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Technical note: Refining δ15N isotopic fingerprints of local NOx for accurate source identification of nitrate in PM2.5 技术说明:完善当地 NOx 的 δ15N 同位素指纹,准确识别 PM2.5 中硝酸盐的来源
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-27 DOI: 10.5194/egusphere-2024-1621
Hao Xiao, Qinkai Li, Shiyuan Ding, Wenjing Dai, Gaoyang Cui, Xiaodong Li
{"title":"Technical note: Refining δ15N isotopic fingerprints of local NOx for accurate source identification of nitrate in PM2.5","authors":"Hao Xiao, Qinkai Li, Shiyuan Ding, Wenjing Dai, Gaoyang Cui, Xiaodong Li","doi":"10.5194/egusphere-2024-1621","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1621","url":null,"abstract":"<strong>Abstract.</strong> Stable nitrogen isotopic composition (δ<sup>15</sup>N) has proven to be a valuable tool for identifying sources of nitrates (NO<sub>3</sub><sup>–</sup>) in PM<sub>2.5</sub>. However, the absence of a systematic study on the δ<sup>15</sup>N values of domestic NOx sources hinders accurate identification of NO<sub>3</sub><sup>–</sup> sources in China. Here, we systematically determined and refined δ<sup>15</sup>N values for six categories of NOx sources in the local Tianjin area using an active sampling method. Moreover, the δ<sup>15</sup>N values of NO<sub>3</sub><sup>–</sup> in PM<sub>2.5</sub> were measured during pre-heating, mid-heating and late-heating periods, which are the most heavily polluted in Tianjin. Results shown that the representative nature and region-specific characteristics of isotopic fingerprints for six categories of NOx sources in Tianjin. The Bayesian isotope mixing (MixSIAR) model demonstrated that coal combustion, biomass burning, and vehicle exhaust collectively contributed more than 60 %, dominating the sources of NO<sub>3</sub><sup>–</sup> during sampling periods in Tianjin. However, failure to consider the isotopic signatures of local NOx sources could result in an underestimation of the contribution from coal combustion. Additionally, the absence of industrial sources, an uncharacterized source in previous studies, may directly result in the contribution fraction of other sources being overestimated by the model more than 15 %. Notably, as the number of sources input to the model increased, the contribution of various NOx sources was becoming more stable, and the inter-influence between various sources significantly reduced. This study demonstrated that the refined isotopic fingerprint in a region-specific context could more effectively distinguish source of NO<sub>3</sub><sup>–</sup>, thereby providing valuable insights for controlling NO<sub>3</sub><sup>–</sup> pollution.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"131 10 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Potential impacts of marine fuel regulations on Arctic clouds and radiative feedbacks 海洋燃料法规对北极云层和辐射反馈的潜在影响
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-27 DOI: 10.5194/egusphere-2024-1891
Luís Filipe Escusa dos Santos, Hannah C. Frostenberg, Alejandro Baró Pérez, Annica M. L. Ekman, Luisa Ickes, Erik S. Thomson
{"title":"Potential impacts of marine fuel regulations on Arctic clouds and radiative feedbacks","authors":"Luís Filipe Escusa dos Santos, Hannah C. Frostenberg, Alejandro Baró Pérez, Annica M. L. Ekman, Luisa Ickes, Erik S. Thomson","doi":"10.5194/egusphere-2024-1891","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1891","url":null,"abstract":"&lt;strong&gt;Abstract.&lt;/strong&gt; Increased surface warming over the Arctic, triggered by increased greenhouse gas concentrations and feedback processes in the climate system, has been causing a steady decline in sea-ice extent and thickness. With the retreating sea-ice, shipping activity will likely increase in the future driven by economic activity and the potential for realizing time and fuel savings from transiting shorter trade routes. Moreover, over the last decade, the global shipping sector has been subject to regulatory changes, that affect the physicochemical properties of exhaust particles. International regulations aiming to reduce SO&lt;sub&gt;x&lt;/sub&gt; and particulate matter (PM) emissions, mandate ships to burn fuels with reduced sulfur content or alternatively, use wet scrubbing as exhaust after-treatment when using fuels with sulfur contents exceeding regulatory limits. Compliance measures affect the physicochemical properties of exhaust particles and their cloud condensation nuclei (CCN) activity in different ways, with the potential to have both direct and indirect impacts on atmospheric processes such as the formation and lifetime of clouds. Given the relatively pristine Arctic environment, ship exhaust particle emissions could be a large perturbation to natural baseline Arctic aerosol concentrations. Low-level