Pub Date : 2025-12-03DOI: 10.1016/j.atmosenv.2025.121731
Chun Chen , Haijie Zhang , Yele Sun , Junling Li , Zhiqiang Zhang , Jian Gao , Rui Gao , Lianfang Wei , Nan Ma , Wanyun Xu , Pingqing Fu
Hydroxymethanesulfonate (HMS) is a key secondary organosulfur compound formed through aqueous-phase or heterogeneous atmospheric processes, significantly affecting the atmospheric sulfur budget. However, the relationship between HMS and PM2.5 components, as well as its formation mechanism, remains insufficiently explored. This study presents a comprehensive analysis of HMS at two sites in the North China Plain (NCP). Using offline filter analysis combined with theoretical calculations, we found that the HMS mass concentration in Gucheng during the winter of 2019 averaged 2.58 ± 2.56 μg/m3, approximately 1.5 times of that in Beijing during winter and 5.0 times of that in Beijing during autumn. This elevated concentration in Gucheng is attributed to higher relative humidity, elevated particle pH, and higher precursor concentrations. Correlation analyses demonstrated that aerosol liquid water content (AWC) is a key factor influencing HMS formation, while ammonium and nitrate may also contribute significantly. Theoretical calculations suggest that HMS formation primarily occurs through the reaction between SO32− and HCHO, with an additional contribution from the reaction of HSO3− with HCHO. Aqueous H2O and NH3 can act as catalysts, reducing the reaction barrier between HSO3− and HCHO from 9.76 kcal/mol (uncatalyzed) to 5.01 and 6.48 kcal/mol, respectively, thus promoting HMS formation. Increasing concentrations of aqueous H3O+ and NH4+ during polluted periods do not exhibit a catalytic effect but instead strongly inhibit HMS formation. These results indicate that a comprehensive consideration of the combined effects of various aqueous species is essential in atmospheric models.
{"title":"Characterization and influencing factors of hydroxymethanesulfonate (HMS) in the North China plain: integration of field measurements and theoretical calculations","authors":"Chun Chen , Haijie Zhang , Yele Sun , Junling Li , Zhiqiang Zhang , Jian Gao , Rui Gao , Lianfang Wei , Nan Ma , Wanyun Xu , Pingqing Fu","doi":"10.1016/j.atmosenv.2025.121731","DOIUrl":"10.1016/j.atmosenv.2025.121731","url":null,"abstract":"<div><div>Hydroxymethanesulfonate (HMS) is a key secondary organosulfur compound formed through aqueous-phase or heterogeneous atmospheric processes, significantly affecting the atmospheric sulfur budget. However, the relationship between HMS and PM<sub>2.5</sub> components, as well as its formation mechanism, remains insufficiently explored. This study presents a comprehensive analysis of HMS at two sites in the North China Plain (NCP). Using offline filter analysis combined with theoretical calculations, we found that the HMS mass concentration in Gucheng during the winter of 2019 averaged 2.58 ± 2.56 μg/m<sup>3</sup>, approximately 1.5 times of that in Beijing during winter and 5.0 times of that in Beijing during autumn. This elevated concentration in Gucheng is attributed to higher relative humidity, elevated particle pH, and higher precursor concentrations. Correlation analyses demonstrated that aerosol liquid water content (AWC) is a key factor influencing HMS formation, while ammonium and nitrate may also contribute significantly. Theoretical calculations suggest that HMS formation primarily occurs through the reaction between SO<sub>3</sub><sup>2−</sup> and HCHO, with an additional contribution from the reaction of HSO<sub>3</sub><sup>−</sup> with HCHO. Aqueous H<sub>2</sub>O and NH<sub>3</sub> can act as catalysts, reducing the reaction barrier between HSO<sub>3</sub><sup>−</sup> and HCHO from 9.76 kcal/mol (uncatalyzed) to 5.01 and 6.48 kcal/mol, respectively, thus promoting HMS formation. Increasing concentrations of aqueous H<sub>3</sub>O<sup>+</sup> and NH<sub>4</sub><sup>+</sup> during polluted periods do not exhibit a catalytic effect but instead strongly inhibit HMS formation. These results indicate that a comprehensive consideration of the combined effects of various aqueous species is essential in atmospheric models.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"367 ","pages":"Article 121731"},"PeriodicalIF":3.7,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145683969","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 : 2025-12-03DOI: 10.1016/j.atmosenv.2025.121728
Gaofeng Zhou , Junjie Wang , Wenting Lv , Yingjie Li , Yuan Li , Xuefeng Zhang , Li Han , Tao Jiang
The Sichuan Basin is one of China's most haze-prone regions due to its unique topography and stagnant meteorological conditions. To understand the winter haze formation mechanisms in the Sichuan Basin, a field campaign was conducted in a previously identified pollution hotspot (Southern Sichuan, December 2024 to February 2025). During this campaign, PM2.5 concentration averaged 63.79 ± 42.92 μg m−3, and we identified three haze episodes (H1-H3) during this campaign. The chemical speciation of fine aerosol was characterized using a quadrupole aerosol chemical speciation monitor (Q-ACSM), and the apportionment of organic aerosols (OAs) was solved by EPA PMF 5.0. The results indicated that OAs dominated the PM2.5 composition throughout this campaign, with OA concentrations particularly high in H1 (64.63 ± 20.77 μg m−3) and H2 (64.11 ± 19.05 μg m−3). Biomass burning organic aerosols (BBOA) and oxygenated organic aerosols (OOA) were the primary contributors to these high concentrations. The haze episodes resulted mainly from early-stage biomass burning emissions and less-aged OOA, occurring concurrently with the highest levels of aerosol liquid water content (ALWC), suggesting the humid air can favor the formation of haze. In addition to local emissions, regional transport synergized with meteorological conditions also significantly contributed to haze formation during this campaign, especially in H2 (38.2 %), quantified by a machine learning based deweathering analysis. This study underscores the intricate interplay between emissions, regional transport, and meteorology in driving haze formation in the Sichuan Basin and demonstrates the utility of machine learning aided diagnostics for source attribution and regulatory insights.
