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Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model 基于多阶段模型的 2000-2100 年全球环境活性氮成分估计值
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/acp-24-7623-2024
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, Gehui Wang
Abstract. High contents of reactive nitrogen components aggravate air pollution and could also impact ecosystem structures and functioning across the terrestrial–aquatic–marine continuum. However, the long-term historical trends and future predictions of reactive nitrogen components at the global scale still remain highly uncertain. In our study, field observations, satellite products, model outputs, and many other covariates were integrated into the multi-stage machine-learning model to capture the global patterns of reactive nitrogen components during 2000–2019. In order to decrease the estimate uncertainties in the future scenarios, the constructed reactive nitrogen component dataset for the historical period was utilised as the constraint to calibrate the CMIP6 dataset in four scenarios. The results suggested that the cross-validation (CV) R2 values of four species showed satisfying performance (R2>0.55). The concentrations of estimated reactive nitrogen components in China experienced persistent increases during 2000–2013, while they suffered drastic decreases from 2013, except for NH3. This might be associated with the impact of clean-air policies. However, in Europe and the United States, these compounds have remained relatively stable since 2000. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations, respectively. Although the reactive nitrogen concentrations in some heavy-pollution scenarios (SSP3-7.0) also experienced decreases during 2020–2100, SSP1-2.6 and SSP2-4.5 (middle-emission scenario) still showed more rapidly decreasing trends. Our results emphasise the need for carbon neutrality pathways to reduce global atmospheric N pollution.
摘要高含量的活性氮成分会加剧空气污染,也会影响陆地-水生-海洋连续体的生态系统结构和功能。然而,全球范围内活性氮成分的长期历史趋势和未来预测仍存在很大的不确定性。在我们的研究中,实地观测、卫星产品、模型输出和许多其他协变量被整合到多阶段机器学习模型中,以捕捉 2000-2019 年间全球活性氮组分的模式。为了降低未来情景的估计不确定性,利用构建的历史时期活性氮组分数据集作为约束条件,对 CMIP6 数据集进行了四种情景的校准。结果表明,四个物种的交叉验证(CV)R2 值表现令人满意(R2>0.55)。2000-2013年期间,中国估计的活性氮组分浓度持续上升,而从2013年开始,除NH3外,其他组分浓度急剧下降。这可能与清洁空气政策的影响有关。然而,在欧洲和美国,这些化合物自 2000 年以来一直保持相对稳定。在未来情景中,SSP3-7.0(传统能源情景)和 SSP1-2.6(碳中和情景)分别显示出最高和最低的活性氮成分浓度。虽然一些重污染情景(SSP3-7.0)中的活性氮浓度在 2020-2100 年期间也出现了下降,但 SSP1-2.6 和 SSP2-4.5(中等排放情景)仍然呈现出更快的下降趋势。我们的研究结果强调了减少全球大气氮污染的碳中和途径的必要性。
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引用次数: 0
The marinada fall wind in the eastern Ebro sub-basin: physical mechanisms and role of the sea, orography and irrigation 埃布罗河流域东部的海洋秋风:物理机制以及海洋、地形和灌溉的作用
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/acp-24-7637-2024
Tanguy Lunel, Maria Antonia Jimenez, Joan Cuxart, Daniel Martinez-Villagrasa, Aaron Boone, Patrick Le Moigne
Abstract. During the warm months of the year in Catalonia, the marine air overcomes the coastal mountain range and reaches the eastern Ebro sub-basin. This phenomenon is called marinada and has recently been thoroughly characterized for the first time by Jiménez et al. (2023), based on surface climatological data. However, the main physical mechanisms involved in its arrival and propagation remain to be discovered. This study aims to understand how the marinada is formed and how it interacts with the already developed atmospheric boundary layer. Surface and atmospheric observations are used in combination with the coupled surface–atmosphere model Meso-NH to reveal the mechanisms at play. It is shown that the marinada is generated by the advection of a cool marine air mass over the Catalan Pre-coastal Range by the action of the sea breeze and the upslope wind. This marine air mass then flows into the Ebro basin, creating what is known as the marinada. The characteristics and dynamics of the marinada allow it to be classified as a fall wind. It is also shown that the arrival, propagation and decay of the marinada is strongly dependent on the larger-scale weather situation: westerlies or thermal low. The current study provides a consistent framework for understanding the marinada, paving the way for better modeling and prediction of the phenomenon.
