Dihui Chen, Ansheng Zhu, Ling Huang, Elly Yaluk, Yangjun Wang, Maggie Chel Gee Ooi, Ying Gu, Andy Chan and Li Li
The planetary boundary layer (PBL) plays a crucial role in determining meteorological fields and the diffusion of atmospheric pollutants. Therefore, accurate PBL simulation is necessary for precise meteorological and air quality simulations, and the choice of PBL scheme significantly influences the accuracy of simulation results. In this study, we investigate the seasonal and diurnal variations of typical meteorological variables over the Yangtze River Delta (YRD) region by using the Weather Research and Forecasting (WRF) model using four different closure schemes. These closure schemes include two non-local closure schemes, i.e., Yonsei University (YSU) and Asymmetric Convective Model version 2 (ACM2), as well as two local closure schemes named Mellor–Yamada–Janjic (MYJ) and Mellor–Yamada Nakanishi and Niino (MYNN). By comparing observations and model inter-comparisons, we discuss the similarities and differences in simulated results among different PBL schemes. The results indicate that local closure schemes, i.e., MYJ and MYNN, generally produce more realistic simulations of meteorological parameters. MYNN performs best in summer with a mean bias (MB) of 0.41 °C for temperature and 0.44 m s−1 for wind speed, while MYJ shows better results under stable conditions during winter with a MB of 0.64 °C for temperature and −5.76% for relative humidity. YSU is found to have less bias in PBL height during summer with the highest R up to 0.81, while MYJ outperforms the three other schemes with the least MB of 38 m (R = 0.65) in winter. Each PBL closure scheme, i.e., the MYJ and MYNN local closure schemes, may not accurately capture all physical processes, leading to performance variations, especially during transitional seasons and under specific diurnal conditions. Thus, it is important to note that each scheme has its strengths and weaknesses, and the selection of the most appropriate scheme should depend on the specific variables and scenarios under consideration.
{"title":"Sensitivity analysis of planetary boundary layer parameterization on meteorological simulations in the Yangtze river delta region, China†","authors":"Dihui Chen, Ansheng Zhu, Ling Huang, Elly Yaluk, Yangjun Wang, Maggie Chel Gee Ooi, Ying Gu, Andy Chan and Li Li","doi":"10.1039/D4EA00038B","DOIUrl":"https://doi.org/10.1039/D4EA00038B","url":null,"abstract":"<p >The planetary boundary layer (PBL) plays a crucial role in determining meteorological fields and the diffusion of atmospheric pollutants. Therefore, accurate PBL simulation is necessary for precise meteorological and air quality simulations, and the choice of PBL scheme significantly influences the accuracy of simulation results. In this study, we investigate the seasonal and diurnal variations of typical meteorological variables over the Yangtze River Delta (YRD) region by using the Weather Research and Forecasting (WRF) model using four different closure schemes. These closure schemes include two non-local closure schemes, <em>i.e.</em>, Yonsei University (YSU) and Asymmetric Convective Model version 2 (ACM2), as well as two local closure schemes named Mellor–Yamada–Janjic (MYJ) and Mellor–Yamada Nakanishi and Niino (MYNN). By comparing observations and model inter-comparisons, we discuss the similarities and differences in simulated results among different PBL schemes. The results indicate that local closure schemes, <em>i.e.</em>, MYJ and MYNN, generally produce more realistic simulations of meteorological parameters. MYNN performs best in summer with a mean bias (MB) of 0.41 °C for temperature and 0.44 m s<small><sup>−1</sup></small> for wind speed, while MYJ shows better results under stable conditions during winter with a MB of 0.64 °C for temperature and −5.76% for relative humidity. YSU is found to have less bias in PBL height during summer with the highest <em>R</em> up to 0.81, while MYJ outperforms the three other schemes with the least MB of 38 m (<em>R</em> = 0.65) in winter. Each PBL closure scheme, <em>i.e.</em>, the MYJ and MYNN local closure schemes, may not accurately capture all physical processes, leading to performance variations, especially during transitional seasons and under specific diurnal conditions. Thus, it is important to note that each scheme has its strengths and weaknesses, and the selection of the most appropriate scheme should depend on the specific variables and scenarios under consideration.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 10","pages":" 1129-1144"},"PeriodicalIF":2.8,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00038b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142397568","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}
Bruno Vitali, Manuel Bettineschi, Arineh Cholakian, Dino Zardi, Federico Bianchi, Victoria A. Sinclair, Johannes Mikkola, Paolo Cristofanelli, Angela Marinoni, Martina Mazzini, Liine Heikkinen, Minna Aurela, Marco Paglione, Bertrand Bessagnet, Paolo Tuccella and Giancarlo Ciarelli
<p >Sources and transport processes of aerosols over the Italian northern Apennines are investigated with a focus on the area of the WMO/GAW global station of Mt. Cimone (CMN, 2165 m a.s.l.). The site is characterized by complex orography, representing a challenge for chemical transport model (CTM) applications when simulating processes controlling advection and diffusion of air pollutants within and above the planetary boundary layer (PBL). First, we extensively evaluated the skills of the WRF-CHIMERE (v2020r3) coupled CTM in reproducing both the meteorological conditions observed at the surface level of multiple weather stations and the sub-micrometre aerosol mass concentrations from intensive <em>in situ</em> measurements performed at CMN during July 2017. The analysis of the meteorological fields revealed that the local thermally-driven flows occurring over the adjacent coastal and mountainous regions are very well reproduced