{"title":"Unveiling the causes of winter haze in southern Sichuan via observations and explainable machine learning","authors":"Gaofeng Zhou , Junjie Wang , Wenting Lv , Yingjie Li , Yuan Li , Xuefeng Zhang , Li Han , Tao Jiang","doi":"10.1016/j.atmosenv.2025.121728","DOIUrl":"10.1016/j.atmosenv.2025.121728","url":null,"abstract":"<div><div>The Sichuan Basin is one of China's most haze-prone regions due to its unique topography and stagnant meteorological conditions. To understand the winter haze formation mechanisms in the Sichuan Basin, a field campaign was conducted in a previously identified pollution hotspot (Southern Sichuan, December 2024 to February 2025). During this campaign, PM<sub>2.5</sub> concentration averaged 63.79 ± 42.92 μg m<sup>−3</sup>, and we identified three haze episodes (H1-H3) during this campaign. The chemical speciation of fine aerosol was characterized using a quadrupole aerosol chemical speciation monitor (Q-ACSM), and the apportionment of organic aerosols (OAs) was solved by EPA PMF 5.0. The results indicated that OAs dominated the PM<sub>2.5</sub> composition throughout this campaign, with OA concentrations particularly high in H1 (64.63 ± 20.77 μg m<sup>−3</sup>) and H2 (64.11 ± 19.05 μg m<sup>−3</sup>). Biomass burning organic aerosols (BBOA) and oxygenated organic aerosols (OOA) were the primary contributors to these high concentrations. The haze episodes resulted mainly from early-stage biomass burning emissions and less-aged OOA, occurring concurrently with the highest levels of aerosol liquid water content (ALWC), suggesting the humid air can favor the formation of haze. In addition to local emissions, regional transport synergized with meteorological conditions also significantly contributed to haze formation during this campaign, especially in H2 (38.2 %), quantified by a machine learning based deweathering analysis. This study underscores the intricate interplay between emissions, regional transport, and meteorology in driving haze formation in the Sichuan Basin and demonstrates the utility of machine learning aided diagnostics for source attribution and regulatory insights.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"367 ","pages":"Article 121728"},"PeriodicalIF":3.7,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145734459","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 : 2025-12-02DOI: 10.1016/j.atmosenv.2025.121729
Xi Huang , Dina Wang , Qing Zhang , Dayan Wang , Yuelong Shu , Shenglan Xiao
Influenza is a serious respiratory infection that imposes significant public health challenges. However, the precise impact of pollutants on influenza virus activity remains unclear. In this study, we aimed to investigate the effects of different air pollutants on the incidence of influenza-like illness (ILI), influenza A (Flu A), and influenza B (Flu B) in China based on nationwide air pollution and influenza data from 554 sentinel hospitals across 30 provinces and municipalities from 2014 to 2017. A Distributed Lag Nonlinear Model (DLNM) was employed to discern the lagged effects of six distinct air pollutants, namely PM2.5, PM10, O3, CO, SO2, and NO2, on the incidence of ILI, Flu A, and Flu B. Our analysis indicated that the relationship between air pollutants and influenza varied among ILI, Flu A, and Flu B, with Flu B being more sensitive to SO2 than Flu A. Elevated levels of air pollutants were generally associated with an increased risk of influenza; however, relative risks declined slightly at extreme concentrations of PM2.5, SO2, and NO2. These results highlight the complex associations between air pollution and influenza.
