ACS ES&T Air最新文献

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Chlorine-Initiated Oxidation of Limonene under Simulated Indoor and Outdoor Lighting Conditions 模拟室内和室外光照条件下氯引发的柠檬烯氧化
ACS ES&T Air Pub Date : 2025-07-22 DOI: 10.1021/acsestair.5c00075
Pearl Abue, Mrinali Modi, Lea El Khoury and Lea Hildebrandt Ruiz*, 
{"title":"Chlorine-Initiated Oxidation of Limonene under Simulated Indoor and Outdoor Lighting Conditions","authors":"Pearl Abue,&nbsp;Mrinali Modi,&nbsp;Lea El Khoury and Lea Hildebrandt Ruiz*,&nbsp;","doi":"10.1021/acsestair.5c00075","DOIUrl":"https://doi.org/10.1021/acsestair.5c00075","url":null,"abstract":"<p >Limonene is the fourth most emitted biogenic volatile organic compound and is often used as a fragrance and emitted from personal care products, cleaning products, and others. Chlorine gas (Cl<sub>2</sub>), a precursor for Cl atoms, is emitted from anthropogenic activities, including cleaning, disinfection, and industrial activities, and it also forms from heterogeneous reactions involving sea salt. Thus, limonene and Cl radical precursors can both be present in indoor and outdoor environments. We studied the chlorine-initiated oxidation of limonene under indoor lighting (LED lights) and simulated outdoor lighting (a combination of UVA and LED lights) using an environmental chamber and a suite of instruments measuring gas and particle phase products. OH radicals formed and dominated the oxidation of limonene in the presence of NO<sub><i>x</i></sub>, Cl<sub>2</sub>, and LED lights, highlighting that Cl-initiated chemistry can generate OH chemistry in indoor environments, even in the absence of sunlight. Measurements from an iodide chemical ionization mass spectrometer showed gas phase reaction products from both Cl and OH addition to limonene, including nitrated species LIMANO<sub>3</sub> (C<sub>10</sub>H<sub>17</sub>NO<sub>4</sub>) and LIMALNO<sub>3</sub> (C<sub>10</sub>H<sub>17</sub>NO<sub>6</sub>). Secondary organic aerosol (SOA) yields were high, exceeding 1.1 in experiments with low NO<sub><i>x</i></sub> and high limonene concentrations, and showed strong dependence on temperature, NO<sub><i>x</i></sub>, and the VOC/Cl<sub>2</sub> ratio. These findings suggest that Cl<sub>2</sub> can contribute to the indoor and outdoor SOA formation from limonene oxidation through direct oxidation and secondary OH chemistry.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1586–1597"},"PeriodicalIF":0.0,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Theoretical Mapping of the Gas-Phase Ozonolysis of α-Pinene: Formation of First-Generation Products under Different Atmospheric Conditions α-蒎烯气相臭氧分解的理论映射:不同大气条件下第一代产物的形成
ACS ES&T Air Pub Date : 2025-07-21 DOI: 10.1021/acsestair.5c00101
Jing Chen, Christopher M. Kenseth, Joel A. Thornton and Henrik G. Kjaergaard*, 
{"title":"Theoretical Mapping of the Gas-Phase Ozonolysis of α-Pinene: Formation of First-Generation Products under Different Atmospheric Conditions","authors":"Jing Chen,&nbsp;Christopher M. Kenseth,&nbsp;Joel A. Thornton and Henrik G. Kjaergaard*,&nbsp;","doi":"10.1021/acsestair.5c00101","DOIUrl":"https://doi.org/10.1021/acsestair.5c00101","url":null,"abstract":"<p >Ozonolysis of α-pinene is a significant and well-established source of atmospheric secondary organic aerosol (SOA), which plays a pivotal role in climate, air quality, and human health. The products of α-pinene ozonolysis measured experimentally are typically characterized by only their molecular formulas, while their structures and formation mechanisms often remain unclear. In this work, we theoretically map the oxidation pathways, structures, and formation time scales of the major first-generation products formed from α-pinene ozonolysis by calculating the H-shift and bond-scission reaction rate coefficients of the peroxy (RO<sub>2</sub>) and alkoxy (RO) radicals that arise under atmospheric conditions with different RO<sub>2</sub> bimolecular reaction rates (<i>k</i><sub>bi</sub>): polluted (<i>k</i><sub>bi</sub> &gt; 0.2 s<sup>–1</sup>), moderate (0.2 s<sup>–1</sup> &gt; <i>k</i><sub>bi</sub> &gt; 0.01 