by the model. The accuracy is less at higher altitudes in proximity of CMN and on the slopes facing the Po valley, where also fewer observational meteorological data were available. The discrepancies between the model output and observations, especially in the near-surface wind dynamics, are mainly associated with the smoothed topography of the terrain as represented in the model: at the resolution of 1 km small-scale orographic features and related meteorological phenomena cannot be adequately reproduced. Our results indicate that the modeled particle mass concentrations and its chemical composition are in good agreement with observational data, with organic aerosol contributing to about 60% of the total sub-micrometer aerosol load during the investigated time period and sulphate being the most important inorganic component. Additionally, a model-based source apportionment analysis revealed that organic aerosol, and specifically secondary organic aerosol (SOA), were mostly of biogenic origin (contributing up to 66% of the secondary organic aerosol fraction). We further analyze the transport of organic aerosol particles associated with the typical wind pattern developing at the interface between plains, valleys and ridges of the northern Apennines mountains. Despite uncertainties in source areas and formation mechanisms, the model results indicated that the upslope valley winds might sustain the funneling of biogenic aerosol particles to higher elevations up to the Apennines ridge, eventually to above the diagnosed PBL height. For biogenic organic aerosol this process is more effective on the south-western slope of the Apennines range. This may result from either more favourable meteorological conditions or larger availability of aerosol particles over the lowlands. This work represents the first high-resolution (1 km) CTM study investigating the region of Mt. Cimone and is intended to provide original insights on the vertical transport of aerosols particles into the free troposphere in regions characterized by a complex
{"title":"Analysis of chemical and transport processes of biogenic aerosols over the northern Apennines: insights from the WRF-CHIMERE model†","authors":"Bruno Vitali, Manuel Bettineschi, Arineh Cholakian, Dino Zardi, Federico Bianchi, Victoria A. Sinclair, Johannes Mikkola, Paolo Cristofanelli, Angela Marinoni, Martina Mazzini, Liine Heikkinen, Minna Aurela, Marco Paglione, Bertrand Bessagnet, Paolo Tuccella and Giancarlo Ciarelli","doi":"10.1039/D4EA00040D","DOIUrl":"https://doi.org/10.1039/D4EA00040D","url":null,"abstract":"<p >Sources and transport processes of aerosols over the Italian northern Apennines are investigated with a focus on the area of the WMO/GAW global station of Mt. Cimone (CMN, 2165 m a.s.l.). The site is characterized by complex orography, representing a challenge for chemical transport model (CTM) applications when simulating processes controlling advection and diffusion of air pollutants within and above the planetary boundary layer (PBL). First, we extensively evaluated the skills of the WRF-CHIMERE (v2020r3) coupled CTM in reproducing both the meteorological conditions observed at the surface level of multiple weather stations and the sub-micrometre aerosol mass concentrations from intensive <em>in situ</em> measurements performed at CMN during July 2017. The analysis of the meteorological fields revealed that the local thermally-driven flows occurring over the adjacent coastal and mountainous regions are very well reproduced by the model. The accuracy is less at higher altitudes in proximity of CMN and on the slopes facing the Po valley, where also fewer observational meteorological data were available. The discrepancies between the model output and observations, especially in the near-surface wind dynamics, are mainly associated with the smoothed topography of the terrain as represented in the model: at the resolution of 1 km small-scale orographic features and related meteorological phenomena cannot be adequately reproduced. Our results indicate that the modeled particle mass concentrations and its chemical composition are in good agreement with observational data, with organic aerosol contributing to about 60% of the total sub-micrometer aerosol load during the investigated time period and sulphate being the most important inorganic component. Additionally, a model-based source apportionment analysis revealed that organic aerosol, and specifically secondary organic aerosol (SOA), were mostly of biogenic origin (contributing up to 66% of the secondary organic aerosol fraction). We further analyze the transport of organic aerosol particles associated with the typical wind pattern developing at the interface between plains, valleys and ridges of the northern Apennines mountains. Despite uncertainties in source areas and formation mechanisms, the model results indicated that the upslope valley winds might sustain the funneling of biogenic aerosol particles to higher elevations up to the Apennines ridge, eventually to above the diagnosed PBL height. For biogenic organic aerosol this process is more effective on the south-western slope of the Apennines range. This may result from either more favourable meteorological conditions or larger availability of aerosol particles over the lowlands. This work represents the first high-resolution (1 km) CTM study investigating the region of Mt. Cimone and is intended to provide original insights on the vertical transport of aerosols particles into the free troposphere in regions characterized by a complex","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 9","pages":" 967-987"},"PeriodicalIF":2.8,"publicationDate":"2024-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00040d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142169788","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}
Joe Adabouk Amooli, Kwame Oppong Hackman, Bernard Nana and Daniel M. Westervelt