{"title":"Impact of ambient air pollutants on influenza-like illness, influenza A and influenza B: A nationwide time-series study in China","authors":"Xi Huang , Dina Wang , Qing Zhang , Dayan Wang , Yuelong Shu , Shenglan Xiao","doi":"10.1016/j.atmosenv.2025.121729","DOIUrl":"10.1016/j.atmosenv.2025.121729","url":null,"abstract":"<div><div>Influenza is a serious respiratory infection that imposes significant public health challenges. However, the precise impact of pollutants on influenza virus activity remains unclear. In this study, we aimed to investigate the effects of different air pollutants on the incidence of influenza-like illness (ILI), influenza A (Flu A), and influenza B (Flu B) in China based on nationwide air pollution and influenza data from 554 sentinel hospitals across 30 provinces and municipalities from 2014 to 2017. A Distributed Lag Nonlinear Model (DLNM) was employed to discern the lagged effects of six distinct air pollutants, namely PM2.5, PM10, O<sub>3</sub>, CO, SO<sub>2</sub>, and NO<sub>2</sub>, on the incidence of ILI, Flu A, and Flu B. Our analysis indicated that the relationship between air pollutants and influenza varied among ILI, Flu A, and Flu B, with Flu B being more sensitive to SO<sub>2</sub> than Flu A. Elevated levels of air pollutants were generally associated with an increased risk of influenza; however, relative risks declined slightly at extreme concentrations of PM2.5, SO<sub>2</sub>, and NO<sub>2</sub>. These results highlight the complex associations between air pollution and influenza.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"367 ","pages":"Article 121729"},"PeriodicalIF":3.7,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145683967","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 : 2025-12-02DOI: 10.1016/j.atmosenv.2025.121727
Mengli Chen , Jariya Kayee , Armin Sorooshian , Grace Betito , Paola Angela Bañaga , Rachel A. Braun , Maria Obiminda Cambaliza , Melliza Templonuevo Cruz , Alexander B. MacDonald , James Bernard Simpas , Connor Stahl , Iravati Ray , Reshmi Das , Zunya Wang , Xianfeng Wang
The global phase-out of leaded gasoline marked a major milestone in pollution control, yet modern uses of lead (Pb) continue to pose significant health risks, especially in low- and middle-income countries. In the Philippines, significant data gaps still exist despite increasing exposure. This study presents to the best of our knowledge, the first Pb isotopic fingerprinting of atmospheric aerosols in Metro Manila, Philippines, covering fine (0.56–1 μm) and coarse (5.6–10 μm) fractions, collected in 2018–2019. Results show that local sources, mainly industrial activities (45–62 %) and fossil fuel combustion (30–45 %), are now the dominant contributors to airborne Pb, while a minor legacy leaded gasoline and geogenic Pb persists (<18 %) through soil resuspension. Stable isotopes show no clear seasonal pattern. Together with 25 fold higher Pb concentration in the fine fraction, these indicate limited transboundary input. Regional comparison highlights overlapping Pb isotopic composition across Southeast Asia, but is distinct from areas farther north due to intensive coal use in China. The consistency between isotopic fingerprinting and Positive Matrix Factorization (PMF) results demonstrates the value of combining methods for robust source apportionment. These findings demonstrate the continuing importance of isotopic monitoring for distinguishing contemporary and legacy Pb sources and informing targeted air quality management in rapidly developing regions.
{"title":"Lead sources detected in Manila's air after the phase-out of leaded gasoline","authors":"Mengli Chen , Jariya Kayee , Armin Sorooshian , Grace Betito , Paola Angela Bañaga , Rachel A. Braun , Maria Obiminda Cambaliza , Melliza Templonuevo Cruz , Alexander B. MacDonald , James Bernard Simpas , Connor Stahl , Iravati Ray , Reshmi Das , Zunya Wang , Xianfeng Wang","doi":"10.1016/j.atmosenv.2025.121727","DOIUrl":"10.1016/j.atmosenv.2025.121727","url":null,"abstract":"<div><div>The global phase-out of leaded gasoline marked a major milestone in pollution control, yet modern uses of lead (Pb) continue to pose significant health risks, especially in low- and middle-income countries. In the Philippines, significant data gaps still exist despite increasing exposure. This study presents to the best of our knowledge, the first Pb isotopic fingerprinting of atmospheric aerosols in Metro Manila, Philippines, covering fine (0.56–1 μm) and coarse (5.6–10 μm) fractions, collected in 2018–2019. Results show that local sources, mainly industrial activities (45–62 %) and fossil fuel combustion (30–45 %), are now the dominant contributors to airborne Pb, while a minor legacy leaded gasoline and geogenic Pb persists (<18 %) through soil resuspension. Stable isotopes show no clear seasonal pattern. Together with 25 fold higher Pb concentration in the fine fraction, these indicate limited transboundary input. Regional comparison highlights overlapping Pb isotopic composition across Southeast Asia, but is distinct from areas farther north due to intensive coal use in China. The consistency between isotopic fingerprinting and Positive Matrix Factorization (PMF) results demonstrates the value of combining methods for robust source apportionment. These findings demonstrate the continuing importance of isotopic monitoring for distinguishing contemporary and legacy Pb sources and informing targeted air quality management in rapidly developing regions.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"367 ","pages":"Article 121727"},"PeriodicalIF":3.7,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145683970","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 : 2025-11-28DOI: 10.1016/j.atmosenv.2025.121713
Irfan Karim , Bernhard Rappenglück
This study integrates in-situ and satellite observations to characterize urban greenhouse gas (GHG) emissions across Houston, Texas USA. Surface-based background concentrations show seasonal reductions from ∼435 to ∼410 ppm for carbon dioxide (CO2) due to photosynthetic uptake, and from ∼2.02 to ∼1.88 ppm for methane (CH4) predominantly due to oxidation by the hydroxyl radical (OH). Boundary layer height corrected excess CO2 and CH4 (ΔCO2, ΔCH4) peak in winter (∼139.4 ppm, ∼5.5 ppm) and drop in summer (∼5.6 ppm, ∼0.08 ppm), highlighting emission seasonality. The observed annual ΔCH4/ΔCO2 ratio (9.4 ppb ppm−1) exceeds EDGAR and EPA inventory estimates by 65–70 %, and spatial mapping identifies key CH4 hotspots - such as McCarty and Blue Ridge landfills - with ratios larger than 40–70 ppb ppm−1, which are severely underrepresented in emission inventories.