摘要在加泰罗尼亚一年中温暖的月份里,海洋空气会越过沿海山脉,到达埃布罗河流域东部。这种现象被称为 "海洋气流"(marinada),Jiménez 等人(2023 年)最近首次根据地表气候数据对其进行了全面描述。然而,其到达和传播所涉及的主要物理机制仍有待发现。本研究旨在了解海洋气旋是如何形成的,以及它是如何与已经形成的大气边界层相互作用的。地面和大气观测结果与地面-大气耦合模型 Meso-NH 结合使用,揭示了其中的作用机制。研究表明,在海风和上坡风的作用下,加泰罗尼亚前海岸山脉上空的冷海洋气团平流产生了海洋气团。海洋气团随后流入埃布罗河盆地,形成所谓的海洋气流。根据 Marinada 的特征和动态,可以将其归类为秋风。研究还表明,海洋风的到达、传播和衰减与大尺度天气形势(西风或热低压)密切相关。目前的研究为理解马林纳达提供了一个一致的框架,为更好地模拟和预测该现象铺平了道路。
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引用次数: 0
How atmospheric CO2 can inform us on annual and decadal shifts in the biospheric carbon uptake period 大气中的二氧化碳如何让我们了解生物圈碳吸收期的年度和十年期变化
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/egusphere-2024-1382
Theertha Kariyathan, Ana Bastos, Markus Reichstein, Wouter Peters, Julia Marshall
Abstract. The carbon uptake period (CUP) refers to the time of each year during which the rate of photosynthetic uptake surpasses that of respiration in the terrestrial biosphere, resulting in a net absorption of CO2 from the atmosphere to the land. Since climate drivers influence both photosynthesis and respiration, the CUP offers valuable insights into how the terrestrial biosphere responds to climate variations and affects the carbon budget. Several studies have assessed large-scale changes in CUP based on seasonal metrics from CO2 mole fraction measurements. However, an in-depth understanding of the sensitivity of the CUP as derived from the CO2 mole fraction data (CUPMR) to actual changes in the CUP of the net ecosystem exchange (CUPNEE) is missing. In this study, we specifically assess the impact of (i) atmospheric transport (ii) inter-annual variability in CUPNEE (iii) regional contribution to the signals that integrate at different background sites where CO2 dry air mole fraction measurements are made. We conducted idealized simulations where we imposed known changes (∆) to the CUPNEE in the Northern Hemisphere to test the effect of the aforementioned factors in CUPMR metrics at ten Northern Hemisphere sites. Our analysis indicates a significant damping of changes in the simulated ∆CUPMR due to the integration of signals with varying CUPNEE timing across regions. CUPMR at well-studied sites such as Mauna Loa, Barrow, and Alert showed only 50 % of the applied ∆CUPNEE under non interannually-varying atmospheric transport conditions. Further, our synthetic analyses conclude that interannual variability (IAV) in atmospheric transport accounts for a significant part of the changes in the observed signals. However, even after separating the contribution of transport IAV, the estimates of surface changes in CUP by previous studies are not likely to provide an accurate magnitude of the actual changes occurring over the surface. The observed signal experiences significant damping as the atmosphere averages out non-synchronous signals from various regions.
摘要碳吸收期(CUP)是指每年陆地生物圈中光合作用吸收速率超过呼吸作用吸收速率,从而导致陆地从大气中净吸收二氧化碳的时间。由于气候驱动因素对光合作用和呼吸作用都有影响,因此陆地生物圈如何对气候变异做出反应并影响碳收支,陆地碳收支提供了宝贵的见解。有几项研究根据二氧化碳摩尔分数测量值的季节性指标评估了CUP的大规模变化。然而,我们还没有深入了解二氧化碳摩尔分数数据(CUPMR)得出的生态系统净交换量(CUPNEE)对生态系统碳平衡实际变化的敏感性。在本研究中,我们特别评估了以下因素的影响:(i)大气传输;(ii)CUPNEE 的年际变化;(iii)区域因素对在二氧化碳干空气摩尔分数测量的不同背景站点整合信号的影响。我们进行了理想化模拟,对北半球的 CUPNEE 施加了已知变化(∆),以测试上述因素对北半球十个站点的 CUPMR 指标的影响。我们的分析表明,由于不同地区的 CUPNEE 时间信号的整合,模拟 ∆CUPMR 的变化受到了明显的抑制。在非年际变化的大气传输条件下,莫纳洛亚、巴罗和阿勒特等研究充分的站点的 CUPMR 仅为应用 ∆CUPNEE 的 50%。此外,我们的合成分析得出结论,大气传输的年际变化(IAV)占观测信号变化的很大一部分。然而,即使在分离了大气传输年际变率的贡献之后,以往研究对 CUP 表面变化的估计也不可能提供表面实际变化的准确量级。由于大气层会平均掉来自不同区域的非同步信号,因此观测到的信号会出现明显的阻尼。
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引用次数: 0
Measurement Report: Changes of ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice core record 测量报告:从厄尔布鲁士(俄罗斯高加索)冰芯记录推断东南欧 18 世纪以来氨排放的变化
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/egusphere-2024-1381
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, Susanne Preunkert