This study estimates PM2.5 concentrations in Ouagadougou using satellite-based aerosol optical depth (AOD) and meteorological parameters such as temperature, precipitation, relative humidity, wind speed, and wind direction. First, Simple Linear Regression (SLR), Multiple Linear Regression (MLR), Decision Tree (DT), Random Forest (RF), and eXtreme Gradient Boosting (XGBoost) models were developed using the available labeled data (AOD and meteorological parameters with corresponding PM2.5 values) in the city. The XGBoost model outperformed all other models that were used, with a coefficient of determination (R2) of 0.87 and a root-mean-square error (RMSE) of 15.8 μg m−3 after a five-fold cross-validation. The performance of the supervised XGBoost model was upgraded by incorporating a semi-supervised algorithm to use large amounts of unlabeled data in the city and allow for a more accurate and extensive estimation of PM2.5 for the period 2000–2022. This semi-supervised XGBoost model had an R2 of 0.97 and an RMSE of 8.3 μg m−3 after a five-fold cross-validation. The results indicate that the estimated 24 hour mean PM2.5 concentrations in the city are 2 to 4 times higher than the World Health Organization (WHO) 24 hour guidelines of 15 μg m−3 in the rainy season and 2 to 22 times higher than the WHO 24 hour guideline in the dry season. The results also reveal that the average annual estimated PM2.5 concentrations are 11 to 14 times higher than the WHO average annual guideline of 5 μg m−3. Finally, we find higher PM2.5 concentrations in the city's center and industrial areas than in the other areas. The results indicate a need for future air pollution policy and mitigation in Burkina Faso to achieve desired health benefits such as reduced respiratory and cardiovascular problems, which will, in turn, lead to decreased PM2.5 mortality rates.
{"title":"Fine particulate air pollution estimation in Ouagadougou using satellite aerosol optical depth and meteorological parameters†","authors":"Joe Adabouk Amooli, Kwame Oppong Hackman, Bernard Nana and Daniel M. Westervelt","doi":"10.1039/D4EA00057A","DOIUrl":"https://doi.org/10.1039/D4EA00057A","url":null,"abstract":"<p >This study estimates PM<small><sub>2.5</sub></small> concentrations in Ouagadougou using satellite-based aerosol optical depth (AOD) and meteorological parameters such as temperature, precipitation, relative humidity, wind speed, and wind direction. First, Simple Linear Regression (SLR), Multiple Linear Regression (MLR), Decision Tree (DT), Random Forest (RF), and eXtreme Gradient Boosting (XGBoost) models were developed using the available labeled data (AOD and meteorological parameters with corresponding PM<small><sub>2.5</sub></small> values) in the city. The XGBoost model outperformed all other models that were used, with a coefficient of determination (<em>R</em><small><sup>2</sup></small>) of 0.87 and a root-mean-square error (RMSE) of 15.8 μg m<small><sup>−3</sup></small> after a five-fold cross-validation. The performance of the supervised XGBoost model was upgraded by incorporating a semi-supervised algorithm to use large amounts of unlabeled data in the city and allow for a more accurate and extensive estimation of PM<small><sub>2.5</sub></small> for the period 2000–2022. This semi-supervised XGBoost model had an <em>R</em><small><sup>2</sup></small> of 0.97 and an RMSE of 8.3 μg m<small><sup>−3</sup></small> after a five-fold cross-validation. The results indicate that the estimated 24 hour mean PM<small><sub>2.5</sub></small> concentrations in the city are 2 to 4 times higher than the World Health Organization (WHO) 24 hour guidelines of 15 μg m<small><sup>−3</sup></small> in the rainy season and 2 to 22 times higher than the WHO 24 hour guideline in the dry season. The results also reveal that the average annual estimated PM<small><sub>2.5</sub></small> concentrations are 11 to 14 times higher than the WHO average annual guideline of 5 μg m<small><sup>−3</sup></small>. Finally, we find higher PM<small><sub>2.5</sub></small> concentrations in the city's center and industrial areas than in the other areas. The results indicate a need for future air pollution policy and mitigation in Burkina Faso to achieve desired health benefits such as reduced respiratory and cardiovascular problems, which will, in turn, lead to decreased PM<small><sub>2.5</sub></small> mortality rates.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 9","pages":" 1012-1025"},"PeriodicalIF":2.8,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00057a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142169804","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}
The present long-term study has been conducted with dual objectives: firstly, to monitor the spatio-temporal variation of ambient air quality parameters and secondly, to evaluate the impact of air pollutants on the Delhi population. Five years (January 2019 to December 2023) of data of six key pollutants (PM10, PM2.5, NO2, O3, Benzene, and Toluene) were collected by continuous ambient air quality monitoring stations, obtained from the Central Pollution Control Board portal. The impact of air pollutants on human health was assessed using different indices and the AirQ+ model developed by the World Health Organization (WHO). Additionally, the ozone formation potential (OFP) of benzene and toluene was evaluated. The findings of the study revealed that the concentrations of PM10 and PM2.5 exceeded both national and global guidelines across all the sites throughout the study period. Notably, industrial sites were classified as the severe category according to the National Air Quality Index. At industrial sites, the OFP of volatile organic compounds (VOCs) was observed to be higher in comparison to commercial sites. The AirQ+ model analysis in the health risk assessment indicated a strong association between PM10 exposure and mortality from respiratory (91.36%) and chronic bronchitis (90.85%) diseases. Additionally, long-term PM2.5 exposure was linked to an increased risk of stroke (65%) and circulatory (63.83%) mortality.