Satellite-derived enhancements from OCO-3 and TROPOMI offer broader coverage but lack sensitivity to surface plumes. For example, in situ bivariate plots show sharp ΔCO2 enhancements >30 ppm and ΔCH4 up to ∼0.3 ppm over industrial zones like the Ship Channel, while satellite ΔXCO2 (∼5–7 ppm) and ΔXCH4 (∼0.03–0.04 ppm) show moderate enhancements over the urban core. TROPOMI NO2 (∼1 × 10−4 μmol/m2) and HCHO (∼2.0 × 10−4 mol/m2) enhancements further confirm co-located industrial emissions. This synthesis underscores the value of combining surface and satellite data for robust urban emission assessments and improved emission inventory evaluation.
{"title":"Integrating surface-based in-situ and satellite observations to characterize CO2 and CH4 emission hotspots in Houston, USA","authors":"Irfan Karim , Bernhard Rappenglück","doi":"10.1016/j.atmosenv.2025.121713","DOIUrl":"10.1016/j.atmosenv.2025.121713","url":null,"abstract":"<div><div>This study integrates in-situ and satellite observations to characterize urban greenhouse gas (GHG) emissions across Houston, Texas USA. Surface-based background concentrations show seasonal reductions from ∼435 to ∼410 ppm for carbon dioxide (CO<sub>2</sub>) due to photosynthetic uptake, and from ∼2.02 to ∼1.88 ppm for methane (CH<sub>4</sub>) predominantly due to oxidation by the hydroxyl radical (OH). Boundary layer height corrected excess CO<sub>2</sub> and CH<sub>4</sub> (ΔCO<sub>2</sub>, ΔCH<sub>4</sub>) peak in winter (∼139.4 ppm, ∼5.5 ppm) and drop in summer (∼5.6 ppm, ∼0.08 ppm), highlighting emission seasonality. The observed annual ΔCH<sub>4</sub>/ΔCO<sub>2</sub> ratio (9.4 ppb ppm<sup>−1</sup>) exceeds EDGAR and EPA inventory estimates by 65–70 %, and spatial mapping identifies key CH<sub>4</sub> hotspots - such as McCarty and Blue Ridge landfills - with ratios larger than 40–70 ppb ppm<sup>−1</sup>, which are severely underrepresented in emission inventories.</div><div>Satellite-derived enhancements from OCO-3 and TROPOMI offer broader coverage but lack sensitivity to surface plumes. For example, in situ bivariate plots show sharp ΔCO<sub>2</sub> enhancements >30 ppm and ΔCH<sub>4</sub> up to ∼0.3 ppm over industrial zones like the Ship Channel, while satellite ΔXCO<sub>2</sub> (∼5–7 ppm) and ΔXCH<sub>4</sub> (∼0.03–0.04 ppm) show moderate enhancements over the urban core. TROPOMI NO<sub>2</sub> (∼1 × 10<sup>−4</sup> μmol/m<sup>2</sup>) and HCHO (∼2.0 × 10<sup>−4</sup> mol/m<sup>2</sup>) enhancements further confirm co-located industrial emissions. This synthesis underscores the value of combining surface and satellite data for robust urban emission assessments and improved emission inventory evaluation.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"366 ","pages":"Article 121713"},"PeriodicalIF":3.7,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622271","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 : 2025-11-28DOI: 10.1016/j.atmosenv.2025.121705
Ali Ismaeel , Jin Wu , Amos P.K. Tai
Ammonia (NH3) emissions significantly impact air quality and the Earth's radiation balance through their interactions with other atmospheric chemical species to form particulate matter. Reducing NH3 emissions from croplands without compromising productivity is challenging due to the widespread and diffuse nature of NH3 sources. In the absence of direct monitoring networks, emission inventories provide the crucial basis for designing and implementing emission control measures. In South Asia (SA), knowledge of NH3 emissions at the regional scale is limited by the coarse-resolution global emission inventories, which carry significant uncertainties due to generalized emission factors. Here, we estimated remote sensing-based NH3 emissions from SA croplands at a 250-m spatial resolution between 2003 and 2020 by incorporating local knowledge of farming practices. Our estimates reveal that an average of 5.7 Tg NH3 is emitted annually from SA croplands. We found a ∼25 % increase in total NH3 emissions over the period, attributable to cropland expansion and a shift toward more fertilizer-demanding crop cultivation. A comparison of the modeled annual NH3 fluxes with global emission inventories reveals discrepancies in the range of −10 to +30 %. The comparison of total column NH3 concentrations retrieved from satellite observations and simulated by chemical transport model simulations using our fine-scale NH3 emission inventory shows a high correlation coefficient (r ≥ 0.47) but indicates an average bias of −21 %. We estimated that without adopting any mitigation strategies to reduce NH3 emissions, future climate change under specific Shared Socioeconomic Pathway (SSP2-RCP4.5) will exacerbate environmental pollution by increasing NH3 volatilization by 6 % in the 2050s. However, mitigation strategies, such as incorporating fertilizers into the soil at the time of crop sowing, could decrease NH3 emissions by 18 % even under future climate conditions, relative to current levels. Our work highlights the importance of strategic agricultural management to make the SA food systems more sustainable and resilient to climate change.
