sub><sup>+</sup>, indicating an inland moisture source. No clear association was found for SO<sub>4</sub><sup>2−</sup> and Ca<sup>2+</sup> and rainfall isotopic composition. Hysplit back trajectory analyses showed that air masses traveling across the ocean contain higher amounts of marine ions like Na<sup>+</sup> and Cl<sup>−</sup>. Conversely, air masses transported across the continent incorporated higher amounts of ions with terrestrial origins, such as NO<sub>3</sub><sup>−</sup> and NH<sub>4</sub><sup>+</sup>.Our findings suggest a tight coupling between moisture, ion sources and air mass trajectories in the Río de la Plata basin region.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"345 ","pages":"Article 121047"},"PeriodicalIF":4.2,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143277263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Air pollution is one of the most harmful consequences of industrialization because of its strong influence on both human health quality and climate in general. Often there appears a need to identify one single strong source of air pollution appearing as a result of an accident. In this paper, we propose a new algorithm for a single pollution source localization. The proposed algorithm uses the source–receptor matrix concept and assumption about the linearity of pollution transport that allows us to use the pollution spread simulations backward in time. In particular realization, we make use of the weather regional forecast model WRF for airflow simulation and of Lagrangian particle dispersion simulation software FLEXPART-WRF for pollution advection simulation both forward and backward in time. As a result, our algorithm produces the semi-empirical heatmap of possible pollution source locations with marked point of the biggest probability and estimative emission intensity at this point as a function of time. The algorithm is tested on several semi-synthetic and practical cases and compared with other solutions in this field. The mean distance between the predicted and the real sources is around 7 km for the Moscow dataset with 1096 experiments and 45 km region size and around 3 km for the Regional dataset with 803 experiments and 30 km region size. We also conduct an experiment on European Tracer Experiment-1 and get a strong performance on it: distance between the real and the predicted sources is around 6 km, which is comparable or superior to other approaches.
{"title":"Regional-scale air pollution source identification using backward particle dynamics","authors":"Mariia Filippova , Oleg Bakhteev , Fedor Meshchaninov , Evgeny Burnaev , Vladimir Vanovskiy","doi":"10.1016/j.atmosenv.2025.121044","DOIUrl":"10.1016/j.atmosenv.2025.121044","url":null,"abstract":"<div><div>Air pollution is one of the most harmful consequences of industrialization because of its strong influence on both human health quality and climate in general. Often there appears a need to identify one single strong source of air pollution appearing as a result of an accident. In this paper, we propose a new algorithm for a single pollution source localization. The proposed algorithm uses the source–receptor matrix concept and assumption about the linearity of pollution transport that allows us to use the pollution spread simulations backward in time. In particular realization, we make use of the weather regional forecast model WRF for airflow simulation and of Lagrangian particle dispersion simulation software FLEXPART-WRF for pollution advection simulation both forward and backward in time. As a result, our algorithm produces the semi-empirical heatmap of possible pollution source locations with marked point of the biggest probability and estimative emission intensity at this point as a function of time. The algorithm is tested on several semi-synthetic and practical cases and compared with other solutions in this field. The mean distance between the predicted and the real sources is around 7 km for the Moscow dataset with 1096 experiments and 45 km region size and around 3 km for the Regional dataset with 803 experiments and 30 km region size. We also conduct an experiment on European Tracer Experiment-1 and get a strong performance on it: distance between the real and the predicted sources is around 6 km, which is comparable or superior to other approaches.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"345 ","pages":"Article 121044"},"PeriodicalIF":4.2,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143277262","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-10DOI: 10.1016/j.atmosenv.2025.121049
Chunlin Li , Dongmei Cai , Michal Pardo , Hongwei Pang , Zheng Fang , Jianmin Chen , Ke Hao , Yinon Rudich
Nitrogen-containing heterocyclic aromatic compounds (NHACs) significantly contribute to urban air pollution but remain understudied. This study investigates the formation and transformation of secondary organic aerosol (SOA) from prototypical NHACs, indole, under various day- and night-time atmospheric processes. We examined the relationship between the evolving redox potential and cytotoxicity of indole-derived SOA (Indole-SOA) and its chemical alternations. Results show that Indole-SOA exhibits high oxidative potential (OPDTT of 88–268 pmol min−1 μg−1) and antioxidant capacity (AOC of 0.41–0.83 nmol trolox μg−1), exceeding most biogenic and anthropogenic organic aerosols. Indole-SOA induces significant cytotoxicity in lung epithelial cells, characterized by oxidative stress, mitochondrial dysfunction, and CYP1A1-driven detoxification pathways. The strongly correlated OPDTT and cytotoxicity of Indole-SOA are influenced by atmospheric agings and are closely related to particulate-phase products of aromatic carbonyl and reduced-nitrogen compounds. Nighttime chemistry involving O3 and NO3• produces Indole-SOA with lower yields but higher redox potential and cytotoxicity. Furthermore, Indole-SOA mixing with ambient PM2.5 shows a positive redox interaction, with the synergistic effect on OPDTT determined by Indole-SOA type and proportion. Molecular markers of Indole-SOA can be identified in Shanghai urban PM2.5, indicating potential health risks from indole and its derivatives in Chinese megacities.