Abstract. To investigate the historical levels of atmospheric ammonia (NH3) pollution in south-eastern Europe, a 182 m long ice core was extracted from Mount Elbrus in the Caucasus, Russia. This ice core contains a record of ammonium (NH4+) levels from ~1750 CE (Common Era) to 2009 CE. The NH4+ ice core record indicates a 3.5-fold increase of annual concentrations from 34 ± 7 ng g-1 (~1750–1830) to 117 ± 23 ng g-1 over the recent decades (1980–2009). The increase remained moderate until 1950 CE (mean concentration of 49 ± 14 ng g-1 over the 1830–1950 period), and then accelerated to reach a maximum close to 120 ng g-1 in 1989. This ice core trend is compared to estimated past anthropogenic NH3 emissions in Europe by using state-of-the-art atmospheric transport modeling of submicron aerosols (FLEXPART model driven with 0.5° x 0.5° ERA5 reanalysis data). It is shown that in summer, when both vertical atmospheric mixing and agricultural NH3 emissions are strengthened, the NH4+ ice core trend is in good agreement with the course of estimated NH3 emissions from south-eastern Europe since ~1750 with a main contribution from south European Russia, Turkey, Georgia, and Ukraine. Examination of Mount Elbrus ice deposited over the second half of the 18th century when agricultural activities were less than 10% of those during the 1990s, suggest a pre-1750 annual NH4+ ice concentration related to natural emissions of 25 ng g-1. This pre-1750 natural level mainly related to natural soil emissions represents ~20% of the 1980–2009 NH4+ level, a level mainly related to current agricultural emissions that almost completely outweigh biogenic emissions from natural soils.
摘要为了研究欧洲东南部大气氨(NH3)污染的历史水平,从俄罗斯高加索地区的厄尔布鲁士山提取了 182 米长的冰芯。该冰芯包含公元前约 1750 年(公元纪年)至公元 2009 年期间的氨(NH4+)水平记录。NH4+ 冰芯记录表明,在最近几十年(1980-2009 年),年浓度从 34 ± 7 纳克/克-1(约 1750-1830 年)增加到 117 ± 23 纳克/克-1,增加了 3.5 倍。在西元 1950 年之前,上升幅度一直不大(1830-1950 年期间的平均浓度为 49 ± 14 纳克 g-1),随后加速上升,1989 年达到最大值,接近 120 纳克 g-1。通过使用最先进的亚微米气溶胶大气传输模型(使用 0.5° x 0.5° ERA5 再分析数据驱动的 FLEXPART 模型),将这一冰芯趋势与欧洲过去的人为 NH3 排放量估计值进行了比较。结果表明,在垂直大气混合和农业 NH3 排放都加强的夏季,NH4+ 冰芯趋势与欧洲东南部自约 1750 年以来的 NH3 估计排放过程非常一致,主要来自欧洲南部的俄罗斯、土耳其、格鲁吉亚和乌克兰。对 18 世纪下半叶沉积的厄尔布鲁士山冰层进行的研究表明,1750 年前与自然排放相关的 NH4+ 冰层年浓度为 25 纳克 g-1。这一 1750 年前的自然水平主要与自然土壤排放有关,约占 1980-2009 年 NH4+ 水平的 20%,而这一水平主要与当前的农业排放有关,农业排放几乎完全超过了自然土壤的生物排放。
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引用次数: 0
Measurement report: Size-resolved secondary organic aerosol formation modulated by aerosol water uptake in wintertime haze 测量报告:粒度分辨的二次有机气溶胶形成受冬季雾霾中气溶胶吸水的影响
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/acp-24-7687-2024
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, Colin O'Dowd
Abstract. This study investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, on secondary organic aerosol (SOA) formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi'an, northwestern China. The composition of inorganic aerosol showed significant changes in winter 2018–2019 compared to winter 2013–2014, shifting from a sulfate-rich profile to a nitrate-rich profile. In particular, the fraction of sulfate and chloride decreased, but that of nitrate increased in the entire size range, while ammonium mainly increased at larger particle sizes. These changes thus resulted in a size-dependent evolution in water uptake. Increased water uptake was observed in most cases, mainly associated with enhanced contributions of both nitrate and ammonium, with the highest increase ratio reaching 5 %–35 % at larger particle sizes and higher relative humidity (RH>70 %). The non-negligible influence of chloride on aerosol water uptake was also emphasized. The random forest analysis coupled with a Shapley additive explanation algorithm (SHAP) further showed an enhanced relative importance of aerosol water in impacting SOA formation. Aerosol water exhibited a significant contribution to SOA formation during winter 2018–2019, particularly at larger particle sizes. The SHAP value of aerosol water increased alongside higher levels of aerosol water, indicating an enhanced contribution of aerosol water to SOA formation. This implies that the majority of enhanced aerosol water uptake at larger particle sizes and high RH might facilitate the efficient aqueous-phase SOA formation. This study highlights the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes. As challenges to further improve China's air quality remain and because SOA plays an increasing role in haze pollution, these results provide insight into the size-resolved evolution characteristics and offer guidance for future controls.
