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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 Q1 ENVIRONMENTAL SCIENCES 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
Abstract. 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 SOx 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-3, exhaust wet scrubbing already led to significant changes at concentrations of 100 cm-3. Additional simulations with cloud ice water path increased from ≈5.5 g m-2 to ≈9.3 g m-2, 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
摘要由于温室气体浓度增加和气候系统中的反馈过程,北极地区地表变暖,导致海冰范围和厚度持续下降。随着海冰的消退,未来航运活动很可能会在经济活动的推动下增加,而且通过更短的贸易航线可以节省时间和燃料。此外,在过去的十年中,全球航运业一直受到法规变化的影响,从而影响到废气颗粒的物理化学特性。旨在减少硫氧化物和微粒物质(PM)排放的国际法规要求船舶燃烧硫含量较低的燃料,或者在使用硫含量超过法规限制的燃料时使用湿式洗涤作为尾气后处理。合规措施会以不同的方式影响废气颗粒的物理化学特性及其云凝结核 (CCN) 活性,有可能对云的形成和寿命等大气过程产生直接和间接影响。鉴于北极环境相对原始,船舶废气颗粒排放可能会对北极气溶胶的自然基线浓度造成巨大干扰。低层平流混合相云覆盖了北极地区的大片区域,在区域能量预算中发挥着重要作用。实验室船用发动机测量的结果研究了降低燃料硫含量(FSC)和湿式洗涤对废气颗粒特性的影响,这促使我们使用大涡模拟来进一步研究这些颗粒如何影响在北极夏季云海研究活动中观测到的平流混合相云的微观和宏观物理特性。模拟的船舶废气颗粒增强主要影响了云的液相特性,导致液面降水减少、云反照率增加和长波表面增温。影响的大小在很大程度上取决于船舶废气颗粒的浓度、吸湿性和大小,其中颗粒大小的影响在吸湿性的影响中占主导地位。虽然在废气颗粒浓度为 1000 cm-3 时,观察到低 FSC 废气颗粒对云特性的影响最大,但在浓度为 100 cm-3 时,废气湿式洗涤已经导致了显著的变化。在将云冰水路径从≈5.5 g m-2 增加到≈9.3 g m-2 的其他模拟中,对船舶废气扰动的反应更加微弱,但发现根据云的微物理状态,废气扰动甚至可能导致轻微的辐射冷却效应。因此,航运活动对北极云特性的区域影响可能在很大程度上取决于船舶燃料类型、船舶是否使用湿式洗涤器以及决定主要云特性的环境热力学条件。
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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 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-27 DOI: 10.5194/acp-24-7385-2024
Flora Maria Brocza, Peter Rafaj, Robert Sander, Fabian Wagner, Jenny Marie Jones
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.
摘要人为排放到大气中的汞(Hg)是对人类和环境健康的长期危害。联合国《汞问题水俣公约》正寻求通过一系列政策,从禁止某些汞用途到减少不同活动中无意释放的汞,来降低人为汞排放。除了独立的汞政策外,减少温室气体、颗粒物(PM)和二氧化硫的战略也可以降低汞排放,从而带来共同利益。本研究利用温室气体-空气污染互动与协同作用(GAINS)模型,研究了不同的清洁空气和气候政策对未来全球汞排放的影响。基准情景假定了当前的能源使用和汞排放趋势,以及当前的清洁空气立法、汞政策和气候政策。此外,我们还探讨了《水俣公约》的影响、气候和严格空气污染政策的共同效益以及最大可行的汞减排措施。由于全球化石燃料和传统生物质使用量的减少,2050 年前的汞排放预测显示,所有情景下燃烧部门的汞排放都有明显减少,基线减排量为 33%,如果将严格的气候控制和最有效的汞控制结合起来,减排量可达 90%。在当前空气污染政策下,水泥和有色金属的排放量在所有情景下都会增加,但如果采取针对汞的严格措施,到 2050 年可分别减少 72% 和 46%。其他排放物(包括废弃物)是本研究中一个重要的不确定来源,根据气候和清洁空气政策的不同,其预测值在 2050 年增加 22% 到减少 54% 之间。汞减排的绝对潜力最大,但绝对排放量的不确定性也最大的领域是小规模和手工黄金生产,在这一领域,减排措施可消除 601-1371 吨(95% 置信区间)的汞年排放量,但估计值的不确定性非常高,可能会使所有其他领域的减排努力黯然失色。总的来说,90% 的汞排放都在《水俣公约》的规定范围内。总之,研究结果表明,除了严格的气候、可吸入颗粒物和二氧化硫政策外,还必须实施有针对性的汞控制政策,以实现汞排放的大幅减少。
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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 Q1 ENVIRONMENTAL SCIENCES 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
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.