{"title":"Variability in air quality, ozone formation potential by VOCs, and associated air pollution attributable health risks for Delhi's inhabitants†","authors":"Saurabh Sharma, Anjum Singhal, Veluswamy Venkatramanan, Pawan Verma and Mayank Pandey","doi":"10.1039/D4EA00064A","DOIUrl":"https://doi.org/10.1039/D4EA00064A","url":null,"abstract":"<p >The present long-term study has been conducted with dual objectives: firstly, to monitor the spatio-temporal variation of ambient air quality parameters and secondly, to evaluate the impact of air pollutants on the Delhi population. Five years (January 2019 to December 2023) of data of six key pollutants (PM<small><sub>10</sub></small>, PM<small><sub>2.5</sub></small>, NO<small><sub>2</sub></small>, O<small><sub>3</sub></small>, Benzene, and Toluene) were collected by continuous ambient air quality monitoring stations, obtained from the Central Pollution Control Board portal. The impact of air pollutants on human health was assessed using different indices and the AirQ+ model developed by the World Health Organization (WHO). Additionally, the ozone formation potential (OFP) of benzene and toluene was evaluated. The findings of the study revealed that the concentrations of PM<small><sub>10</sub></small> and PM<small><sub>2.5</sub></small> exceeded both national and global guidelines across all the sites throughout the study period. Notably, industrial sites were classified as the severe category according to the National Air Quality Index. At industrial sites, the OFP of volatile organic compounds (VOCs) was observed to be higher in comparison to commercial sites. The AirQ+ model analysis in the health risk assessment indicated a strong association between PM<small><sub>10</sub></small> exposure and mortality from respiratory (91.36%) and chronic bronchitis (90.85%) diseases. Additionally, long-term PM<small><sub>2.5</sub></small> exposure was linked to an increased risk of stroke (65%) and circulatory (63.83%) mortality.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 8","pages":" 897-910"},"PeriodicalIF":2.8,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00064a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141966431","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}
Flobert A. Ndah, Marja Maljanen, Riikka Rinnan, Hem Raj Bhattarai, Cleo L. Davie-Martin, Santtu Mikkonen, Anders Michelsen and Minna Kivimäenpää
Climate warming is projected to be particularly pronounced in the northern high latitudes coupled with reduced light availability due to increased cloudiness. The changing climate may alter the fluxes of greenhouse gases (GHGs) and atmospherically reactive trace gases, which can drive important climate feedbacks. We investigated the individual and combined effects of warming and increased cloudiness on methane (CH4), carbon dioxide (CO2), nitrous oxide (N2O), nitric oxide (NO), nitrous acid (HONO) and biogenic volatile organic compound (BVOC) fluxes in mesocosms from two tundra and one palsa mire ecosystems kept under strict environmental control in climate chambers. We also examined whether and how prevailing soil physiochemical properties and plant species composition affected the fluxes. In control conditions, all sites were net sinks of CH4 and CO2 during both growing seasons except for the palsa site which was a net source of CO2 in the second growing season. Warming enhanced CH4 uptake, mostly observed in the palsa site, and turned the palsa site from a sink to a source of CO2 in the first growing season and increased the CO2 source strength in the second growing season. Warming increased BVOC emissions while increased cloudiness mostly decreased the emissions. The combined treatment of warming and increased cloudiness decreased CH4 uptake, mostly observed in the palsa site, and BVOC emissions. Fluxes of CO2 were linked to availability of soil carbon and organic matter, litter input, soil pH and bulk density, and cover of mosses. Low emissions of N2O, NO, and HONO could mainly be explained by limited availability of mineral nitrogen. Warming-enhanced CH4 uptake and BVOC emissions will provide a negative feedback to climate while enhanced CO2 release from palsa mires will exacerbate global warming. Under combined warming and increased cloudiness, subarctic ecosystems may shift from sinks to sources of CH4, providing a positive feedback to climate. Prevailing soil physiochemical properties and vegetation composition will play a significant role in controlling the fluxes, hence contributing to the overall climate change effects and feedback.