s<sup>–1</sup>), and pristine (<i>k</i><sub>bi</sub> ≈ 0.01 s<sup>–1</sup>). In polluted environments, almost no RO<sub>2</sub> unimolecular reactions are of importance and ozonolysis leads to nitrates and small fragmented products. By contrast, in moderate to pristine atmospheres, C<sub>10</sub> highly oxygenated organic molecules (HOMs) with up to 12 oxygen atoms can form from either purely unimolecular or a combination of unimolecular and bimolecular reactions. Our results suggest that explicit chemical mechanisms of α-pinene ozonolysis used ubiquitously in the literature require significant revision in their treatment of unimolecular-isomerization and stereoisomer-specific reactions.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1625–1639"},"PeriodicalIF":0.0,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806900","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Determining Methane Emission Rates from Urban Compressed Natural Gas Stations Using Mobile Measurements and a New Urban Vertical Dispersion Parameterization 利用移动测量和新的城市垂直分散参数化确定城市压缩天然气站的甲烷排放率
ACS ES&T Air Pub Date : 2025-07-21 DOI: 10.1021/acsestair.5c00016
Yufei Huang, Yuheng Zhang, Conghui Xie, Yayong Liu, Yanrong Yang, Tianran Han, Jietao Zhou, Chang Liu, Haijiong Sun, Keyu Chen, Zhijun Wu and Shao-Meng Li*, 
{"title":"Determining Methane Emission Rates from Urban Compressed Natural Gas Stations Using Mobile Measurements and a New Urban Vertical Dispersion Parameterization","authors":"Yufei Huang,&nbsp;Yuheng Zhang,&nbsp;Conghui Xie,&nbsp;Yayong Liu,&nbsp;Yanrong Yang,&nbsp;Tianran Han,&nbsp;Jietao Zhou,&nbsp;Chang Liu,&nbsp;Haijiong Sun,&nbsp;Keyu Chen,&nbsp;Zhijun Wu and Shao-Meng Li*,&nbsp;","doi":"10.1021/acsestair.5c00016","DOIUrl":"https://doi.org/10.1021/acsestair.5c00016","url":null,"abstract":"<p >This study introduced a high-resolution mobile measurement method and a new Gaussian vertical dispersion parametrization for plume dispersion in urban surface, with an application to CH<sub>4</sub> emission measurements of compressed natural gas (CNG) stations in urban Beijing, China. Tracer release experiments were conducted at two urban sites, and the results showed that the vertical plume dispersion coefficient in urban surface has an exponential relationship with plume travel distance, despite the surface topology. The results were fitted to a new vertical dispersion parametrization: ln(<i>D<sub>z</sub></i>) = −2.42 × ln(<i>x</i>) + 6.28. Using the new vertical dispersion parametrization along with lateral dispersion widths mapped through mobile measurements, the CH<sub>4</sub> emission rates of CNG fueling stations were determined, with an average of 2.5 (95% CI [0.21,30]) kg h<sup>–1</sup> for normal operating conditions, and 0.56 (95% CI [0.07,4.4]) kg h<sup>–1</sup> for stations under nonoperating conditions. A CH<sub>4</sub> emission factor (EF) of CNG fueling stations in Beijing was calculated based on the measured CH<sub>4</sub> emission rate and the annual CNG consumption in transportation, with an average of 0.010 (95% CI [0.001,0.087]) kg/kg. This indicates that the CH<sub>4</sub> emission of CNG fueling stations is nonnegligible compared with the emission of natural gas vehicles and should be considered in an inventory study.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1488–1495"},"PeriodicalIF":0.0,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Quantifying Dissemination of Antibiotic Resistance Genes in Air from a Dairy Farm and Swine Farm 某奶牛场和养猪场空气中抗生素耐药基因的定量传播
ACS ES&T Air Pub Date : 2025-07-18 DOI: 10.1021/acsestair.5c00055
David A. Kormos, Gabriel Isaacman-VanWertz, Jactone A. Ogejo, Amy Pruden and Linsey C. Marr*, 