摘要极端寒冷对人类社会影响巨大。了解主导极端寒冷变化的物理过程对于可靠预测未来气候变化至关重要。在过去几十年中,观测到的极端寒冷现象有所减少,在未来全球变暖的情况下,这一趋势仍将持续。在此,我们利用两套气候模式的大集合模拟,定量确定了过去几十年和未来温暖气候下动态效应(大尺度大气环流变化)和热力学效应(全球变暖导致气温升高)对东亚极端寒冷的贡献。我们的研究表明,在过去 50 年中,动态成分占寒冷月份(北方冬季最冷的 5%月份)地表气温异常的 80% 以上。然而,在未来的暖气候中,热力学变化是导致东亚极端寒冷强度和发生概率下降的主要原因,而动力学变化也是原因之一。21 世纪末,东亚极端寒冷强度将下降约 5 °C,其中热动力(动态)变化的贡献率约为 75%(25%)。目前(1986-2005 年)的东亚极端寒冷天气在 2035 年左右之后几乎不会再出现,而这将在 10 年之后发生,原因完全在于热动力变化。类似北极涛动的正向海平面压力模式的上升趋势主导了动态成分的变化。这一发现为决策者开展气候变化适应活动提供了有益的参考。
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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 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-26 DOI: 10.5194/egusphere-2024-1848
Feng Jiang, Harald Saathoff, Junwei Song, Hengheng Zhang, Linyu Gao, Thomas Leisner
Abstract. 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 17th February to 16th 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−3, and 31 potential BrC (including 4 NACs) molecules were identified in the gas phase contributing on average 6.2 ± 5.0 ng m−3 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 (MAC370) of 9.5 m2 g−1. 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.
摘要棕碳气溶胶(BrC)是造成欧洲大气污染的主要因素之一,尤其是在冬季。因此,我们于 2 月 17 日至 3 月 16 日在德国西南部的一个农村地区研究了褐碳气溶胶的化学成分、昼夜变化和来源。在整个研究过程中,我们总共在颗粒相中发现了 178 个潜在的溴化碳分子(包括 7 个硝基芳香族化合物),平均含量为 63 ± 32 纳克/立方米;在气相中发现了 31 个潜在的溴化碳分子(包括 4 个硝基芳香族化合物),平均含量为 6.2 ± 5.0 纳克/立方米。这 178 个潜在的 BrC 分子仅占有机物总质量的 2.3 ± 1.5%,但可以解释 370 纳米波长处 BrC 吸收总量的 11 ± 11%(假设 370 纳米波长处的平均质量吸收系数 (MAC370) 为 9.5 m2 g-1)。少数 BrC 分子主导了 BrC 的总吸收。此外,昼夜变化表明气相 BrC 在白天较高,而在夜间较低。它主要受二次形成(如光氧化)和颗粒与气体之间的分配控制。相应地,颗粒相的 BrC 在白天较低,在夜间较高。二次形成在颗粒相 BrC 中占主导地位,为 61 ± 21%,而 39 ± 21% 来自生物质燃烧。此外,由于光化学老化,颗粒相 BrC 的光吸收率不断下降。这项研究扩展了目前对欧洲中部某地气相和颗粒相褐碳气溶胶实时行为的了解。
{"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 Q1 ENVIRONMENTAL SCIENCES 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
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