{"title":"Fine-scale estimates of ammonia emissions from South Asian croplands under changing climate","authors":"Ali Ismaeel , Jin Wu , Amos P.K. Tai","doi":"10.1016/j.atmosenv.2025.121705","DOIUrl":"10.1016/j.atmosenv.2025.121705","url":null,"abstract":"<div><div>Ammonia (NH<sub>3</sub>) emissions significantly impact air quality and the Earth's radiation balance through their interactions with other atmospheric chemical species to form particulate matter. Reducing NH<sub>3</sub> emissions from croplands without compromising productivity is challenging due to the widespread and diffuse nature of NH<sub>3</sub> sources. In the absence of direct monitoring networks, emission inventories provide the crucial basis for designing and implementing emission control measures. In South Asia (SA), knowledge of NH<sub>3</sub> emissions at the regional scale is limited by the coarse-resolution global emission inventories, which carry significant uncertainties due to generalized emission factors. Here, we estimated remote sensing-based NH<sub>3</sub> emissions from SA croplands at a 250-m spatial resolution between 2003 and 2020 by incorporating local knowledge of farming practices. Our estimates reveal that an average of 5.7 Tg NH<sub>3</sub> is emitted annually from SA croplands. We found a ∼25 % increase in total NH<sub>3</sub> emissions over the period, attributable to cropland expansion and a shift toward more fertilizer-demanding crop cultivation. A comparison of the modeled annual NH<sub>3</sub> fluxes with global emission inventories reveals discrepancies in the range of −10 to +30 %. The comparison of total column NH<sub>3</sub> concentrations retrieved from satellite observations and simulated by chemical transport model simulations using our fine-scale NH<sub>3</sub> emission inventory shows a high correlation coefficient (<em>r</em> ≥ 0.47) but indicates an average bias of −21 %. We estimated that without adopting any mitigation strategies to reduce NH<sub>3</sub> emissions, future climate change under specific Shared Socioeconomic Pathway (SSP2-RCP4.5) will exacerbate environmental pollution by increasing NH<sub>3</sub> volatilization by 6 % in the 2050s. However, mitigation strategies, such as incorporating fertilizers into the soil at the time of crop sowing, could decrease NH<sub>3</sub> emissions by 18 % even under future climate conditions, relative to current levels. Our work highlights the importance of strategic agricultural management to make the SA food systems more sustainable and resilient to climate change.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"366 ","pages":"Article 121705"},"PeriodicalIF":3.7,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145691535","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 : 2025-11-28DOI: 10.1016/j.atmosenv.2025.121693
Gopika Gupta , B.L. Madhavan , M. Venkat Ratnam
Assessing long-term changes in Aerosol Optical Depth (AOD) together with Aerosol Radiative Forcing Efficiency (ARFE, defined as radiative forcing per unit visible AOD) provides critical insight into the evolving role of different aerosol species in regional climate forcing. In this study, we analyse two decades of AOD trends (2001–2020) across eight climatically diverse regions using a multivariate regression framework, and quantify species-specific radiative effects with the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model. The regions were chosen to represent contrasting trends in total AOD. Our results show that sulfate aerosols, which account for the largest share of AOD over India (∼36–45 %), are the primary driver of increasing AOD and associated atmospheric warming. Black carbon (BC), although contributing only a minor fraction to total AOD (2–10 %), emerges as the dominant warming agent across most regions, with particularly strong forcing signals over the Middle East. In contrast, sea-salt (SS) aerosols exert the largest cooling influence, most prominently over the Southern African (SAF) region, partially offsetting warming from absorbing species. Europe, despite an overall decline in AOD, exhibits a slight increase in SS that sustains a regional cooling effect. These findings demonstrate that species composition, vertical distribution, and optical properties govern ARFE more strongly than the total AOD magnitude alone. By linking AOD trends with species-resolved radiative forcing efficiency across multiple regions, this study advances the interpretability of ARFE as a climate indicator and highlights its potential to inform policy-relevant assessment of aerosol-driven warming and cooling.