stratiform mixed-phase clouds cover large areas of the Arctic region and play an important role in the regional energy budget. Results from laboratory marine engine measurements, which investigated the impact of fuel sulfur content (FSC) reduction and wet scrubbing on exhaust particle properties, motivate the use of large eddy simulations to further investigate how such particles may influence the micro- and macrophysical properties of a stratiform mixed-phase cloud case observed during the Arctic Summer Cloud Ocean Study campaign. Simulated enhancements of ship exhaust particles predominantly affected the liquid-phase properties of the cloud and led to a decrease in liquid surface precipitation, increased cloud albedo and increased longwave surface warming. The magnitude of the impact strongly depended on ship exhaust particle concentration, hygroscopicity, and size where the effect of particle size dominated the impact of hygroscopicity. While low FSC exhaust particles were mostly observed to affect cloud properties at exhaust particle concentrations of 1000 cm&lt;sup&gt;-3&lt;/sup&gt;, exhaust wet scrubbing already led to significant changes at concentrations of 100 cm&lt;sup&gt;-3&lt;/sup&gt;. Additional simulations with cloud ice water path increased from ≈5.5 g m&lt;sup&gt;-2&lt;/sup&gt; to ≈9.3 g m&lt;sup&gt;-2&lt;/sup&gt;, show more muted responses to ship exhaust perturbations but revealed that exhaust perturbations may even lead to a slight radiative cooling effect depending on the microphysical state of the cloud. The regional impact of shipping activity on Arctic cloud properties may, therefore, strongly depend on ship fuel type, whether ships utilize wet scrubbers, and","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"33 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Extreme Heat and Wildfire Emissions Enhance Volatile Organic Compounds: Insights on Future Climate 极端高温和野火排放会增加挥发性有机化合物:对未来气候的启示
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-27 DOI: 10.5194/egusphere-2024-1808
Christian Mark Garcia Salvador, Jeffrey D. Wood, Emma Grace Cochran, Hunter A. Seubert, Bella D. Kamplain, Sam S. Overby, Kevin R. Birdwell, Lianhong Gu, Melanie A. Mayes
{"title":"Extreme Heat and Wildfire Emissions Enhance Volatile Organic Compounds: Insights on Future Climate","authors":"Christian Mark Garcia Salvador, Jeffrey D. Wood, Emma Grace Cochran, Hunter A. Seubert, Bella D. Kamplain, Sam S. Overby, Kevin R. Birdwell, Lianhong Gu, Melanie A. Mayes","doi":"10.5194/egusphere-2024-1808","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1808","url":null,"abstract":"<strong>Abstract.</strong> Climate extremes are projected to cause unprecedented deviations in the emission and transformation of volatile organic compounds (VOCs), which trigger feedback mechanisms that will impact the atmospheric oxidation and formation of aerosols and clouds. However, the response of VOCs to future conditions such as extreme heat and wildfire events is still uncertain. This study explored the modification of the mixing ratio and distribution of several anthropogenic and biogenic VOCs in a temperate oak–hickory–juniper forest as a response to increased temperature and transported biomass burning plumes. A chemical ionization mass spectrometer was deployed on a tower at a height of 32 m in rural central Missouri, United States, for the continuous and in situ measurement of VOCs from June to August of 2023. The maximum observed temperature in the region was 38 °C, and during multiple episodes the temperature remained above 32 °C for several hours. Biogenic VOCs such as isoprene and monoterpene followed closely the temperature daily profile but at varying rates, whereas anthropogenic VOCs were insensitive to elevated temperature. During the measurement period, wildfire emissions were transported to the site and substantially increased the mixing ratios of acetonitrile and benzene, which are produced from burning of biomass. An in-depth analysis of the mass spectra revealed more than 250 minor compounds, such as formamide and methylglyoxal. The overall volatility, O:C, and H:C ratios of the extended list of VOCs responded to the changes in extreme heat and the presence of combustion plumes. Multivariate analysis also clustered the compounds into five factors, which highlighted the sources of the unaccounted-for VOCs. Overall, results here underscore the imminent effect of extreme heat and wildfire on VOC variability, which is important in understanding future interactions between climate and atmospheric chemistry.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"8 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Global scenarios of anthropogenic mercury emissions 全球人为汞排放情景
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-27 DOI: 10.5194/acp-24-7385-2024