摘要氢氟碳化物(HFCs)是一种强大的人为温室气体(GHGs),具有很高的全球升温潜能值(GWPs)。它们被广泛用作制冷剂、绝缘泡沫发泡剂、气溶胶推进剂和灭火剂。自 20 世纪 90 年代中期以来,HFCs 的排放量迅速增加,因为在许多应用中,HFCs 被用来替代消耗臭氧层的氯氟化碳(CFCs)和氯氟烃(HCFCs),而根据《蒙特利尔议定书》(MP),氯氟化碳和氯氟烃的消费和生产已被淘汰。由于氢氟碳化物的全球升温潜能值较高,《蒙特利尔议定书》的《基加利修正案》要求逐步减少氢氟碳化物的生产和消费,到 2047 年实现 80%-85% 的减排量,非第 5 条国家(发达国家)从 2019 年开始,在每个确定的基准线上减少 10%,第 5 条国家(发展中国家)的时间表则要晚一些。在本研究中,我们研究了 2008 年至 2020 年期间在韩国济州岛高山站对大气中五种主要 HFCs(HFC-134a、HFC-143a、HFC-32、HFC-125 和 HFC-152a)丰度的长期高精度测量结果。在整个期间,HFCs 的本底丰度逐渐升高,并检测到来自周围污染源区域的污染气团丰度升高。根据这些污染事件,我们利用两个独立的拉格朗日粒子扩散模型和贝叶斯反演框架(FLEXPART-FLEXINVERT+ 和 NAME-InTEM)推断出了区域和国家特定的 HFC 排放估计值。得出的所有 HFCs 的 "自上而下"(基于测量)排放量的空间分布显示,该地区的大城市和工业区有大量 HFCs 排放。我们最重要的发现是,从 2016 年到 2018 年,中国东部和日本的 HFC 排放量急剧增加。东亚 HFC 排放量占全球总量的比例从 9%(2008-2014 年)增至 13%(2016-2020 年)。特别是日本(附件一国家)的 HFC 排放量从 2016 年起迅速上升,累计推断的 HFC 排放总量为 1.14 亿吨/年,比向《联合国气候变化框架公约》(UNFCCC)报告的 "自下而上"(即基于活动数据和排放因子)排放量 3.8 亿吨/年高出 7.6 亿吨/年。这可能与日本国内对制冷剂和空调系统相关产品的需求增加以及核算不完整有关。HFC 排放量从 2019 年开始呈下降趋势,这反映了日本含氟温室气体政策的有效性。中国东部和韩国虽然没有义务向《联合国气候变化框架公约》报告,但自愿报告了排放量,这也显示了自上而下和自下而上的排放量估算之间的差异,表明需要进行大气测量、全面的数据分析和准确的报告,以实现精确的排放管理。此外,随着时间的推移,各国二氧化碳当量 HFC 排放量的比例也发生了变化,HFC-134a 在减少,而 HFC-125 在增加。这表明各国导致全球变暖的主要 HFC 物质发生了转变。
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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 Q1 ENVIRONMENTAL SCIENCES 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
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.
摘要颗粒物(PM)在体内产生活性氧(ROS)导致氧化应激的能力被认为是吸入颗粒物影响健康的主要途径。可吸入颗粒物产生的外源性 ROS 可通过细胞氧化电位(OP)测量来评估,以此作为肺部氧化应激诱导的替代物。在这里,我们研究了不同类型环境中 PM10 来源的 OP 分布的 OP 分摊方法的重要性。从受体模型(如 EPA 正矩阵因式分解(EPA PMF))得出的 PM10 来源与表达 PM10 来源与通过抗坏血酸(OPAA)和二硫苏糖醇测定法(OPDTT)测量的 PM10 OP 之间关系的回归模型相结合。这些关系通过八种回归技术进行了比较:普通最小二乘法、加权最小二乘法、正最小二乘法、Ridge、Lasso、广义线性模型、随机森林和多层感知器。这些模型对法国六个不同类型地点的一年 PM10 样品和化学分析进行了评估,以评估 PM10 源变异性对 PM10 OP 分配可能产生的影响。不同模型的PM10特定源OPDTT和OPAA以及样本外分摊的准确性差异很大,这突出了根据数据集选择模型的重要性。提供了选择最准确模型的建议,包括多共线性和同方差等考虑因素。
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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 Q1 ENVIRONMENTAL SCIENCES 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
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).