摘要本研究基于对中国西北部西安市非难降解细颗粒物(NR-PM2.5)的粒径分辨测量,研究了无机物变化对气溶胶吸水的潜在影响,进而研究了冬季灰霾天气中二次有机气溶胶(SOA)形成的潜在影响。与2013-2014年冬季相比,2018-2019年冬季无机气溶胶的组成发生了显著变化,从富含硫酸盐的剖面转变为富含硝酸盐的剖面。其中,硫酸盐和氯化物的比例有所下降,但硝酸盐的比例在整个粒径范围内均有所上升,而铵主要在粒径较大时有所增加。因此,这些变化导致了摄水量随粒径而变化。在大多数情况下都能观察到吸水量的增加,这主要与硝酸盐和铵的增加有关,在粒径较大和相对湿度较高(相对湿度>70%)的情况下,吸水量增加比率最高,达到 5%-35%。氯化物对气溶胶吸水的影响也不容忽视。随机森林分析与沙普利加法解释算法(SHAP)相结合,进一步显示了气溶胶水在影响 SOA 形成方面的相对重要性。在2018-2019年冬季,气溶胶水对SOA的形成有显著贡献,尤其是在粒径较大的情况下。气溶胶水的SHAP值随着气溶胶水含量的增加而增加,表明气溶胶水对SOA形成的贡献增强。这意味着在粒径较大和相对湿度较高的情况下,气溶胶吸水的大部分增强可能会促进水相 SOA 的有效形成。这项研究强调了气溶胶水作为介质在无机物和有机物的多相过程中的关键作用。由于进一步改善中国空气质量的挑战依然存在,而且SOA在灰霾污染中扮演着越来越重要的角色,这些结果提供了对粒径分辨演变特征的深入了解,并为未来的控制提供了指导。
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引用次数: 0
Impact of wildfire smoke on Arctic cirrus formation, part 1: analysis of MOSAiC 2019–2020 observations 野火烟雾对北极卷云形成的影响,第 1 部分:MOSAiC 2019-2020 年观测分析
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/egusphere-2024-2008
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, Ulla Wandinger
Abstract. The number of wildfire smoke layers in the upper troposphere per fire season increased at mid and high northern latitudes during the last years. To consider smoke in weather and climate models appropriately, the influence of smoke on a variety of atmospheric processes needs to be explored in detail. In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. The complex study is based on aerosol and ice cloud observations in the central Arctic during the one-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition. For almost a year (from the summer of 2019 to the spring of 2020), aged Siberian wildfire smoke polluted the tropopause region over the central Arctic and many cirrus systems developed in the polluted upper troposphere. Goal of the data analysis (part 1) is to provide observational evidence for a dominating impact of aged wildfire smoke (organic aerosol particles) on cirrus formation in the central Arctic (over the MOSAiC research icebreaker Polarstern) during the winter half year of 2019–2020. Aim of the simulations in part 2 is to gain a deeper and more detailed insight into the potential smoke impact on ice nucleation as a function of observed aerosol and meteorological conditions (temperature, relative humidity) and by considering realistic gravity wave characteristics (updraft speed, wave amplitude). Vertical movements of air parcels are essential to initiate cloud formation. The measurements presented in part 1 were conducted during the winter half year (October to March), aboard the ice breaker Polarstern. The research vessel Polarstern drifted with the pack ice in the central Arctic mainly at latitudes >85 °N during the winter half year. The cirrus statistics show typical properties of ice clouds of the synoptic cirrus category (top-down generation of cirrus structures). The ice clouds mostly started to evolve at heights close to the tropopause. Cirrus top temperatures accumulated between −60 and −75 °C. The cirrus optical thickness (COT at 532 nm) of the ice clouds covered a wide range of values from < 0.03 (subvisible cirrus fraction, 25 % out of all cases) over 0.03–0.3 (visible thin cirrus, 40 %) to > 0.3 (opaque cirrus fraction, 35 %). In about 30 % out of all high altitude lidar observations, cirrus signatures were detected, much more than expected (10 %). This fact may be taken as a first hint that wildfire smoke was significantly involved in Arctic cirrus formation. The smoke particle surface area concentration around the tropopause was of the order of 5–15 µm2 cm−3 and indicated considerably enhanced levels of aerosol pollutio