Flora Maria Brocza, Peter Rafaj, Robert Sander, Fabian Wagner, Jenny Marie Jones
{"title":"Global scenarios of anthropogenic mercury emissions","authors":"Flora Maria Brocza, Peter Rafaj, Robert Sander, Fabian Wagner, Jenny Marie Jones","doi":"10.5194/acp-24-7385-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7385-2024","url":null,"abstract":"Abstract. Anthropogenic mercury (Hg) emissions to the atmosphere are a long-lived hazard to human and environmental health. The UN Minamata Convention on Mercury is seeking to lower anthropogenic mercury emissions through a mix of policies from banning certain Hg uses to reducing unintentional Hg release from different activities. In addition to independent Hg policy, strategies to mitigate greenhouse gases, particulate matter (PM) and SO2 may also lower Hg emissions as a co-benefit. This study uses the Greenhouse Gas–Air Pollution Interactions and Synergies (GAINS) model to examine the effect of different clean air and climate policies on future global Hg emissions. The baseline scenario assumes current trends for energy use and Hg emissions as well as current legislation for clean air, mercury and climate policy. In addition, we explore the impact of the Minamata Convention, the co-benefits of climate and stringent air pollution policies, and maximum feasible reduction measures for Hg. Hg emission projections until 2050 show noticeable reductions in combustion sectors for all scenarios due to a decrease in global fossil fuel and traditional biomass use, leading to emission reductions of 33 % at baseline and up to 90 % when combining stringent climate controls and the most efficient Hg controls. Cement and non-ferrous metal emissions increase in all scenarios with current air pollution policy but could be reduced by up to 72 % and 46 %, respectively, in 2050 with stringent Hg-specific measures. Other emissions (including waste) are a significant source of uncertainty in this study, and their projections range between a 22 % increase and a 54 % decrease in 2050, depending on both climate and clean air policy. The largest absolute reduction potential for Hg abatement but also the largest uncertainties regarding absolute emissions lie in small-scale and artisanal gold production, where abatement measures could eliminate annual Hg emissions in the range of 601–1371 t (95 % confidence interval), although the uncertainties in the estimate are so high that they might eclipse reduction efforts in all other sectors. In total, 90 % of Hg emissions are covered by provisions of the Minamata Convention. Overall, the findings emphasize the necessity to implement targeted Hg control policies in addition to stringent climate, PM and SO2 policies to achieve significant reductions in Hg emissions.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"22 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461946","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Future reduction of cold extremes over East Asia due to thermodynamic and dynamic warming 热力学和动力学变暖导致东亚地区未来极端寒冷天气减少
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-27 DOI: 10.5194/acp-24-7347-2024
Donghuan Li, Tianjun Zhou, Youcun Qi, Liwei Zou, Chao Li, Wenxia Zhang, Xiaolong Chen
{"title":"Future reduction of cold extremes over East Asia due to thermodynamic and dynamic warming","authors":"Donghuan Li, Tianjun Zhou, Youcun Qi, Liwei Zou, Chao Li, Wenxia Zhang, Xiaolong Chen","doi":"10.5194/acp-24-7347-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7347-2024","url":null,"abstract":"Abstract. Cold extremes have large impacts on human society. Understanding the physical processes dominating the changes in cold extremes is crucial for a reliable projection of future climate change. The observed cold extremes have decreased during the last several decades, and this trend will continue under future global warming. Here, we quantitatively identify the contributions of dynamic (changes in large-scale atmospheric circulation) and thermodynamic (rising temperatures resulting from global warming) effects to East Asian cold extremes in the past several decades and in a future warm climate by using two sets of large-ensemble simulations of climate models. We show that the dynamic component accounts for over 80 % of the cold-month (coldest 5 % boreal winter months) surface air temperature (SAT) anomaly over the past 5 decades. However, in a future warm climate, the thermodynamic change is the main contributor to the decreases in the intensity and occurrence probability of East Asian cold extremes, while the dynamic change is also contributive. The intensity of East Asian cold extremes will decrease by around 5 °C at the end of the 21st century, in which the thermodynamic (dynamic) change contributes approximately 75 % (25 %). The present-day (1986–2005) East Asian cold extremes will almost never occur after around 2035, and this will happen 10 years later due solely to thermodynamic change. The upward trend of a positive Arctic Oscillation-like sea level pressure pattern dominates the changes in the dynamic component. The finding provides a useful reference for policymakers in climate change adaptation activities.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"38 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461805","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Brown carbon aerosol in rural Germany: sources, chemistry, and diurnal variations 德国农村地区的棕碳气溶胶:来源、化学性质和昼夜变化