{"title":"Redox potential and cytotoxicity of N-heterocyclic aromatic SOA from indole oxidation in the atmosphere","authors":"Chunlin Li , Dongmei Cai , Michal Pardo , Hongwei Pang , Zheng Fang , Jianmin Chen , Ke Hao , Yinon Rudich","doi":"10.1016/j.atmosenv.2025.121049","DOIUrl":"10.1016/j.atmosenv.2025.121049","url":null,"abstract":"<div><div>Nitrogen-containing heterocyclic aromatic compounds (NHACs) significantly contribute to urban air pollution but remain understudied. This study investigates the formation and transformation of secondary organic aerosol (SOA) from prototypical NHACs, indole, under various day- and night-time atmospheric processes. We examined the relationship between the evolving redox potential and cytotoxicity of indole-derived SOA (Indole-SOA) and its chemical alternations. Results show that Indole-SOA exhibits high oxidative potential (OP<sup>DTT</sup> of 88–268 pmol min<sup>−1</sup> μg<sup>−1</sup>) and antioxidant capacity (AOC of 0.41–0.83 nmol trolox μg<sup>−1</sup>), exceeding most biogenic and anthropogenic organic aerosols. Indole-SOA induces significant cytotoxicity in lung epithelial cells, characterized by oxidative stress, mitochondrial dysfunction, and CYP1A1-driven detoxification pathways. The strongly correlated OP<sup>DTT</sup> and cytotoxicity of Indole-SOA are influenced by atmospheric agings and are closely related to particulate-phase products of aromatic carbonyl and reduced-nitrogen compounds. Nighttime chemistry involving O<sub>3</sub> and NO<sub>3</sub>• produces Indole-SOA with lower yields but higher redox potential and cytotoxicity. Furthermore, Indole-SOA mixing with ambient PM<sub>2.5</sub> shows a positive redox interaction, with the synergistic effect on OP<sup>DTT</sup> determined by Indole-SOA type and proportion. Molecular markers of Indole-SOA can be identified in Shanghai urban PM<sub>2.5</sub>, indicating potential health risks from indole and its derivatives in Chinese megacities.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"344 ","pages":"Article 121049"},"PeriodicalIF":4.2,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143308525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-10DOI: 10.1016/j.atmosenv.2025.121035
Bingliang Zhuang , Yinan Zhou , Yaxin Hu , Shanrong Liang , Peng Gao , Yiman Gao , Huimin Chen , Shu Li , Tijian Wang , Min Xie , Mengmeng Li
Ship emissions may have significant influences on regional climates with growing trade around the world. Therefore, an updated regional climate model with comprehensive cloud microphysics schemes is employed to investigate the effects of shipping sulfate and primary carbonaceous aerosols on the East Asian summer climate. Investigations indicate that ship emissions have substantial influences on air quality, the radiative energy budget and regional climate change in East Asia in summer. They would directly result in an increment in aerosol surface concentration by at least 10% around the coasts and optical depth by 0.03 over East Asia, which considerably increases the cloud droplet numbers along ship lanes. Subsequently, a very negative instantaneous radiative forcing (>1.5 W/m2) at the surface is exerted, and then the dipoles of anti-cyclone and convergence anomalies might occur from the Bay of Bengal to northeast Asia due to shipping aerosols. These thermal-dynamic responses could further affect cloud formation, hence inducing heterogeneous and nonlocal responses of radiation, air temperature and precipitation. Both cloud optical depth and fraction are likely increased in southwestern to northern China but decreased in parts of southern China and northeastern Asia through shipping aerosols interacting with radiation and clouds. As a result, surface cooling and wetting (warming and drying) are found in the region with positive (negative) cloud change. The absorption of shipping BC to solar radiation could yield a substantial warming tendency, which might have significant contributions to the climate responses in central to northern China.