评估气溶胶光学深度(AOD)和气溶胶辐射强迫效率(ARFE,定义为每单位可见AOD的辐射强迫)的长期变化,为了解不同气溶胶种类在区域气候强迫中的演变作用提供了关键的见解。在本研究中,我们使用多元回归框架分析了8个气候多样化地区20年来的AOD趋势(2001-2020),并使用Santa Barbara DISORT大气辐射传输(SBDART)模型量化了物种特异性辐射效应。选择这些地区是为了代表总AOD的不同趋势。我们的研究结果表明,硫酸盐气溶胶占印度上空AOD的最大份额(~ 36 - 45%),是AOD增加和相关大气变暖的主要驱动力。黑碳(BC)虽然只占总AOD的一小部分(2 - 10%),但在大多数地区成为主要的变暖剂,在中东地区的强迫信号尤其强烈。相比之下,海盐(SS)气溶胶发挥了最大的降温影响,在南部非洲(SAF)地区最为突出,部分抵消了吸收物种造成的变暖。欧洲,尽管AOD总体下降,但SS略有增加,维持了区域降温效应。这些发现表明,物种组成、垂直分布和光学性质对ARFE的影响比AOD总量更大。通过将AOD趋势与多个区域的物种解决的辐射强迫效率联系起来,本研究提高了ARFE作为气候指标的可解释性,并强调了其为气溶胶驱动的增温和降温的政策相关评估提供信息的潜力。
{"title":"Deciphering aerosol impacts: Unravelling long-term AOD trends and radiative forcing across key regions","authors":"Gopika Gupta , B.L. Madhavan , M. Venkat Ratnam","doi":"10.1016/j.atmosenv.2025.121693","DOIUrl":"10.1016/j.atmosenv.2025.121693","url":null,"abstract":"<div><div>Assessing long-term changes in Aerosol Optical Depth (AOD) together with Aerosol Radiative Forcing Efficiency (ARFE, defined as radiative forcing per unit visible AOD) provides critical insight into the evolving role of different aerosol species in regional climate forcing. In this study, we analyse two decades of AOD trends (2001–2020) across eight climatically diverse regions using a multivariate regression framework, and quantify species-specific radiative effects with the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model. The regions were chosen to represent contrasting trends in total AOD. Our results show that sulfate aerosols, which account for the largest share of AOD over India (∼36–45 %), are the primary driver of increasing AOD and associated atmospheric warming. Black carbon (BC), although contributing only a minor fraction to total AOD (2–10 %), emerges as the dominant warming agent across most regions, with particularly strong forcing signals over the Middle East. In contrast, sea-salt (SS) aerosols exert the largest cooling influence, most prominently over the Southern African (SAF) region, partially offsetting warming from absorbing species. Europe, despite an overall decline in AOD, exhibits a slight increase in SS that sustains a regional cooling effect. These findings demonstrate that species composition, vertical distribution, and optical properties govern ARFE more strongly than the total AOD magnitude alone. By linking AOD trends with species-resolved radiative forcing efficiency across multiple regions, this study advances the interpretability of ARFE as a climate indicator and highlights its potential to inform policy-relevant assessment of aerosol-driven warming and cooling.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"367 ","pages":"Article 121693"},"PeriodicalIF":3.7,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145651835","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 : 2025-11-24DOI: 10.1016/j.atmosenv.2025.121706
Xinyao Lian , Jiajia Ji , Guomin Chen , Shuai Jiang , Weiqi Liang , Xindou Chen , Jianhui Guo , Yaqi Wang , Yingbin Fu , Jia Zhang , Xiaoheng Li , Jing Li , Yi Song
The individual and joint effects of short-term exposure to heat waves and ozone (O3) on mortality, particularly on nervous system disease mortality, need further investigation, as global warming leads to frequent heat waves and increased O3 concentrations. Heat waves were identified when the daily maximum apparent temperature reached or exceeded the temperature threshold (the 90th percentile of the temperature in 2019–2023) for at least 2, 3, or 4 consecutive days. High-level O3 was defined as daily maximum 8-h average O3 concentrations above 100 μg/m3. Based on 51,073 death cases from the Shenzhen Mortality Surveillance System in 2019–2023, we found significant individual and joint effects of short-term exposure to heat waves and high-level O3 on mortality, including all-cause non-accidental mortality, circulatory disease mortality, and nervous system disease mortality, employing a case-crossover design and conditional logistic regression models. Excess fractions of all-cause non-accidental deaths, circulatory disease deaths, and nervous system disease deaths attributable to heatwave and high levels of O3 exposure could be as high as 6.42 %, 8.28 %, and 13.21 %. In addition, we found that the elderly and males were more susceptible to joint exposure to heat waves and O3. This study provided a reference for the development of a region-specific early warning system for joint heat waves and O3, and highlighted the priority protection of susceptible populations during heatwaves and higher O3 levels.
{"title":"Short-term effects of exposure to heat waves and ambient ozone on mortality: a case-crossover study","authors":"Xinyao Lian , Jiajia Ji , Guomin Chen , Shuai Jiang , Weiqi Liang , Xindou Chen , Jianhui Guo , Yaqi Wang , Yingbin Fu , Jia Zhang , Xiaoheng Li , Jing Li , Yi Song","doi":"10.1016/j.atmosenv.2025.121706","DOIUrl":"10.1016/j.atmosenv.2025.121706","url":null,"abstract":"<div><div>The individual and joint effects of short-term exposure to heat waves and ozone (O<sub>3</sub>) on mortality, particularly on nervous system disease mortality, need further investigation, as global warming leads to frequent heat waves and increased O<sub>3</sub> concentrations. Heat waves were identified when the daily maximum apparent temperature reached or exceeded the temperature threshold (the 90th percentile of the temperature in 2019–2023) for at least 2, 3, or 4 