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-26 DOI: 10.5194/egusphere-2024-1848
Feng Jiang, Harald Saathoff, Junwei Song, Hengheng Zhang, Linyu Gao, Thomas Leisner
{"title":"Brown carbon aerosol in rural Germany: sources, chemistry, and diurnal variations","authors":"Feng Jiang, Harald Saathoff, Junwei Song, Hengheng Zhang, Linyu Gao, Thomas Leisner","doi":"10.5194/egusphere-2024-1848","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1848","url":null,"abstract":"<strong>Abstract.</strong> Brown carbon aerosol (BrC) is one major contributor to atmospheric air pollution in Europe, especially in winter. Therefore, we studied the chemical composition, diurnal variation, and sources of BrC from 17<sup>th</sup> February to 16<sup>th</sup> March at a rural location in southwest Germany. In total, 178 potential BrC molecules (including 7 nitro aromatic compounds, NACs) were identified in the particle phase comprising on average 63 ± 32 ng m<sup>−3</sup>, and 31 potential BrC (including 4 NACs) molecules were identified in the gas phase contributing on average 6.2 ± 5.0 ng m<sup>−3</sup> during the whole campaign. The 178 potential BrC molecules only accounted for 2.3 ± 1.5 % of the total organic mass, but can explain 11 ± 11 % of the total BrC absorption at 370 nm, assuming an average mass absorption coefficient at 370 nm (MAC<sub>370</sub>) of 9.5 m<sup>2</sup> g<sup>−1</sup>. A few BrC molecules dominated the total BrC absorption. In addition, diurnal variations show that gas phase BrC was higher at daytime and lower at night. It was mainly controlled by secondary formation (e.g. photooxidation) and particle-to-gas partitioning. Correspondingly, the particle phase BrC was lower at daytime and higher at nighttime. Secondary formation dominates the particle-phase BrC with 61 ± 21 %, while 39 ± 21 % originated from biomass burning. Furthermore, the particle-phase BrC showed decreasing light absorption due to photochemical aging. This study extends the current understanding of real-time behaviors of brown carbon aerosol in the gas and particle phase at a location characteristic for the central Europe.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"17 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations 通过长期大气观测揭示亚洲东部氢氟碳化合物(HFC)排放明显加速的情况
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-26 DOI: 10.5194/acp-24-7309-2024
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, Sunyoung Park
{"title":"Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations","authors":"Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, Sunyoung Park","doi":"10.5194/acp-24-7309-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7309-2024","url":null,"abstract":"Abstract. Hydrofluorocarbons (HFCs) are powerful anthropogenic greenhouse gases (GHGs) with high global-warming potentials (GWPs). They have been widely used as refrigerants, insulation foam-blowing agents, aerosol propellants, and fire suppression agents. Since the mid-1990s, emissions of HFCs have been increasing rapidly as they are used in many applications to replace ozone-depleting chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs) whose consumption and production have been phased out under the Montreal Protocol (MP). Due to the high GWP of HFCs, the Kigali Amendment to the MP requires the phasedown of production and consumption of HFCs to gradually achieve an 80 %–85 % reduction by 2047, starting in 2019 for non-Article 5 (developed) countries with a 10 % reduction against each defined baseline and later schedules for Article 5 (developing) countries. In this study, we have examined long-term high-precision measurements of atmospheric abundances of five major HFCs (HFC-134a, HFC-143a, HFC-32, HFC-125, and HFC-152a) at Gosan station, Jeju Island, South Korea, from 2008 to 2020. Background abundances of HFCs gradually increased, and the inflow of polluted air masses with elevated abundances from surrounding source regions were detected over the entire period. From these pollution events, we inferred regional and country-specific HFC emission estimates using two independent Lagrangian particle dispersion models and Bayesian inversion