据预测,气候变暖在北部高纬度地区尤为明显,同时由于云量增加,光照也会减少。气候的变化可能会改变温室气体(GHGs)和大气中活性痕量气体的通量,从而产生重要的气候反馈作用。我们研究了气候变暖和云量增加对甲烷(CH4)、二氧化碳(CO2)、一氧化二氮(N2O)、一氧化氮(NO)、亚硝酸(HONO)和生物挥发性有机化合物(BVOC)通量的单独和综合影响,这些通量来自气候室中严格环境控制下的两个苔原和一个沼泽生态系统。我们还研究了当时的土壤理化性质和植物物种组成是否以及如何影响通量。在对照条件下,除了沼泽地在第二个生长季是二氧化碳的净来源地之外,所有地点在两个生长季都是甲烷和二氧化碳的净吸收汇。在第一个生长季,气候变暖增强了对 CH4 的吸收(主要是在 palsa 地点观察到),并使 palsa 地点从 CO2 的吸收汇变为 CO2 的来源地,同时增加了第二个生长季的 CO2 来源强度。气候变暖增加了 BVOC 排放量,而云量增加则主要减少了排放量。升温和云量增加的综合处理降低了 CH4 吸收量(主要在 palsa 地点观察到)和 BVOC 排放量。二氧化碳的通量与土壤碳和有机物的可用性、垃圾投入量、土壤 pH 值和容重以及苔藓覆盖率有关。N2O、NO和HONO排放量低的主要原因是矿物氮的供应有限。气候变暖会增加 CH4 吸收和 BVOC 排放,从而对气候产生负反馈,而浅海苔藓增加 CO2 释放则会加剧全球变暖。在气候变暖和云量增加的共同作用下,亚北极生态系统可能会从甲烷的吸收汇转变为甲烷的来源,从而对气候产生正反馈。现有的土壤理化特性和植被组成将在控制通量方面发挥重要作用,从而促进整体气候变化效应和反馈。
{"title":"Carbon and nitrogen-based gas fluxes in subarctic ecosystems under climate warming and increased cloudiness†","authors":"Flobert A. Ndah, Marja Maljanen, Riikka Rinnan, Hem Raj Bhattarai, Cleo L. Davie-Martin, Santtu Mikkonen, Anders Michelsen and Minna Kivimäenpää","doi":"10.1039/D4EA00017J","DOIUrl":"https://doi.org/10.1039/D4EA00017J","url":null,"abstract":"<p >Climate warming is projected to be particularly pronounced in the northern high latitudes coupled with reduced light availability due to increased cloudiness. The changing climate may alter the fluxes of greenhouse gases (GHGs) and atmospherically reactive trace gases, which can drive important climate feedbacks. We investigated the individual and combined effects of warming and increased cloudiness on methane (CH<small><sub>4</sub></small>), carbon dioxide (CO<small><sub>2</sub></small>), nitrous oxide (N<small><sub>2</sub></small>O), nitric oxide (NO), nitrous acid (HONO) and biogenic volatile organic compound (BVOC) fluxes in mesocosms from two tundra and one palsa mire ecosystems kept under strict environmental control in climate chambers. We also examined whether and how prevailing soil physiochemical properties and plant species composition affected the fluxes. In control conditions, all sites were net sinks of CH<small><sub>4</sub></small> and CO<small><sub>2</sub></small> during both growing seasons except for the palsa site which was a net source of CO<small><sub>2</sub></small> in the second growing season. Warming enhanced CH<small><sub>4</sub></small> uptake, mostly observed in the palsa site, and turned the palsa site from a sink to a source of CO<small><sub>2</sub></small> in the first growing season and increased the CO<small><sub>2</sub></small> source strength in the second growing season. Warming increased BVOC emissions while increased cloudiness mostly decreased the emissions. The combined treatment of warming and increased cloudiness decreased CH<small><sub>4</sub></small> uptake, mostly observed in the palsa site, and BVOC emissions. Fluxes of CO<small><sub>2</sub></small> were linked to availability of soil carbon and organic matter, litter input, soil pH and bulk density, and cover of mosses. Low emissions of N<small><sub>2</sub></small>O, NO, and HONO could mainly be explained by limited availability of mineral nitrogen. Warming-enhanced CH<small><sub>4</sub></small> uptake and BVOC emissions will provide a negative feedback to climate while enhanced CO<small><sub>2</sub></small> release from palsa mires will exacerbate global warming. Under combined warming and increased cloudiness, subarctic ecosystems may shift from sinks to sources of CH<small><sub>4</sub></small>, providing a positive feedback to climate. Prevailing soil physiochemical properties and vegetation composition will play a significant role in controlling the fluxes, hence contributing to the overall climate change effects and feedback.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 8","pages":" 942-957"},"PeriodicalIF":2.8,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00017j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141966310","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}
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten and Michael Boy
In the last few decades, atmospheric formation of secondary organic aerosols (SOA) has gained increasing attention due to their impact on air quality and climate. However, methods to predict their abundance are mainly empirical and may fail under real atmospheric conditions. In this work, a close-to-mechanistic approach allowing SOA quantification is presented, with a focus on a chain-like chemical reaction called “autoxidation”. A novel framework is employed to (a) describe the gas-phase chemistry, (b) predict the products' molecular structures and (c) explore the contribution of autoxidation chemistry on SOA formation under various conditions. As a proof of concept, the method is applied to benzene, an important anthropogenic SOA precursor. Our results suggest autoxidation to explain up to 100% of the benzene-SOA formed under low-NOx laboratory conditions. Under atmospheric-like day-time conditions, the calculated benzene-aerosol mass continuously forms, as expected based on prior work. Additionally, a prompt increase, driven by the NO3 radical, is predicted by the model at dawn. This increase has not yet been explored experimentally and stresses the potential for atmospheric SOA formation via secondary oxidation of benzene by O3 and NO3.