摘要在过去几年中,北纬中高纬度地区每个火灾季节对流层上层的野火烟雾层数量有所增加。为了在天气和气候模式中适当考虑烟雾,需要详细探讨烟雾对各种大气过程的影响。在本研究中,我们重点关注野火烟雾对卷云形成的潜在影响。在两篇系列文章的第一部分中,我们首次将利用激光雷达和雷达进行的最先进的气溶胶和卷云观测与第二部分中卷云演变过程中重力波诱导冰核形成的综合建模紧密联系起来。这项复杂的研究以为期一年的北极气候研究多学科漂流观测站(MOSAiC)考察期间在北极中部进行的气溶胶和冰云观测为基础。在将近一年的时间里(从 2019 年夏季到 2020 年春季),西伯利亚野火的高龄烟雾污染了北极中部上空的对流层顶区域,许多卷云系统在受污染的对流层上部形成。数据分析(第 1 部分)的目标是提供观测证据,证明老化野火烟雾(有机气溶胶颗粒)对 2019-2020 年冬半年期间北极中部(MOSAiC 研究破冰船 Polarstern 上空)卷云形成的主要影响。第 2 部分模拟的目的是通过观测气溶胶和气象条件(温度、相对湿度),并考虑现实重力波特征(上升气流速度、波幅),更深入、更详细地了解烟雾对冰核形成的潜在影响。气团的垂直运动对于云的形成至关重要。第 1 部分介绍的测量是在冬半年(10 月至次年 3 月)在 Polarstern 号破冰船上进行的。在这半年的冬季,Polarstern 号科考船主要在北纬 85 度的北极中部随冰群漂流。卷云统计数据显示了同步卷云类冰云的典型特性(卷云结构自上而下生成)。冰云大多在接近对流层顶的高度开始演变。卷云顶部温度累积在 -60 至 -75 °C 之间。冰云的卷云光学厚度(532 纳米波长的 COT)范围很广,从 0.03(亚可见卷云部分,占所有案例的 25%)到 0.03-0.3(可见薄卷云,占 40%)再到 0.3(不透明卷云部分,占 35%)。在所有高空激光雷达观测中,约有 30% 发现了卷云特征,远远超过预期(10%)。这一事实首次表明,野火烟雾在很大程度上参与了北极卷云的形成。对流层顶附近的烟雾颗粒表面积浓度约为 5-15 µm2 cm-3,表明对流层上部的气溶胶污染水平大大提高。根据激光雷达和雷达的联合测量结果,我们从冰水含量(IWC)、冰晶数量浓度(ICNC)和可见光消光系数的剖面分析了 20 个卷云案例。冰水含量大多在 0.001-0.01 克/米-3 之间,冰晶数浓度(在冰裂隙中)累积在 0.01-10 升-1 之间。三个事实(结合在一起)证实了我们的假设,即老化的野火烟雾引发了许多观测到的卷云系统中冰的形成:(1)低 ICNC 值指向异质冰核形成,(2)烟雾污染水平的升高(就颗粒表面积浓度而言)足以显著影响对流层上部的冰核形成,以及(3)高冰饱和度比在 1.3-1.4 左右累积。3-1.4 左右的高冰饱和度,这表明在有机气溶胶颗粒(野火烟雾颗粒)的情况下,INPs 的效率非常低。
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引用次数: 0
Towards a sector-specific CO∕CO2 emission ratio: satellite-based observations of CO release from steel production in Germany 实现特定行业的 CO∕CO2 排放比:基于卫星的德国钢铁生产 CO 释放观测数据
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-05 DOI: 10.5194/acp-24-7609-2024
Oliver Schneising, Michael Buchwitz, Maximilian Reuter, Michael Weimer, Heinrich Bovensmann, John P. Burrows, Hartmut Bösch
Abstract. Global crude steel production is expected to continue to increase in the coming decades to meet the demands of the growing world population. Currently, the dominant steelmaking technology worldwide is the conventional highly CO2-intensive blast furnace–basic oxygen furnace production route (also known as the Linz–Donawitz process), which uses iron ore as raw material and coke as a reducing agent. As a result, large quantities of special gases that are rich in carbon monoxide (CO) are by-products of the various stages of the steelmaking process. Given the challenges associated with satellite-based estimates of carbon dioxide (CO2) emissions at the scale of emitting installations due to significant background levels, co-emitted CO may serve as a valuable indicator of the carbon footprint of steel plants. We show that regional CO release from steel production sites can be monitored from space using 5 years of measurements (2018–2022) from the TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor satellite, benefiting from its relatively high spatial resolution and daily global coverage. We analyse all German steel plants with blast furnaces and basic oxygen furnaces and obtain associated CO emissions in the range of 50–400 kt yr−1 per site. A comparison with the respective CO2 emissions on the level of emitting installations available from emissions trading data of the European Union Emissions Trading System yields a linear relationship with a sector-specific CO/CO2 emission ratio for the analysed steelworks of 3.24 % [2.73–3.89; 1σ], suggesting the feasibility of using CO as a proxy for CO2 emissions from comparable steel production sites. An evaluation at other steel production sites indicates that the derived CO/CO2 emission ratio is also representative of other highly optimised state-of-the-art Linz–Donawitz steelworks outside Germany and that the emission ratio is potentially valuable for estimating sector-specific CO2 emissions from remotely sensed CO emissions, provided that the underlying CO emission estimate is not affected by other sources.