frameworks (FLEXPART-FLEXINVERT+ and NAME-InTEM). The spatial distribution of the derived “top-down” (measurement based) emissions for all HFCs shows large fluxes from megacities and industrial areas in the region. Our most important finding is that HFC emissions in eastern China and Japan have sharply increased from 2016 to 2018. The contribution of East Asian HFC emissions to the global total increased from 9 % (2008–2014) to 13 % (2016–2020). In particular, HFC emissions in Japan (Annex I country) rose rapidly from 2016 onward, with accumulated total inferred HFC emissions being ∼ 114 Gg yr−1, which is ∼ 76 Gg yr−1 higher for 2016–2020 than the “bottom-up” (i.e., based on activity data and emission factors) emissions of ∼ 38 Gg yr−1 reported to the United Nations Framework Convention on Climate Change (UNFCCC). This is likely related to the increase in domestic demand in Japan for refrigerants and air-conditioning-system-related products and incomplete accounting. A downward trend of HFC emissions that started in 2019 reflects the effectiveness of the F-gas policy in Japan. Eastern China and South Korea, though not obligated to report to the UNFCCC, voluntarily reported emissions, which also show differences between top-down and bottom-up emission estimates, demonstrating the need for atmospheric measurements, comprehensive data analysis, and accurate reporting for precise emission management. Further, the proportional contribution of each country's CO2-equivalent HFC emissions has changed over tim","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"12 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452807","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10 揭示 PM10 氧化潜能源分配的最佳回归模型
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-26 DOI: 10.5194/acp-24-7261-2024
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, Gaëlle Uzu
{"title":"Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10","authors":"Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, Gaëlle Uzu","doi":"10.5194/acp-24-7261-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7261-2024","url":null,"abstract":"Abstract. The capacity of particulate matter (PM) to generate reactive oxygen species (ROS) in vivo leading to oxidative stress is thought to be a main pathway in the health effects of PM inhalation. Exogenous ROS from PM can be assessed by acellular oxidative potential (OP) measurements as a proxy of the induction of oxidative stress in the lungs. Here, we investigate the importance of OP apportionment methods for OP distribution by PM10 sources in different types of environments. PM10 sources derived from receptor models (e.g., EPA positive matrix factorization (EPA PMF)) are coupled with regression models expressing the associations between PM10 sources and PM10 OP measured by ascorbic acid (OPAA) and dithiothreitol assay (OPDTT). These relationships are compared for eight regression techniques: ordinary least squares, weighted least squares, positive least squares, Ridge, Lasso, generalized linear model, random forest, and multilayer perceptron. The models are evaluated on 1 year of PM10 samples and chemical analyses at each of six sites of different typologies in France to assess the possible impact of PM source variability on PM10 OP apportionment. PM10 source-specific OPDTT and OPAA and out-of-sample apportionment accuracy vary substantially by model, highlighting the importance of model selection according to the datasets. Recommendations for the selection of the most accurate model are provided, encompassing considerations such as multicollinearity and homoscedasticity.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"43 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452918","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Uncertainty in simulated brightness temperature due to sensitivity to atmospheric gas spectroscopic parameters from the centimeter- to submillimeter-wave range 厘米波至亚毫米波范围内大气气体光谱参数敏感性导致的模拟亮度温度的不确定性
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-26 DOI: 10.5194/acp-24-7283-2024
Donatello Gallucci, Domenico Cimini, Emma Turner, Stuart Fox, Philip W. Rosenkranz, Mikhail Y. Tretyakov, Vinia Mattioli, Salvatore Larosa, Filomena Romano