consecutive days. High-level O<sub>3</sub> was defined as daily maximum 8-h average O<sub>3</sub> concentrations above 100 μg/m<sup>3</sup>. Based on 51,073 death cases from the Shenzhen Mortality Surveillance System in 2019–2023, we found significant individual and joint effects of short-term exposure to heat waves and high-level O<sub>3</sub> on mortality, including all-cause non-accidental mortality, circulatory disease mortality, and nervous system disease mortality, employing a case-crossover design and conditional logistic regression models. Excess fractions of all-cause non-accidental deaths, circulatory disease deaths, and nervous system disease deaths attributable to heatwave and high levels of O<sub>3</sub> exposure could be as high as 6.42 %, 8.28 %, and 13.21 %. In addition, we found that the elderly and males were more susceptible to joint exposure to heat waves and O<sub>3</sub>. This study provided a reference for the development of a region-specific early warning system for joint heat waves and O<sub>3</sub>, and highlighted the priority protection of susceptible populations during heatwaves and higher O<sub>3</sub> levels.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"366 ","pages":"Article 121706"},"PeriodicalIF":3.7,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622260","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}
Kathmandu Valley is one of the most densely populated cities in Nepal, facing significant air quality challenges. This study presents a comprehensive analysis based on twelve months of continuous air quality measurement data collected at the Khumaltar Air Quality Monitoring Station (ICIMOD AQMS), which is located in the southern part of the Kathmandu Valley. The study investigates particulate matter (PM10, PM2.5, PM (PM10–PM2.5)) alongside trace gases (O3, NO, SO2, and CO), focuses on their seasonal, diurnal variations, interspecies correlations, potential sources, and the impact of regional atmospheric transport. The results reveal that the annual PM2.5 concentration (49 ) largely exceeds the WHO air quality guideline of 5 . Pollutant concentrations show clear seasonal variation, with peaks during the winter and pre-monsoon seasons, and a noticeable decline during the monsoon. A strong correlation (r = 0.82, p = 0.00) between PM2.5 and NO indicates that fossil fuel combustion is a dominant source of fine particulate pollution. During the pre-monsoon season, O3 concentrations occasionally exceed 100 ppb (8-hr running average), with seasonal diurnal concentration observed close to 90 ppb in the afternoon. The study found that temperature and relative humidity significantly influence coarse PM levels, with a strong negative correlation (r = −0.89, p = 0.00) between coarse PM and the relative humidity, suggesting less resuspension under moist conditions. Furthermore, this study highlights the severe air pollution in the Kathmandu Valley throughout the year, driven primarily by local emissions, with regional atmospheric transport further contributing to poor air quality.
加德满都谷地是尼泊尔人口最密集的城市之一,面临着严重的空气质量挑战。本研究基于位于加德满都谷地南部的库穆塔尔空气质量监测站(ICIMOD AQMS)收集的12个月的连续空气质量测量数据进行了全面分析。该研究调查了颗粒物(PM10、PM2.5、PMC (PM10 - PM2.5))和微量气体(O3、NOX、SO2和CO),重点研究了它们的季节、日变化、种间相关性、潜在来源以及区域大气运输的影响。结果表明,PM2.5年浓度(49 μgm−3)大大超过WHO空气质量指标(5 μgm−3)。污染物浓度具有明显的季节变化,在冬季和季风前季节达到峰值,在季风期间明显下降。PM2.5与NOX呈强相关(r = 0.82, p = 0.00),表明化石燃料燃烧是细颗粒物污染的主要来源。在季风前季节,臭氧浓度偶尔超过100 ppb(8小时平均值),在下午观测到的季节性日浓度接近90 ppb。研究发现,温度和相对湿度显著影响粗粒PM水平,粗粒PM与相对湿度呈强负相关(r = - 0.89, p = 0.00),表明湿润条件下重悬浮较少。此外,这项研究强调了加德满都谷地全年严重的空气污染,主要是由当地排放造成的,区域大气运输进一步加剧了空气质量差。
{"title":"A year-long observational analysis of atmospheric trace gases and particulate matter in Kathmandu","authors":"Dikra Prasad Bajgai , Sagar Adhikari , Arshini Saikia , Bertrand Bessagnet , Suresh Pokhrel , Govinda Lamichhane , Deepak Gyawali , Ravi Sahu , Qianggong Zhang","doi":"10.1016/j.atmosenv.2025.121704","DOIUrl":"10.1016/j.atmosenv.2025.121704","url":null,"abstract":"<div><div>Kathmandu Valley is one of the most densely populated cities in Nepal, facing significant air quality challenges. This study presents a comprehensive analysis based on twelve months of continuous air quality measurement data collected at the Khumaltar Air Quality Monitoring Station (ICIMOD AQMS), which is located in the southern part of the Kathmandu Valley. The study investigates particulate matter (PM<sub>10</sub>, PM<sub>2.5</sub>, PM<span><math><msub><mrow></mrow><mrow><mi>C</mi></mrow></msub></math></span> (PM<sub>10</sub>–PM<sub>2.5</sub>)) alongside trace gases (O<sub>3</sub>, NO<span><math><msub><mrow></mrow><mrow><mi>X</mi></mrow></msub></math></span>, SO<sub>2</sub>, and CO), focuses on their seasonal, diurnal variations, interspecies correlations, potential sources, and the impact of regional atmospheric transport. The results reveal that the annual PM<sub>2.5</sub> concentration (49 <span><math><mrow><mi>μ</mi><mtext>g</mtext><mspace></mspace><msup><mrow><mtext>m</mtext></mrow><mrow><mo>−</mo><mn>3</mn></mrow></msup></mrow></math></span>) largely exceeds the WHO air quality guideline of 5 <span><math><mrow><mi>μ</mi><mtext>g</mtext><mspace></mspace><msup><mrow><mtext>m</mtext></mrow><mrow><mo>−</mo><mn>3</mn></mrow></msup></mrow></math></span>. Pollutant concentrations show clear seasonal variation, with peaks during the winter and pre-monsoon seasons, and a noticeable decline