{"title":"Influence of ship emitted sulfur and carbonaceous aerosols on East Asian climate in summer","authors":"Bingliang Zhuang , Yinan Zhou , Yaxin Hu , Shanrong Liang , Peng Gao , Yiman Gao , Huimin Chen , Shu Li , Tijian Wang , Min Xie , Mengmeng Li","doi":"10.1016/j.atmosenv.2025.121035","DOIUrl":"10.1016/j.atmosenv.2025.121035","url":null,"abstract":"<div><div>Ship emissions may have significant influences on regional climates with growing trade around the world. Therefore, an updated regional climate model with comprehensive cloud microphysics schemes is employed to investigate the effects of shipping sulfate and primary carbonaceous aerosols on the East Asian summer climate. Investigations indicate that ship emissions have substantial influences on air quality, the radiative energy budget and regional climate change in East Asia in summer. They would directly result in an increment in aerosol surface concentration by at least 10% around the coasts and optical depth by 0.03 over East Asia, which considerably increases the cloud droplet numbers along ship lanes. Subsequently, a very negative instantaneous radiative forcing (>1.5 W/m<sup>2</sup>) at the surface is exerted, and then the dipoles of anti-cyclone and convergence anomalies might occur from the Bay of Bengal to northeast Asia due to shipping aerosols. These thermal-dynamic responses could further affect cloud formation, hence inducing heterogeneous and nonlocal responses of radiation, air temperature and precipitation. Both cloud optical depth and fraction are likely increased in southwestern to northern China but decreased in parts of southern China and northeastern Asia through shipping aerosols interacting with radiation and clouds. As a result, surface cooling and wetting (warming and drying) are found in the region with positive (negative) cloud change. The absorption of shipping BC to solar radiation could yield a substantial warming tendency, which might have significant contributions to the climate responses in central to northern China.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"344 ","pages":"Article 121035"},"PeriodicalIF":4.2,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143308528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-08DOI: 10.1016/j.atmosenv.2025.121031
Seoyeong Ahn , Hyewon Yun , Jieun Oh , Sooyoung Kim , Hyemin Jang , Yejin Kim , Cinoo Kang , Sojin Ahn , Ayoung Kim , Dohoon Kwon , Jinah Park , Insung Song , Jeongmin Moon , Ejin Kim , Jieun Min , Ho Kim , Whanhee Lee
A considerable number of previous studies have limitations in evaluating the population-representative relationship between ozone and cardiovascular disease (CVD) mortality risk and revealing high-risk populations due to the limited data availability that could not cover unmonitored areas. To estimate the population-representative association between warm-season (Apr–Sep) ozone and CVD mortality and examine high-risk populations, this study conducted a nationwide case-crossover study in South Korea from 2015 to 2019. Stratified analyses and meta-regression were also performed for each cause of death and demographic characteristics to find high-risk populations. As an exposure, daily modeled warm-season ozone estimated by a machine learning-based ensemble model was used (R2 > 0.92). In the total population, warm-season ozone was associated with an increased risk of total CVD death (OR: 1.010, 95% CI: 1.002–1.018), and mortality due to ischemic heart disease showed the highest OR (1.019, 1.003–1.035). The warm-season ozone-related CVD death risk was the highest in younger age groups (0–59 y) across all causes of CVD deaths, except for cerebrovascular disease death. The higher accessibility to hospital beds per 1000 was associated with a lower ozone risk of CVD mortality. The estimated excess CVD mortality fractions and years of life lost from mortality (YLL) attributable to warm-season ozone were 5.10% and 119,353.37 years. Our findings suggest that younger populations should be recognized as novel high-risk populations related to warm-season ozone and CVD mortality, and this study also provides potential benefits for constructing stricter ozone mitigation action plans.