{"title":"Uncertainty in simulated brightness temperature due to sensitivity to atmospheric gas spectroscopic parameters from the centimeter- to submillimeter-wave range","authors":"Donatello Gallucci, Domenico Cimini, Emma Turner, Stuart Fox, Philip W. Rosenkranz, Mikhail Y. Tretyakov, Vinia Mattioli, Salvatore Larosa, Filomena Romano","doi":"10.5194/acp-24-7283-2024","DOIUrl":"https://doi.org/10.5194/acp-24-7283-2024","url":null,"abstract":"Abstract. Atmospheric radiative transfer models are extensively used in Earth observation to simulate radiative processes occurring in the atmosphere and to provide both upwelling and downwelling synthetic brightness temperatures for ground-based, airborne, and satellite radiometric sensors. For a meaningful comparison between simulated and observed radiances, it is crucial to characterize the uncertainty in such models. The purpose of this work is to quantify the uncertainty in radiative transfer models due to uncertainty in the associated spectroscopic parameters and to compute simulated brightness temperature uncertainties for millimeter- and submillimeter-wave channels of downward-looking satellite radiometric sensors (MicroWave Imager, MWI; Ice Cloud Imager, ICI; MicroWave Sounder, MWS; and Advanced Technology Microwave Sounder, ATMS) as well as upward-looking airborne radiometers (International Submillimetre Airborne Radiometer, ISMAR, and Microwave Airborne Radiometer Scanning System, MARSS). The approach adopted here is firstly to study the sensitivity of brightness temperature calculations to each spectroscopic parameter separately, then to identify the dominant parameters and investigate their uncertainty covariance, and finally to compute the total brightness temperature uncertainty due to the full uncertainty covariance matrix for the identified set of relevant spectroscopic parameters. The approach is applied to a recent version of the Millimeter-wave Propagation Model, taking into account water vapor, oxygen, and ozone spectroscopic parameters, though the approach is general and can be applied to any radiative transfer code. A set of 135 spectroscopic parameters were identified as dominant for the uncertainty in simulated brightness temperatures (26 for water vapor, 109 for oxygen, none for ozone). The uncertainty in simulated brightness temperatures is computed for six climatology conditions (ranging from sub-Arctic winter to tropical) and all instrument channels. Uncertainty is found to be up to few kelvins [K] in the millimeter-wave range, whereas it is considerably lower in the submillimeter-wave range (less than 1 K).","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"27 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere 对城市大气中可培养气载微生物的外代谢组学探索
IF 6.3 1区 地球科学
Atmospheric Chemistry and Physics Pub Date : 2024-06-25 DOI: 10.5194/egusphere-2024-1880
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, Pingqing Fu
{"title":"Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere","authors":"Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, Pingqing Fu","doi":"10.5194/egusphere-2024-1880","DOIUrl":"https://doi.org/10.5194/egusphere-2024-1880","url":null,"abstract":"<strong>Abstract.</strong> The interactions of metabolically active atmospheric microorganisms with cloud organic matter can alter the atmospheric carbon cycle. Upon deposition, atmospheric microorganisms can influence microbial communities in surface Earth systems. However, the metabolic activities of cultivable atmospheric microorganisms in settled habitats remain less understood. Here, we investigated exometabolites produced by typical bacterial and fungal species isolated from the urban atmosphere to elucidate their biogeochemical roles. Molecular compositions of exometabolites were analyzed using ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry. Annotation through the Kyoto Encyclopedia of Genes and Genomes database helped identify metabolic processes. Results showed that bacterial and fungal strains produce exometabolites with lower H/C and higher O/C ratios than consumed and resistant compounds. CHON compounds constituted over 50 % of the identified formulas of exometabolites. Bacterial exometabolites contained more abundant CHONS compounds (25.2 %), while fungal exometabolites were rich in CHO compounds (31.7 %). These microbial exometabolites predominantly comprised aliphatic/peptide-like and carboxyl-rich alicyclic molecules (CRAM-like). Significant variations in metabolites were observed among different strains. Bacteria showed a performance for amino acid synthesis, while fungi were more active in transcription and expression processes. Lipid metabolism, amino acid metabolism, and carbohydrate metabolism varied widely among bacterial strains, while fungi exhibited marked differences in carbohydrate metabolism and secondary metabolism. This comprehensive examination of metabolite characteristics at the molecular level for typical culturable airborne microorganisms enhances our understanding of their potential metabolic activities at air-land/water interfaces. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"27 1","pages":""},"PeriodicalIF":6.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141452863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","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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