{"title":"Quantifying Dissemination of Antibiotic Resistance Genes in Air from a Dairy Farm and Swine Farm","authors":"David A. Kormos,&nbsp;Gabriel Isaacman-VanWertz,&nbsp;Jactone A. Ogejo,&nbsp;Amy Pruden and Linsey C. Marr*,&nbsp;","doi":"10.1021/acsestair.5c00055","DOIUrl":"https://doi.org/10.1021/acsestair.5c00055","url":null,"abstract":"<p >Farms are a suspected source of dissemination of antibiotic resistance genes (ARGs) to the atmosphere, but their contribution remains poorly quantified. This study investigated the concentrations, emission rates, and particle size distributions of ARGs in air around a dairy farm and swine farm, as well as in farm wastewater and soil as potential sources, during a yearlong sampling campaign. Analysis targeted genes corresponding to a cross-section of antibiotic classes used in human and veterinary medicine, along with 16S rRNA and <i>intI1</i> as indicators of total bacterial load and anthropogenic sources of ARGs, respectively. Two approaches were demonstrated for estimating emissions to account for the physical configurations of the farms. A custom sampler that collected size-resolved aerosol particles at a flow rate of 2.25 L/min only when the wind originated from the direction of interest was used to collect aerosol particles near potential sources. At the dairy and swine farms, <i>bla</i><sub><i>CTX-M1</i></sub> concentrations varied significantly by sampling location, averaging 10<sup>2</sup> gene copies per cubic meter (gc m<sup>–3</sup>) across seasons and peaking at 10<sup>4</sup> gc m<sup>–3</sup> during the summer sampling period. At the swine farm, maximum concentrations reached 10<sup>5</sup> gc m<sup>–3</sup> for <i>intI1</i>, <i>ermF</i>, and <i>qnrA</i> near the buildings’ exhaust fans. Emission rates reached ∼ 10<sup>5</sup> gc s<sup>–1</sup> for some ARGs, including <i>bla</i><sub><i>CTX-M1</i></sub>, and 10<sup>6</sup> gc s<sup>–1</sup> for <i>intI1</i>. ARGs were predominantly associated with coarse particles (&gt;5 μm) near emission sources and were also present in fine (&lt;1 μm) and accumulation (1–5 μm) mode particles near the source and at downwind locations, indicating potential for inhalation exposure and long-range transport.</p><p >An observational study reveals insights into sources, emissions, and transport of antibiotic resistance genes in the atmosphere around swine and dairy farms.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1552–1564"},"PeriodicalIF":0.0,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsestair.5c00055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dynamic Chemical Exposure from Face Masks Induced by Ambient Ozone Oxidation Chemistry 环境臭氧氧化化学诱导面罩的动态化学暴露
ACS ES&T Air Pub Date : 2025-07-17 DOI: 10.1021/acsestair.5c00160
Qifan Liu*, Runzeng Liu*, Scott A. Mabury and Jonathan P. D. Abbatt, 
{"title":"Dynamic Chemical Exposure from Face Masks Induced by Ambient Ozone Oxidation Chemistry","authors":"Qifan Liu*,&nbsp;Runzeng Liu*,&nbsp;Scott A. Mabury and Jonathan P. D. Abbatt,&nbsp;","doi":"10.1021/acsestair.5c00160","DOIUrl":"https://doi.org/10.1021/acsestair.5c00160","url":null,"abstract":"<p >The widespread use of face masks on a global scale calls for a comprehensive evaluation of the associated chemical exposure. However, researchers mainly focus on the chemicals directly emitted from masks, with no consideration given to their possible transformation chemistry and the associated potential health impacts during the use of masks. Here, via mask wearing experiments (by volunteers), ambient air-mask interaction experiments, and ozone-mask reaction experiments, we find that the chemical exposure will be substantially changed during mask wearing due to gas-mask multiphase reactions with ambient ozone. In particular, this ozone oxidation chemistry leads to the formation of gaseous carbonyl compounds and a surface-bound organophosphate ester tris(2,4-di-<i>tert</i>-butylphenyl) phosphate (TDtBPP, an emerging contaminant), with concentrations up to five times higher than those present in unused masks. While exposure assessments indicate that the health risks posed by gaseous carbonyl compounds and surface-bound organophosphate esters are likely to be minor, the present work emphasizes the importance of considering the dynamic evolution of mask-related chemicals when evaluating the overall chemical exposure related to face mask usage.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1784–1792"},"PeriodicalIF":0.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Traffic-Emitted Amines Promote New Particle Formation at Roadsides 交通排放的胺促进路边新颗粒的形成