{"title":"Short-term exposure to warm-season ozone, cardiovascular mortality, and novel high-risk populations: A nationwide time-stratified case-crossover study","authors":"Seoyeong Ahn , Hyewon Yun , Jieun Oh , Sooyoung Kim , Hyemin Jang , Yejin Kim , Cinoo Kang , Sojin Ahn , Ayoung Kim , Dohoon Kwon , Jinah Park , Insung Song , Jeongmin Moon , Ejin Kim , Jieun Min , Ho Kim , Whanhee Lee","doi":"10.1016/j.atmosenv.2025.121031","DOIUrl":"10.1016/j.atmosenv.2025.121031","url":null,"abstract":"<div><div>A considerable number of previous studies have limitations in evaluating the population-representative relationship between ozone and cardiovascular disease (CVD) mortality risk and revealing high-risk populations due to the limited data availability that could not cover unmonitored areas. To estimate the population-representative association between warm-season (Apr–Sep) ozone and CVD mortality and examine high-risk populations, this study conducted a nationwide case-crossover study in South Korea from 2015 to 2019. Stratified analyses and meta-regression were also performed for each cause of death and demographic characteristics to find high-risk populations. As an exposure, daily modeled warm-season ozone estimated by a machine learning-based ensemble model was used (R<sup>2</sup> > 0.92). In the total population, warm-season ozone was associated with an increased risk of total CVD death (OR: 1.010, 95% CI: 1.002–1.018), and mortality due to ischemic heart disease showed the highest OR (1.019, 1.003–1.035). The warm-season ozone-related CVD death risk was the highest in younger age groups (0–59 y) across all causes of CVD deaths, except for cerebrovascular disease death. The higher accessibility to hospital beds per 1000 was associated with a lower ozone risk of CVD mortality. The estimated excess CVD mortality fractions and years of life lost from mortality (YLL) attributable to warm-season ozone were 5.10% and 119,353.37 years. Our findings suggest that younger populations should be recognized as novel high-risk populations related to warm-season ozone and CVD mortality, and this study also provides potential benefits for constructing stricter ozone mitigation action plans.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"345 ","pages":"Article 121031"},"PeriodicalIF":4.2,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143277272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-07DOI: 10.1016/j.atmosenv.2025.121032
Jie Liang , Jian Hang , Shiguo Jia , Jiajia Hua , Bo Zhao , Xuelin Zhang , Hong Ling , Ziwei Mo
Solar radiation is a significant factor affecting the concentration and dispersion patterns of photochemical pollutants in urban environments. This impact is mediated through alterations in temperature and thermally-driven airflow patterns, but the full extent of these effects has not yet been quantified. To address this gap, ANSYS Fluent and APFoam were used to simulate the dispersion of photochemical pollutants in a 2D street canyon (aspect ratio = 1), incorporating the complex O3-NOx-VOCs chemical mechanism via the CS07 mechanism to accurately represent the chemical processes. The novelty lies in its comprehensive assessment of how solar radiation, emissions, and dynamic and chemical processes interact to affect photochemical pollution. It was found that under different radiation conditions, NOx and O3 concentrations exhibit distinct distribution patterns. Compared to the neutral condition, the decreased NOx concentrations (23%) and increased O3 concentrations (8.7%) are observed in the morning and at noon, whereas in the afternoon, NOx concentrations rises (111%) and O3 concentrations decreases (20%) in the canyon. At night, NOx accumulates at the bottom of the windward side. Through sensitivity tests, we found that the primary pathway through which solar radiation affects the dispersion of photochemical pollutants is dynamic process. The pedestrian health risks of photochemical pollutants were evaluated that NO2 health risks are more pronounced in the afternoon and at night, while O3 risks are more severe in the morning and at noon. Overall, this study quantitatively demonstrates the significant impact of solar radiation on the photochemical pollutants and identifies the pathways of influence.
{"title":"O3–NOx–VOCs photochemical pollutant dispersion in 2D street canyon under effects of solar radiation","authors":"Jie Liang , Jian Hang , Shiguo Jia , Jiajia Hua , Bo Zhao , Xuelin Zhang , Hong Ling , Ziwei Mo","doi":"10.1016/j.atmosenv.2025.121032","DOIUrl":"10.1016/j.atmosenv.2025.121032","url":null,"abstract":"<div><div>Solar radiation is a significant factor affecting the concentration and dispersion patterns of photochemical pollutants in urban environments. This impact is mediated through alterations in temperature and thermally-driven airflow patterns, but the full extent of these effects has not yet been quantified. To address this gap, ANSYS Fluent and APFoam were used to simulate the dispersion of photochemical pollutants in a 2D street canyon (aspect ratio = 1), incorporating the complex O<sub>3</sub>-NO<sub>x</sub>-VOCs chemical mechanism via the CS07 mechanism to accurately represent the chemical processes. The novelty lies in its comprehensive assessment of how solar radiation, emissions, and dynamic and chemical processes interact to affect photochemical pollution. It was found that under different radiation conditions, NO<sub>x</sub> and O<sub>3</sub> concentrations exhibit distinct distribution patterns. Compared to the neutral condition, the decreased NO<sub>x</sub> concentrations (23%) and increased O<sub>3</sub> concentrations (8.7%) are observed in the morning and at noon, whereas in the afternoon, NO<sub>x</sub> concentrations rises (111%) and O<sub>3</sub> concentrations decreases (20%) in the canyon. At night, NO<sub>x</sub> accumulates at the bottom of the windward side. Through sensitivity tests, we found that the primary pathway through which solar radiation affects the dispersion of photochemical pollutants is dynamic process. The pedestrian health risks of photochemical pollutants were evaluated that NO<sub>2</sub> health risks are more pronounced in the afternoon and at night, while O<sub>3</sub> risks are more severe in the morning and at noon. Overall, this study quantitatively demonstrates the significant impact of solar radiation on the photochemical pollutants and identifies the pathways of influence.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"344 ","pages":"Article 121032"},"PeriodicalIF":4.2,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143308527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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