在过去几十年中,大气中形成的二次有机气溶胶(SOA)因其对空气质量和气候的影响而日益受到关注。然而,预测其丰度的方法主要是经验性的,在实际大气条件下可能会失效。在这项工作中,提出了一种接近于机理的方法来量化 SOA,重点是一种称为 "自氧化 "的链式化学反应。该方法采用了一个新颖的框架:(a)描述气相化学反应;(b)预测产物的分子结构;(c)探索自氧化化学反应在各种条件下对 SOA 形成的影响。作为概念验证,该方法被应用于苯--一种重要的人为 SOA 前体。我们的研究结果表明,在低氮实验室条件下,自氧化作用可解释高达 100% 的苯 SOA 形成。在类似大气的日间条件下,计算出的苯-气溶胶质量会持续形成,这也是之前研究的预期结果。此外,根据模型预测,在黎明时分,由 NO3 自由基驱动的苯气溶胶会迅速增加。这种增加尚未经过实验探索,它强调了大气 SOA 通过 O3 和 NO3 对苯的二次氧化形成的可能性。
{"title":"Towards automated inclusion of autoxidation chemistry in models: from precursors to atmospheric implications†","authors":"Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten and Michael Boy","doi":"10.1039/D4EA00054D","DOIUrl":"10.1039/D4EA00054D","url":null,"abstract":"<p >In the last few decades, atmospheric formation of secondary organic aerosols (SOA) has gained increasing attention due to their impact on air quality and climate. However, methods to predict their abundance are mainly empirical and may fail under real atmospheric conditions. In this work, a close-to-mechanistic approach allowing SOA quantification is presented, with a focus on a chain-like chemical reaction called “autoxidation”. A novel framework is employed to (a) describe the gas-phase chemistry, (b) predict the products' molecular structures and (c) explore the contribution of autoxidation chemistry on SOA formation under various conditions. As a proof of concept, the method is applied to benzene, an important anthropogenic SOA precursor. Our results suggest autoxidation to explain up to 100% of the benzene-SOA formed under low-NO<small><sub><em>x</em></sub></small> laboratory conditions. Under atmospheric-like day-time conditions, the calculated benzene-aerosol mass continuously forms, as expected based on prior work. Additionally, a prompt increase, driven by the NO<small><sub>3</sub></small> radical, is predicted by the model at dawn. This increase has not yet been explored experimentally and stresses the potential for atmospheric SOA formation <em>via</em> secondary oxidation of benzene by O<small><sub>3</sub></small> and NO<small><sub>3</sub></small>.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 8","pages":" 879-896"},"PeriodicalIF":2.8,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11307592/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141918234","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}
Mohanraj Gopikrishnan, Kanimozhi Subramanian, Ashwin Krn, George Priya Doss C., B. Srimuruganandam and Natarajan Chandrasekaran
Global air pollution presents substantial risks to both human health and the environment. Particulate Matter (PM) adversely affects ecosystems through pollution, bioaccumulation, and endangerment of aquatic organisms. These contaminants enter water systems via precipitation and industrial runoff, damaging aquatic invertebrates through physical, physiological, and molecular mechanisms, leading to developmental issues and organ toxicity. This study investigates the combined toxicological effect of environmental exposure to polystyrene (PS) nanoparticles and varying PM concentrations from indoor and outdoor dust particles on Artemia salina. Our findings reveal noteworthy elevations in reactive oxygen species (ROS) and malondialdehyde (MDA) levels in air conditioner (AC) dust and PM2.5 exposures, highlighting potential health risks associated with high particulate contamination. Conversely, superoxide dismutase (SOD) activity decreased, indicating harm to enzyme systems. In contrast, catalase activity (CAT) increased, suggesting a compensatory response to oxidative stress induced by Polystyrene (PS) and suspended particulate pollutants. These results underscore the severe oxidative stress experienced by marine zooplankton when exposed to PM2.5 combined with NPs, potentially impairing growth. Further research should explore the combined toxicological effects of PM2.5 and NPs on other marine species and investigate long-term exposure effects and bioaccumulation pathways. Understanding these dynamics is crucial for developing effective strategies to mitigate NP pollution and protect human health and aquatic ecosystems.