摘要。大气辐射传输模型被广泛用于地球观测,以模拟大气中发生的辐射过程,并为地基、机载和卫星辐射测量传感器提供上涌和下沉合成亮度温度。要对模拟辐射和观测辐射进行有意义的比较,就必须确定这些模型的不确定性。这项工作的目的是量化由于相关光谱参数的不确定性而导致的辐射传递模型的不确定性,并计算下视卫星辐射测量传感器毫米波和亚毫米波通道(微波成像仪,MWI;冰云成像仪(ICI)、微波探测仪(MWS)和先进技术微波探测仪(ATMS))以及上视机载辐射计(国际亚毫米波机载辐射计(ISMAR)和微波机载辐射计扫描系统(MARSS))。这里采用的方法首先是分别研究亮度温度计算对每个光谱参数的敏感性,然后确定主要参数并研究它们的不确定性协方差,最后计算由于已确定的相关光谱参数集的全不确定性协方差矩阵而产生的总亮度温度不确定性。该方法应用于最新版本的毫米波传播模型,考虑到了水蒸气、氧气和臭氧光谱参数,但该方法具有通用性,可应用于任何辐射传递代码。一组 135 个光谱参数被确定为模拟亮度温度不确定性的主要因素(水蒸气 26 个,氧气 109 个,臭氧 0 个)。计算了六种气候条件(从亚北极冬季到热带)和所有仪器通道下模拟亮度温度的不确定性。发现毫米波范围内的不确定性高达几开尔文[K],而亚毫米波范围内的不确定性要低得多(小于 1 K)。
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引用次数: 0
Impact of Asian aerosols on the summer monsoon strongly modulated by regional precipitation biases 亚洲气溶胶对夏季季风的影响受区域降水偏差的强烈调节
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-25 DOI: 10.5194/acp-24-7227-2024
Zhen Liu, Massimo A. Bollasina, Laura J. Wilcox
Abstract. Reliable attribution of Asian summer monsoon variations to aerosol forcing is critical to reducing uncertainties in future projections of regional water availability, which is of utmost importance for risk management and adaptation planning in this densely populated region. Yet, simulating the monsoon remains a challenge for climate models that suffer from long-standing biases, undermining their reliability in attributing anthropogenically forced changes. We analyze a suite of climate model experiments to identify a link between model biases and monsoon responses to Asian aerosols and associated physical mechanisms, including the role of large-scale circulation changes. The aerosol impact on monsoon precipitation and circulation is strongly influenced by a model's ability to simulate the spatio-temporal variability in the climatological monsoon winds, clouds, and precipitation across Asia, which modulates the magnitude and efficacy of aerosol–cloud–precipitation interactions, an important component of the total aerosol response. There is a strong interplay between South Asia and East Asia monsoon precipitation biases and their relative predominance in driving the overall monsoon response. We found a striking contrast between the early- and late-summer aerosol-driven changes ascribable to opposite signs and seasonal evolution of the biases in the two regions. A realistic simulation of the evolution of the large-scale atmospheric circulation is crucial to realize the full extent of the aerosol impact over Asia. These findings provide important implications for better understanding and constraining the diversity and inconsistencies of model responses to aerosol changes over Asia in historical simulations and future projections.
摘要。将亚洲夏季季风的变化可靠地归因于气溶胶的作用,对于减少未来区域水供应预测的不确定性至关重要,而这对这一人口稠密地区的风险管理和适应规划至关重要。然而,模拟季风对于气候模型来说仍然是一个挑战,因为气候模型长期以来存在偏差,这削弱了它们归因于人为强迫变化的可靠性。我们分析了一系列气候模式实验,以确定模式偏差与季风对亚洲气溶胶的响应及相关物理机制之间的联系,包括大尺度环流变化的作用。气溶胶对季风降水和环流的影响深受模型模拟亚洲各地气候学季风风、云和降水时空变化能力的影响,这种能力会调节气溶胶-云-降水相互作用的程度和效果,而这是气溶胶总响应的一个重要组成部分。南亚和东亚季风降水偏差及其在驱动整体季风响应中的相对主导地位之间存在着强烈的相互作用。我们发现,气溶胶驱动的初夏和夏末变化之间形成了鲜明对比,这是因为这两个地区的偏差具有相反的符号和季节演变。大尺度大气环流演变的真实模拟对于全面了解气溶胶对亚洲的影响至关重要。这些发现对更好地理解和制约历史模拟和未来预测中模式对亚洲上空气溶胶变化的反应的多样性和不一致性具有重要意义。
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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 Q1 ENVIRONMENTAL SCIENCES 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
Abstract. 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.