ACS ES&T Air Pub Date : 2025-07-16 DOI: 10.1021/acsestair.5c00119
James Brean, Federica Bortolussi, Alex Rowell, David C. S. Beddows, Kay Weinhold, Peter Mettke, Maik Merkel, Avinash Kumar, Shawon Barua, Siddharth Iyer, Alexandra Karppinen, Hilda Sandström, Patrick Rinke, Alfred Wiedensohler, Mira Pöhlker, Miikka Dal Maso, Matti Rissanen, Zongbo Shi and Roy M. Harrison*, 
{"title":"Traffic-Emitted Amines Promote New Particle Formation at Roadsides","authors":"James Brean,&nbsp;Federica Bortolussi,&nbsp;Alex Rowell,&nbsp;David C. S. Beddows,&nbsp;Kay Weinhold,&nbsp;Peter Mettke,&nbsp;Maik Merkel,&nbsp;Avinash Kumar,&nbsp;Shawon Barua,&nbsp;Siddharth Iyer,&nbsp;Alexandra Karppinen,&nbsp;Hilda Sandström,&nbsp;Patrick Rinke,&nbsp;Alfred Wiedensohler,&nbsp;Mira Pöhlker,&nbsp;Miikka Dal Maso,&nbsp;Matti Rissanen,&nbsp;Zongbo Shi and Roy M. Harrison*,&nbsp;","doi":"10.1021/acsestair.5c00119","DOIUrl":"https://doi.org/10.1021/acsestair.5c00119","url":null,"abstract":"<p >New particle formation (NPF) is a major source of atmospheric aerosol particles, significantly influencing particle number concentrations in urban environments. High condensation and coagulation sinks at highly trafficked roadside sites should suppress NPF due to the low survival probability of clusters and new particles, however, observations show that roadside NPF is frequent and intense. Here, we investigate NPF at an urban background and roadside site in Central Europe using simultaneous measurements of sulfuric acid, amines, highly oxygenated organic molecules (HOMs), and particle number size distributions. We demonstrate that sulfuric acid and amines, particularly traffic-derived C<sub>2</sub>-amines, are the primary participants in particle formation. C<sub>2</sub>-amine concentrations at the roadside are enhanced by over a factor of 4 relative to the background, overcoming the effect of enhanced coagulation and condensation sinks. Using machine learning we identify a further but uncertain enhancing role of HOMs. These findings reveal the critical role of traffic emissions in urban NPF.</p><p >Traffic is a source of amines which enhance the formation rates of new particles.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1704–1713"},"PeriodicalIF":0.0,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsestair.5c00119","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806394","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mitigation of Indoor Ozone and Secondary Products from 222 nm Germicidal Ultraviolet Light Using Commercial Air Cleaners 商用空气净化器减少222 nm杀菌紫外线对室内臭氧和二次产物的影响
ACS ES&T Air Pub Date : 2025-07-16 DOI: 10.1021/acsestair.5c00138
Nadia Tahsini*, Selena Zhang, Matthew B. Goss, Seamus C. Frey, Yaowei Li, Jessica B. Smith, Norton T. Allen, M Pang, Richard D. Williamson, Frank N. Keutsch and Jesse H. Kroll*, 
{"title":"Mitigation of Indoor Ozone and Secondary Products from 222 nm Germicidal Ultraviolet Light Using Commercial Air Cleaners","authors":"Nadia Tahsini*,&nbsp;Selena Zhang,&nbsp;Matthew B. Goss,&nbsp;Seamus C. Frey,&nbsp;Yaowei Li,&nbsp;Jessica B. Smith,&nbsp;Norton T. Allen,&nbsp;M Pang,&nbsp;Richard D. Williamson,&nbsp;Frank N. Keutsch and Jesse H. Kroll*,&nbsp;","doi":"10.1021/acsestair.5c00138","DOIUrl":"https://doi.org/10.1021/acsestair.5c00138","url":null,"abstract":"<p >Far ultraviolet-C (UVC) light, especially germicidal UV light at 222 nm (GUV<sub>222</sub>), has received considerable attention for its potential to deactivate airborne pathogens indoors and prevent the spread of infectious disease. However, GUV<sub>222</sub> also generates ozone (O<sub>3</sub>), posing human health risks and initiating additional photochemistry that may degrade indoor air quality. Air cleaners present an opportunity to counteract the drawbacks of GUV<sub>222</sub> by removing harmful byproducts; however, to our knowledge, this has never been demonstrated. Here, we conduct laboratory experiments in a 7.5 m<sup>3</sup> Teflon chamber using two commercially available air cleaners─a manganese-oxide-catalyst “ozone cleaner” and