{"title":"Particulate matter and nanoplastics: synergistic impact on Artemia salina","authors":"Mohanraj Gopikrishnan, Kanimozhi Subramanian, Ashwin Krn, George Priya Doss C., B. Srimuruganandam and Natarajan Chandrasekaran","doi":"10.1039/D4EA00065J","DOIUrl":"https://doi.org/10.1039/D4EA00065J","url":null,"abstract":"<p >Global air pollution presents substantial risks to both human health and the environment. Particulate Matter (PM) adversely affects ecosystems through pollution, bioaccumulation, and endangerment of aquatic organisms. These contaminants enter water systems <em>via</em> precipitation and industrial runoff, damaging aquatic invertebrates through physical, physiological, and molecular mechanisms, leading to developmental issues and organ toxicity. This study investigates the combined toxicological effect of environmental exposure to polystyrene (PS) nanoparticles and varying PM concentrations from indoor and outdoor dust particles on <em>Artemia salina</em>. Our findings reveal noteworthy elevations in reactive oxygen species (ROS) and malondialdehyde (MDA) levels in air conditioner (AC) dust and PM<small><sub>2.5</sub></small> exposures, highlighting potential health risks associated with high particulate contamination. Conversely, superoxide dismutase (SOD) activity decreased, indicating harm to enzyme systems. In contrast, catalase activity (CAT) increased, suggesting a compensatory response to oxidative stress induced by Polystyrene (PS) and suspended particulate pollutants. These results underscore the severe oxidative stress experienced by marine zooplankton when exposed to PM<small><sub>2.5</sub></small> combined with NPs, potentially impairing growth. Further research should explore the combined toxicological effects of PM<small><sub>2.5</sub></small> and NPs on other marine species and investigate long-term exposure effects and bioaccumulation pathways. Understanding these dynamics is crucial for developing effective strategies to mitigate NP pollution and protect human health and aquatic ecosystems.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 9","pages":" 988-999"},"PeriodicalIF":2.8,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00065j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142169809","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}
We would like to take this opportunity to thank all of Environmental Science: Atmospheres’s reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for Environmental Science: Atmospheres in 2023.
{"title":"Outstanding Reviewers for Environmental Science: Atmospheres in 2023","authors":"","doi":"10.1039/D4EA90025A","DOIUrl":"https://doi.org/10.1039/D4EA90025A","url":null,"abstract":"<p >We would like to take this opportunity to thank all of <em>Environmental Science: Atmospheres</em>’s reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for <em>Environmental Science: Atmospheres</em> in 2023.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 7","pages":" 707-707"},"PeriodicalIF":2.8,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea90025a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141583658","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}
Stefan Osterwalder, Ron Schibler, Christoph Hüglin, Beat Schwarzenbach, Geoff Stupple, Katrina MacSween, Kevin Bishop, Christine Alewell and Nina Buchmann
Mercury (Hg) is a threat to the environment and human health. As a consequence, the Minamata Convention on Mercury was adopted in 2013 to reduce Hg pollution by curbing anthropogenic emissions. Analysis of gaseous elemental Hg (Hg0) concentration trends in the atmosphere has been identified as a cost-effective means to evaluate progress on reducing Hg pollution. Therefore, spatial coverage of atmospheric Hg0 concentration measurements should be expanded. We established an atmospheric Hg0 concentration monitoring network with 22 sites across Switzerland, using the Mercury Passive Air Sampler (MerPAS®). The mean annual atmospheric Hg0 concentration in Switzerland was 1.34 ± 0.20 ng m−3 (August 22, 2022 – September 21, 2023), similar to current observations at European air monitoring stations. Mean atmospheric Hg0 concentrations were significantly lower at rural stations (1.25 ± 0.11 ng m−3) than at urban (1.37 ± 0.14 ng m−3) stations (Mann-Whitney U-test, p < 0.01). This concentration difference can be explained by more local Hg emissions at urban sites (e.g., by fuel combustion) throughout the year as well as by more pronounced stomatal Hg0 uptake at rural sites during spring and summer. We recommend continuing the Swiss Atmospheric Mercury Network to support the call from the Minamata Convention to monitor atmospheric Hg0 as a control on whether international efforts are successful in reducing Hg in the environment. Longer term records from such monitoring networks will also help improve the understanding of both regional and global Hg cycles.