during the monsoon. A strong correlation (r = 0.82, p = 0.00) between PM<sub>2.5</sub> and NO<span><math><msub><mrow></mrow><mrow><mi>X</mi></mrow></msub></math></span> indicates that fossil fuel combustion is a dominant source of fine particulate pollution. During the pre-monsoon season, O<sub>3</sub> concentrations occasionally exceed 100 ppb (8-hr running average), with seasonal diurnal concentration observed close to 90 ppb in the afternoon. The study found that temperature and relative humidity significantly influence coarse PM levels, with a strong negative correlation (r = −0.89, p = 0.00) between coarse PM and the relative humidity, suggesting less resuspension under moist conditions. Furthermore, this study highlights the severe air pollution in the Kathmandu Valley throughout the year, driven primarily by local emissions, with regional atmospheric transport further contributing to poor air quality.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"366 ","pages":"Article 121704"},"PeriodicalIF":3.7,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145623420","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 : 2025-11-22DOI: 10.1016/j.atmosenv.2025.121694
Ashish Gupta, Deepika Bhattu
Carbonaceous aerosols (CA) strongly impact regional and global climate through their light-absorbing and scattering properties, yet their effects remain uncertain in dust-influenced regions. We investigated the optical properties, source contributions, and radiative impacts of CA at two climatically distinct regions in northwestern India: an arid region (AR, Jodhpur; post-monsoon) and a semi-arid region (SAR, Kota; winter). Mean absorption Ångström exponent (AAE) values were comparable between the two regions (AR: 1.416 ± 0.173; SAR: 1.395 ± 0.069), but temporal cluster analysis revealed source-specific variability, with lower AAE during traffic-dominated periods (∼1.30) and elevated AAE during solid fuel and biomass combustion (1.68 in AR and 1.52 in SAR). While equivalent BC (eBC) levels were higher in AR with a relatively uniform liquid-fuel contribution (BClf = 80.06 ± 1.98 %), the mass absorption cross-section of BC (MACBC) in SAR was ∼4.5X greater, driven by local solid fuel combustion and transported biomass burning emissions (BCsf = 34.61 ± 6.88 %). Mie modelling indicated higher SSA in AR due to higher contribution of mineral dust, in contrast to SAR, where carbonaceous aerosols caused stronger absorption, forward scattering, and higher imaginary refractive index (kOBD). Although absorption enhancement (Eλ) was slightly higher in AR (∼1.11 vs. ∼0.99), SAR aerosols nearly doubled the warming potential (ΔRFE), with RFE values of ∼0.87 W/m2 in SAR versus ∼0.43 W/m2 in AR. These findings highlight strong source-specific and site-specific variability in aerosol absorption and radiative, emphasizing the need to integrate region-specific parameters into climate models and air quality assessments for data-scarce arid and semi-arid South Asian environments.
{"title":"Optical properties of carbonaceous aerosols and their radiative effects in arid and semi-arid regions of northwestern India","authors":"Ashish Gupta, Deepika Bhattu","doi":"10.1016/j.atmosenv.2025.121694","DOIUrl":"10.1016/j.atmosenv.2025.121694","url":null,"abstract":"<div><div>Carbonaceous aerosols (CA) strongly impact regional and global climate through their light-absorbing and scattering properties, yet their effects remain uncertain in dust-influenced regions. We investigated the optical properties, source contributions, and radiative impacts of CA at two climatically distinct regions in northwestern India: an arid region (AR, Jodhpur; post-monsoon) and a semi-arid region (SAR, Kota; winter). Mean absorption Ångström exponent (AAE) values were comparable between the two regions (AR: 1.416 ± 0.173; SAR: 1.395 ± 0.069), but temporal cluster analysis revealed source-specific variability, with lower AAE during traffic-dominated periods (∼1.30) and elevated AAE during solid fuel and biomass combustion (1.68 in AR and 1.52 in SAR). While equivalent BC (eBC) levels were higher in AR with a relatively uniform liquid-fuel contribution (BC<sub>lf</sub> = 80.06 ± 1.98 %), the mass absorption cross-section of BC (MAC<sub>BC</sub>) in SAR was ∼4.5X greater, driven by local solid fuel combustion and transported biomass burning emissions (BC<sub>sf</sub> = 34.61 ± 6.88 %). Mie modelling indicated higher SSA in AR due to higher contribution of mineral dust, in contrast to SAR, where carbonaceous aerosols caused stronger absorption, forward scattering, and higher imaginary refractive index (<em>k</em><sub><em>OBD</em></sub>). Although absorption enhancement (E<sub>λ</sub>) was slightly higher in AR (∼1.11 vs. ∼0.99), SAR aerosols nearly doubled the warming potential (ΔRFE), with RFE values of ∼0.87 W/m<sup>2</sup> in SAR versus ∼0.43 W/m<sup>2</sup> in AR. These findings highlight strong source-specific and site-specific variability in aerosol absorption and radiative, emphasizing the need to integrate region-specific parameters into climate models and air quality assessments for data-scarce arid and semi-arid South Asian environments.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"366 ","pages":"Article 121694"},"PeriodicalIF":3.7,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145622270","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}