摘要未来几十年,全球粗钢产量预计将继续增加,以满足不断增长的世界人口的需求。目前,全球最主要的炼钢技术是传统的高炉--碱性氧气炉生产工艺(又称林茨-多纳维茨工艺),该工艺以铁矿石为原料,焦炭为还原剂,是一种高度二氧化碳密集型工艺。因此,炼钢过程的各个阶段都会产生大量富含一氧化碳(CO)的特殊气体副产品。由于大量的背景水平,基于卫星的二氧化碳(CO2)排放量估算在排放装置的规模上面临挑战,因此共同排放的 CO 可以作为衡量钢铁厂碳足迹的重要指标。我们利用哨兵-5 号前兆卫星上的 TROPOspheric Monitoring Instrument(TROPOMI)进行了为期 5 年(2018-2022 年)的测量,结果表明,利用其相对较高的空间分辨率和每日全球覆盖范围,可以从太空监测钢铁生产基地的区域性二氧化碳排放。我们对德国所有拥有高炉和氧气炉的钢铁厂进行了分析,获得了每个钢铁厂每年 50-400 kt-1 的相关二氧化碳排放量。根据欧盟排放交易系统的排放交易数据,我们将排放装置的二氧化碳排放量与相应的二氧化碳排放量进行了比较,结果发现,在所分析的钢铁厂中,特定行业的二氧化碳/一氧化碳排放比为 3.24 % [2.73-3.89; 1σ],这表明使用二氧化碳作为可比钢铁生产基地二氧化碳排放量的替代物是可行的。对其他钢铁生产基地的评估表明,推导出的 CO/CO2 排放比也能代表德国以外其他高度优化的林茨-多纳维茨(Linz-Donawitz)先进钢铁厂,并且只要基本的 CO 排放估算不受其他来源的影响,该排放比对于从遥感 CO 排放中估算特定行业的 CO2 排放量具有潜在价值。
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引用次数: 0
Airborne observations of upper troposphere and lower stratosphere composition change in active convection producing above-anvil cirrus plumes 空中观测对流层上部和平流层下部在产生高空卷云羽流的活跃对流中的成分变化
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-04 DOI: 10.5194/acp-24-7591-2024
Andrea E. Gordon, Cameron R. Homeyer, Jessica B. Smith, Rei Ueyama, Jonathan M. Dean-Day, Elliot L. Atlas, Kate Smith, Jasna V. Pittman, David S. Sayres, David M. Wilmouth, Apoorva Pandey, Jason M. St. Clair, Thomas F. Hanisco, Jennifer Hare, Reem A. Hannun, Steven Wofsy, Bruce C. Daube, Stephen Donnelly
Abstract. Tropopause-overshooting convection in the midlatitudes provides a rapid transport pathway for air from the lower troposphere to reach the upper troposphere and lower stratosphere (UTLS) and can result in the formation of above-anvil cirrus plumes (AACPs) that significantly hydrate the stratosphere. Such UTLS composition changes alter the radiation budget and impact climate. Novel in situ observations from the NASA Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are used in this study to examine UTLS impacts from AACP-generating overshooting convection. Namely, a research flight on 31 May 2022 sampled active convection over the state of Oklahoma for more than 3 h with the NASA ER-2 high-altitude research aircraft. An AACP was bisected during this flight, providing the first such extensive in situ sampling of this phenomenon. The convective observations reveal pronounced changes in air mass composition and stratospheric hydration up to altitudes of 2.3 km above the tropopause and concentrations more than double background levels. Unique dynamic and trace gas signatures were found within the AACP, including enhanced vertical mixing near the AACP edge and a positive correlation between water vapor and ozone. Moreover, the water vapor enhancement within the AACP was found to be limited to the saturation mixing ratio of the low temperature overshoot and AACP air. Comparison with all remaining DCOTSS flights demonstrates that the 31 May 2022 flight had some of the largest tropospheric tracer and water vapor perturbations in the stratosphere and within the AACP.