摘要代谢活跃的大气微生物与云层有机物的相互作用可改变大气碳循环。大气微生物在沉积后会影响地球表面系统中的微生物群落。然而,人们对定居栖息地中可培养的大气微生物的代谢活动仍然知之甚少。在这里,我们研究了从城市大气中分离出来的典型细菌和真菌物种产生的外代谢产物,以阐明它们的生物地球化学作用。我们使用超高分辨率傅立叶变换离子回旋共振质谱分析了外代谢物的分子组成。通过京都基因和基因组百科全书数据库进行注释,有助于确定代谢过程。结果表明,细菌和真菌菌株产生的外代谢物与消耗性和抗性化合物相比,H/C 比值较低,O/C 比值较高。在已鉴定的外代谢物配方中,CHON化合物占了50%以上。细菌外代谢物含有更多的 CHONS 化合物(25.2%),而真菌外代谢物则富含 CHO 化合物(31.7%)。这些微生物外代谢物主要包括脂肪族/肽类和富含羧基的脂环族分子(CRAM-like)。不同菌株的代谢物存在显著差异。细菌在氨基酸合成方面表现突出,而真菌在转录和表达过程中更为活跃。细菌菌株之间的脂质代谢、氨基酸代谢和碳水化合物代谢差异很大,而真菌在碳水化合物代谢和次级代谢方面表现出明显差异。对典型的可培养空气传播微生物的代谢物特征进行分子水平的全面研究,加深了我们对它们在空气-陆地-水界面的潜在代谢活动的了解。这些见解对于评估大气微生物沉积后的生物地球化学影响至关重要。
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引用次数: 0
Unheralded contributions of biogenic volatile organic compounds from urban greening to ozone pollution: a high-resolution modeling study 城市绿化产生的生物挥发性有机化合物对臭氧污染的贡献未被察觉:一项高分辨率模型研究
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-06-25 DOI: 10.5194/egusphere-2024-1163
Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Tianhang Zhang, Chong Shen
Abstract. Urban Green Spaces (UGS) are widely advocated for mitigating urban atmospheric environment. However, this study reveals that it can exacerbate urban ozone (O3) levels under certain conditions, as demonstrated by a September 2017 study in Guangzhou, China. Utilizing the Weather Research and Forecasting Model with the Model of Emissions of Gases and Aerosols from Nature (WRF-MEGAN) and the Community Multiscale Air Quality (CMAQ) model with a high horizontal resolution (1 km), we assessed the impact of UGS-related biogenic volatile organic compound (BVOC) emissions on urban O3. Our findings indicate that UGS-BVOC emissions in Guangzhou amounted to 666.49 Gg, primarily from isoprene (ISOP) and terpenes (TERP). These emissions contribute ~30 % of urban ISOP concentrations and their incorporations to the model significantly reduce the underestimation against observations. The study shows improvements in simulation biases for NO2, from 7.01 µg/m3 to 6.03 µg/m3, and for O3, from 7.77 µg/m3 to -1.60 µg/m3. UGS-BVOC and UGS-LUCC (land use cover changes) integration in air quality models notably enhances surface monthly mean O3 predictions by 3.6–8.0 µg/m3 (+3.8–8.5 %) and contributes up to 18.7 µg/m3 (+10.0 %) to MDA8 O3 during O3 pollution episodes. Additionally, UGS-BVOC emissions alone increase the monthly mean O3 levels by 2.2–3.0 µg/m3 (+2.3–3.2 %) in urban areas and contribute up to 6.3 µg/m3 (+3.3 %) to MDA8 O3 levels during O3 pollution episodes. These impacts can extend to surrounding suburban and rural areas through regional transport, highlighting the need for selecting low-emission vegetation and refining vegetation classification in urban planning.
摘要城市绿地(UGS)被广泛提倡用于缓解城市大气环境。然而,本研究发现,在某些条件下,城市绿地会加剧城市臭氧(O3)水平,2017 年 9 月在中国广州进行的一项研究就证明了这一点。利用气象研究和预报模型与自然界气体和气溶胶排放模型(WRF-MEGAN)以及高水平分辨率(1 千米)的社区多尺度空气质量(CMAQ)模型,我们评估了与 UGS 相关的生物挥发性有机化合物(BVOC)排放对城市臭氧(O3)的影响。研究结果表明,广州的 UGS-BVOC 排放量为 666.49 千兆克,主要来自异戊二烯(ISOP)和萜烯(TERP)。这些排放物占城市 ISOP 浓度的约 30%,将其纳入模型可显著减少对观测数据的低估。研究显示,二氧化氮的模拟偏差从 7.01 µg/m3 降至 6.03 µg/m3,臭氧的模拟偏差从 7.77 µg/m3 降至 -1.60 µg/m3。将 UGS-BVOC 和 UGS-LUCC(土地利用覆盖变化)集成到空气质量模型中,可显著提高地表月平均 O3 预测值 3.6-8.0 µg/m3 (+3.8-8.5 %),并在 O3 污染事件期间对 MDA8 O3 的贡献高达 18.7 µg/m3 (+10.0 %)。此外,仅 UGS-BVOC 排放就会使城市地区的月平均 O3 水平增加 2.2-3.0 µg/m3 (+2.3-3.2 %),并在 O3 污染事件期间使 MDA8 的 O3 水平增加高达 6.3 µg/m3 (+3.3 %)。这些影响可通过区域运输扩展到周围的郊区和农村地区,这突出表明了在城市规划中选择低排放植被和完善植被分类的必要性。
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引用次数: 0
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Atmospheric Chemistry and Physics
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