an activated-carbon-HEPA “volatile organic compound (VOC) + particulate matter (PM) cleaner”─each simultaneously with a GUV<sub>222</sub> lamp. We show that both cleaner types remove a wide range of key pollutants, including O<sub>3</sub>, NO<sub>2</sub>, formaldehyde, VOCs, and particles. Application of chamber results to a photochemical model simulating chemistry in a 150 m<sup>3</sup> room suggests that a single cleaner can achieve modest reductions in O<sub>3</sub> levels and substantial reductions in secondary pollutant levels within typical indoor environments. These results indicate that indoor air pollutants from GUV<sub>222</sub> can be mitigated through the use of air cleaning technology, thereby improving indoor air quality while maximizing the potential benefit of germicidal UV for human health.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1750–1757"},"PeriodicalIF":0.0,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806508","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Kinetics and Radioactive Equilibrium of Radon and Radon Progenies in Indoor Air 室内空气中氡及其子体的动力学和放射性平衡
ACS ES&T Air Pub Date : 2025-07-16 DOI: 10.1021/acsestair.5c00115
Yong-Ha Kim*, Melaan Bender, Edward Laws and Wei-Hsung Wang, 
{"title":"Kinetics and Radioactive Equilibrium of Radon and Radon Progenies in Indoor Air","authors":"Yong-Ha Kim*,&nbsp;Melaan Bender,&nbsp;Edward Laws and Wei-Hsung Wang,&nbsp;","doi":"10.1021/acsestair.5c00115","DOIUrl":"https://doi.org/10.1021/acsestair.5c00115","url":null,"abstract":"<p >Human exposure to radon and radon progenies can lead to the development of respiratory diseases, including lung cancer. Accurate predictive models are needed to better understand the effects of inhaled radionuclides on human health. This study aimed at developing a theoretical/analytical approach to simultaneously predict time-dependent changes in the distributions of radon and radon progenies in the air, in aerosols, and on surfaces. Various indoor, aerosol, and radiological processes were combined to develop the approach. The developed approach conserves the total number of nuclides, but it neither requires iteration nor assumes a steady state or radioactive equilibrium. We verified the theoretical/analytical approach by comparing its accuracy to the analytical and steady-state solutions of kinetic equations for the behavior of radon and radon progenies, as well as the numerical analysis of the equations and measurements for the indoor concentrations of the radionuclides. The results of this study can provide useful insights that can enhance our understanding of the behavior of radon and radon progenies in indoor environments with limited ventilation (e.g., underground facilities) and facilitate radiation-induced health risk assessment in areas where precautions are warranted because of the potential for long-term exposure to radon.</p><p >Radon and radon progenies are potential lung carcinogens. This study presents simple approaches to better understand the behavior of radon and radon progenies in indoor environments.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1684–1693"},"PeriodicalIF":0.0,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsestair.5c00115","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Learning to Simulate Aerosol Dynamics with Graph Neural Networks 学习用图神经网络模拟气溶胶动力学
ACS ES&T Air Pub Date : 2025-07-14 DOI: 10.1021/acsestair.4c00261
Fabiana Ferracina, Payton Beeler, Mahantesh Halappanavar, Bala Krishnamoorthy, Marco Minutoli and Laura Fierce*, 