{"title":"Spatial and seasonal dynamics of gaseous elemental mercury concentrations over Switzerland observed by a passive air sampler network†","authors":"Stefan Osterwalder, Ron Schibler, Christoph Hüglin, Beat Schwarzenbach, Geoff Stupple, Katrina MacSween, Kevin Bishop, Christine Alewell and Nina Buchmann","doi":"10.1039/D4EA00052H","DOIUrl":"https://doi.org/10.1039/D4EA00052H","url":null,"abstract":"<p >Mercury (Hg) is a threat to the environment and human health. As a consequence, the Minamata Convention on Mercury was adopted in 2013 to reduce Hg pollution by curbing anthropogenic emissions. Analysis of gaseous elemental Hg (Hg<small><sup>0</sup></small>) concentration trends in the atmosphere has been identified as a cost-effective means to evaluate progress on reducing Hg pollution. Therefore, spatial coverage of atmospheric Hg<small><sup>0</sup></small> concentration measurements should be expanded. We established an atmospheric Hg<small><sup>0</sup></small> concentration monitoring network with 22 sites across Switzerland, using the Mercury Passive Air Sampler (MerPAS®). The mean annual atmospheric Hg<small><sup>0</sup></small> concentration in Switzerland was 1.34 ± 0.20 ng m<small><sup>−3</sup></small> (August 22, 2022 – September 21, 2023), similar to current observations at European air monitoring stations. Mean atmospheric Hg<small><sup>0</sup></small> concentrations were significantly lower at rural stations (1.25 ± 0.11 ng m<small><sup>−3</sup></small>) than at urban (1.37 ± 0.14 ng m<small><sup>−3</sup></small>) stations (Mann-Whitney <em>U</em>-test, <em>p</em> < 0.01). This concentration difference can be explained by more local Hg emissions at urban sites (<em>e.g.</em>, by fuel combustion) throughout the year as well as by more pronounced stomatal Hg<small><sup>0</sup></small> uptake at rural sites during spring and summer. We recommend continuing the Swiss Atmospheric Mercury Network to support the call from the Minamata Convention to monitor atmospheric Hg<small><sup>0</sup></small> as a control on whether international efforts are successful in reducing Hg in the environment. Longer term records from such monitoring networks will also help improve the understanding of both regional and global Hg cycles.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 8","pages":" 848-860"},"PeriodicalIF":2.8,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00052h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141966428","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}
Diana C. Hernandez-Jaramillo, Chris Medcraft, Ramon Campos Braga, Peter Butcherine, Adrian Doss, Brendan Kelaher, Daniel Rosenfeld and Daniel P. Harrison
Our work on aerosol–cloud–radiation interactions became hamstrung by the lack of a suitable aerosol and cloud microphysics equipped aircraft in Australia. To address this infrastructure gap, we have established a new airborne research platform, designed primarily for Marine Cloud Brightening (MCB) field studies but with broader applicability across diverse airborne research domains. This platform, comprising a Cessna 337 aircraft was outfitted with a comprehensive suite of meteorological, aerosol, and cloud microphysical instrumentation normally only found on much larger aircrafts. The aircraft has completed its first field deployment over the Great Barrier Reef (GBR) supporting the Reef Restoration and Adaptation Program. Here we present details of the platform configuration, a flight summary of its first campaign and a case study illustrating the capabilities of the new platform. In the case study presented, data was collected from two well-developed cumulus cloud cells which were similar in macrophysical properties but formed under markedly different aerosol regimes. We observed a strong difference in cloud microphysical properties. Higher aerosol concentrations led to more numerous and smaller cloud drops and suppressed warm rain. Our observations are consistent with the hypothesis that cumulus clouds, dominant over the GBR during summer, are amenable to marine cloud brightening. Our results demonstrate the practical utility of the new research aircraft through a focused case study, laying the groundwork for future scientific investigations of aerosol–cloud interactions.
{"title":"New airborne research facility observes sensitivity of cumulus cloud microphysical properties to aerosol regime over the great barrier reef†","authors":"Diana C. Hernandez-Jaramillo, Chris Medcraft, Ramon Campos Braga, Peter Butcherine, Adrian Doss, Brendan Kelaher, Daniel Rosenfeld and Daniel P. Harrison","doi":"10.1039/D4EA00009A","DOIUrl":"https://doi.org/10.1039/D4EA00009A","url":null,"abstract":"<p >Our work on aerosol–cloud–radiation interactions became hamstrung by the lack of a suitable aerosol and cloud microphysics equipped aircraft in Australia. To address this infrastructure gap, we have established a new airborne research platform, designed primarily for Marine Cloud Brightening (MCB) field studies but with broader applicability across diverse airborne research domains. This platform, comprising a Cessna 337 aircraft was outfitted with a comprehensive suite of meteorological, aerosol, and cloud microphysical instrumentation normally only found on much larger aircrafts. The aircraft has completed its first field deployment over the Great Barrier Reef (GBR) supporting the Reef Restoration and Adaptation Program. Here we present details of the platform configuration, a flight summary of its first campaign and a case study illustrating the capabilities of the new platform. In the case study presented, data was collected from two well-developed cumulus cloud cells which were similar in macrophysical properties but formed under markedly different aerosol regimes. We observed a strong difference in cloud microphysical properties. Higher aerosol concentrations led to more numerous and smaller cloud drops and suppressed warm rain. Our observations are consistent with the hypothesis that cumulus clouds, dominant over the GBR during summer, are amenable to marine cloud brightening. Our results demonstrate the practical utility of the new research aircraft through a focused case study, laying the groundwork for future scientific investigations of aerosol–cloud interactions.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 8","pages":" 861-871"},"PeriodicalIF":2.8,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00009a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141966429","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}