摘要中纬度地区的对流层顶对流为空气从对流层下部到达对流层上部和平流层下部(UTLS)提供了一条快速输送通道,并可形成使平流层显著水化的高空卷云羽流(AACPs)。这种 UTLS 成分变化会改变辐射预算并影响气候。本研究利用美国国家航空航天局(NASA)夏季平流层动力学和化学(DCOTSS)实地观测活动中的新原位观测数据,来研究 AACP 产生的凌空对流对 UTLS 的影响。即,2022 年 5 月 31 日,美国国家航空航天局 ER-2 高空研究飞机对俄克拉荷马州上空的活跃对流进行了超过 3 小时的采样研究飞行。在这次飞行中,一个 AACP 被一分为二,首次对这一现象进行了如此广泛的现场采样。对流观测结果表明,在对流层顶以上 2.3 千米的高度,气团成分和平流层水合作用发生了明显变化,浓度是背景水平的两倍多。在 AACP 内发现了独特的动态和痕量气体特征,包括 AACP 边缘附近增强的垂直混合以及水汽和臭氧之间的正相关。此外,还发现 AACP 内的水汽增强仅限于低温过冲和 AACP 空气的饱和混合比。与 DCOTSS 其余所有飞行的比较表明,2022 年 5 月 31 日的飞行对平流层和 AACP 内的对流层示踪剂和水汽扰动最大。
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引用次数: 0
Measurement report: TURBAN observation campaign combining street-level low-cost air quality sensors and meteorological profile measurements in Prague 测量报告:结合布拉格街道级低成本空气质量传感器和气象剖面测量的 TURBAN 观测活动
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-04 DOI: 10.5194/egusphere-2024-1222
Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Jaroslav Resler, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, Igor Ezau
Abstract. Within the TURBAN project, a "Legerova campaign" focusing on air quality and meteorology in the traffic-loaded part of the Prague city (Czech Republic) was carried out from 30 May 2022 to 28 March 2023. The network comprised of 20 combined low-cost sensor (LCS) stations for NO2, O3, PM10 and PM2.5 concentrations, along with a mobile meteorological mast, a single-channel microwave radiometer and Doppler LIDAR for measurement of vertical temperature and wind profiles. Significant individual deviations of LCSs were detected during the 165 day initial field test of all units at the urban background Prague 4-Libuš reference station (coefficient of variation 17–28 %). Implementing the Multivariate Adaptive Regression Splines method for correction reduced the LCS inter-individual variability and improved correlation with reference monitors in all pollutants (R2 0.88–0.97). The LCSs' data drifts and ageing were checked by the double mass curve method for the entire measurement period. During the Legerova campaign, the highest NO2 concentrations were in traffic-loaded street canyons with continuous building blocks and several traffic lights. Aerosol pollution showed very little variation between the monitored streets. The highest PM10 and PM2.5 concentrations were recorded during temperature inversions and an episode involving pollution transported from a large forest fire in northern Czech Republic in July 2022. This report provides valuable data to support the validation of various predictive models dealing with complex urban environment, such as microscale LES model PALM tested in the TURBAN project.