{"title":"Learning to Simulate Aerosol Dynamics with Graph Neural Networks","authors":"Fabiana Ferracina,&nbsp;Payton Beeler,&nbsp;Mahantesh Halappanavar,&nbsp;Bala Krishnamoorthy,&nbsp;Marco Minutoli and Laura Fierce*,&nbsp;","doi":"10.1021/acsestair.4c00261","DOIUrl":"https://doi.org/10.1021/acsestair.4c00261","url":null,"abstract":"<p >Aerosol effects on climate, weather, and air quality depend on characteristics of individual particles, which are tremendously diverse and change in time. Particle-resolved models are the only models able to capture this diversity in particle physiochemical properties, and these models are computationally expensive. As a strategy for accelerating particle-resolved microphysics models, we introduce Graph-based Learning of Aerosol Dynamics (GLAD) and use this model to train a surrogate of the particle-resolved model PartMC-MOSAIC. GLAD implements a graph-network-based simulator (GNS), a machine learning framework that has been used to emulate particle-based fluid dynamics simulations. In GLAD, each particle is represented as a node in a graph, and the evolution of the particle population over time is simulated through learned message passing. We demonstrate our GNS approach on a simple aerosol system that includes the condensation of sulfuric acid onto particles composed of sulfate, black carbon, organic carbon, and water. A graph with particles as nodes is constructed, and a graph neural network (GNN) is then trained by using the model output from PartMC-MOSAIC. The trained GNN can then be used for simulating and predicting aerosol dynamics over time. Results demonstrate the framework’s ability to accurately learn chemical dynamics and generalize across different scenarios, achieving efficient training and prediction times. We evaluate the performance across three scenarios, highlighting the framework’s robustness and adaptability in modeling aerosol microphysics and chemistry.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1426–1438"},"PeriodicalIF":0.0,"publicationDate":"2025-07-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806269","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interpreting Measurements of the Global Diurnal Variation of Fine Particulate Matter Using the GEOS-Chem Model 利用GEOS-Chem模型解释细颗粒物全球日变化的测量结果
ACS ES&T Air Pub Date : 2025-07-14 DOI: 10.1021/acsestair.5c00068
Yanshun Li*, Randall V. Martin, Yuanjian Zhang, Dandan Zhang, Aaron van Donkelaar, Haihui Zhu and Jun Meng, 
{"title":"Interpreting Measurements of the Global Diurnal Variation of Fine Particulate Matter Using the GEOS-Chem Model","authors":"Yanshun Li*,&nbsp;Randall V. Martin,&nbsp;Yuanjian Zhang,&nbsp;Dandan Zhang,&nbsp;Aaron van Donkelaar,&nbsp;Haihui Zhu and Jun Meng,&nbsp;","doi":"10.1021/acsestair.5c00068","DOIUrl":"https://doi.org/10.1021/acsestair.5c00068","url":null,"abstract":"<p >Globally distributed measurements of the diurnal variation of fine particulate matter (PM<sub>2.5</sub>) reveal a remarkable overall consistency with similar bimodal patterns and some regional variation, neither of which is well understood. We interpret these observations using the GEOS-Chem global model of atmospheric composition in its high-performance configuration (GCHP) at fine resolution of C180 (∼50 km). The base simulation overestimates the PM<sub>2.5</sub> accumulation overnight, leading to excessive diurnal amplitude and earlier PM<sub>2.5</sub> morning peaks than observations. These biases are reduced by applying sector- and species-wise diurnal scaling factors on anthropogenic emissions, by resolving the aerosol subgrid vertical gradient within the surface model layer, by applying revised wet deposition, and by revising the mixing coefficient in the boundary layer. Budget analyses indicate that the morning peak of PM<sub>2.5</sub> is likely driven by changes in the aerosol subgrid vertical gradient with fumigation after sunrise, that the concentration decrease until late afternoon is driven by boundary layer mixing and thermodynamic partitioning of a semivolatile aerosol to the gas phase, that the concentration increase during evening is driven by enhanced secondary chemical production and persistent primary anthropogenic emissions, and that the consistently high concentration overnight is driven by the balance between emissions, chemical production, and boundary layer mixing and deposition.</p>","PeriodicalId":100014,"journal":{"name":"ACS ES&T Air","volume":"2 8","pages":"1575–1585"},"PeriodicalIF":0.0,"publicationDate":"2025-07-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144806090","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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