摘要在 TURBAN 项目范围内,2022 年 5 月 30 日至 2023 年 3 月 28 日开展了一项 "Legerova 行动",重点关注布拉格市(捷克共和国)交通繁忙地区的空气质量和气象。该网络由 20 个用于测量二氧化氮、臭氧、可吸入颗粒物(PM10)和可吸入颗粒物(PM2.5)浓度的组合式低成本传感器(LCS)站以及一个移动气象桅杆、一个单通道微波辐射计和用于测量垂直温度和风廓线的多普勒激光雷达组成。在布拉格 4-Libuš 城市背景参考站对所有设备进行了为期 165 天的初步实地测试(变异系数为 17-28%),发现 LCS 存在明显的个别偏差。采用多元自适应回归样条法进行校正降低了 LCS 的个体间变异性,并提高了与所有污染物参考监测仪的相关性(R2 0.88-0.97)。在整个测量期间,采用双质量曲线法检查了 LCS 的数据漂移和老化情况。在 Legerova 测量活动期间,二氧化氮浓度最高的地方是交通繁忙的街道峡谷,那里有连续的建筑街区和多个交通信号灯。气溶胶污染在受监测街道之间的差异很小。最高的 PM10 和 PM2.5 浓度出现在气温倒伏期间,以及 2022 年 7 月捷克共和国北部一场大规模森林火灾造成的污染期间。该报告提供了宝贵的数据,有助于验证各种处理复杂城市环境的预测模型,例如在 TURBAN 项目中测试的微尺度 LES 模型 PALM。
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引用次数: 0
Technical note: Retrieval of the supercooled liquid fraction in mixed-phase clouds from Himawari-8 observations 技术说明:从 Himawari-8 号观测数据中检索混合相云中的过冷液体部分
IF 6.3 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-07-04 DOI: 10.5194/acp-24-7559-2024
Ziming Wang, Husi Letu, Huazhe Shang, Luca Bugliaro
Abstract. The supercooled liquid fraction (SLF) in mixed-phase clouds (MPCs) is an essential variable of cloud microphysical processes and climate sensitivity. However, the SLF is currently calculated in spaceborne remote sensing only as the cloud phase–frequency ratio of adjacent pixels, which results in a loss of the original resolution in observations of cloud liquid or ice content within MPCs. Here, we present a novel method for retrieving the SLF in MPCs based on the differences in radiative properties of supercooled liquid droplets and ice particles at visible (VIS) and shortwave infrared (SWI) channels of the geostationary Himawari-8. Liquid and ice water paths are inferred by assuming that clouds are composed of only liquid or ice, with the real cloud water path (CWP) expressed as a combination of these two water paths (SLF and 1-SLF as coefficients), and the SLF is determined by referring to the CWP from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). The statistically relatively small cloud phase spatial inhomogeneity at a Himawari-8 pixel level indicates an optimal scene for cloud retrieval. The SLF results are comparable to global SLF distributions observed by active instruments, particularly for single-layered cloud systems. While accessing the method's feasibility, SLF averages are estimated between 74 % and 78 % in Southern Ocean (SO) stratocumulus across seasons, contrasting with a range of 29 % to 32 % in northeastern Asia. The former exhibits a minimum SLF around midday in summer and a maximum in winter, while the latter trend differs. This novel algorithm will be valuable for research to track the evolution of MPCs and constrain the related climate impact.
摘要。混合相云(MPCs)中的过冷液体分数(SLF)是云微物理过程和气候敏感性的一个重要变量。然而,目前在空间遥感中,SLF 仅作为相邻像素的云相频比来计算,这导致了混相云中云液或云冰含量观测分辨率的损失。在此,我们根据地球静止轨道 "向日葵-8 "卫星可见光(VIS)和短波红外(SWI)信道中过冷液滴和冰粒辐射特性的差异,提出了一种新方法来检索多大气压积云中的SLF。通过假设云只由液体或冰组成来推断液态和冰态的水路径,真实的云水路径(CWP)表示为这两种水路径的组合(SLF 和 1-SLF 作为系数),而 SLF 则通过参考云-气溶胶激光雷达和红外探路者卫星观测(CALIPSO)的 CWP 来确定。据统计,Himawari-8 像素级别的云相空间不均匀性相对较小,这表明这是一个最佳的云检索场景。SLF结果与主动仪器观测到的全球SLF分布相当,特别是对于单层云系统。在验证该方法可行性的同时,南大洋层积云各季节的平均SLF估计在74%到78%之间,而亚洲东北部的SLF则在29%到32%之间。前者在夏季正午前后表现出最小的SLF,在冬季表现出最大的SLF,而后者的趋势则不同。这种新颖的算法将对跟踪多云团的演变和制约相关的气候影响具有重要的研究价值。
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引用次数: 0
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Atmospheric Chemistry and Physics
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