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Links between atmospheric aerosols and sea state in the Arctic Ocean 北冰洋大气气溶胶与海况之间的联系
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-26 DOI: 10.1016/j.atmosenv.2024.120844
Alireza Moallemi , Alberto Alberello , Iris Thurnherr , Guangyu Li , Zamin A. Kanji , Filippo Bergamasco , Roman Pohorsky , Filippo Nelli , Alessandro Toffoli , Julia Schmale
Sea spray emission is the largest mass flux of aerosols to the atmosphere with important impact on atmospheric radiative transfer. However, large uncertainties still exit in constraining this mass flux and its climate forcing, in particular in the Arctic, where sea ice and relatively low wind speed in summer constitute a significantly different regime compared to the global ocean. Sea state conditions and marine boundary layer stability are also critical variables, but their contribution is often overlooked. Here we present concurrent observations of sea state using a novel stereo camera system, of sea spray through coarse mode aerosols, and of meteorological variables to determine boundary layer stability in the Barents and Kara Seas during the 2021 Arctic Century Expedition. Our findings reveal that aerosol concentrations were highest over open waters, closely correlating with wave height, followed by wind speed, wave steepness, and wave age. Notably, these correlations were stronger under unstable marine boundary layer conditions, reflecting immediate sea spray generation. By analysing various combinations of sea and atmospheric variables, we identified the wave height Reynolds number as the most effective indicator of atmospheric sea spray concentration, explaining 57% of its variability in unstable conditions. Our study underscores the need to consider sea state, wind, and boundary layer conditions together to accurately estimate atmospheric sea spray concentrations in the Arctic.
海雾排放是大气中最大的气溶胶通量,对大气辐射传输具有重要影响。然而,在制约这种质量通量及其气候强迫方面仍然存在很大的不确定性,特别是在北极地区,那里的海冰和夏季相对较低的风速构成了与全球海洋明显不同的制度。海况条件和海洋边界层稳定性也是关键变量,但它们的作用往往被忽视。在此,我们介绍在 2021 年北极世纪考察期间,利用新型立体摄像系统对海况、通过粗模气溶胶对海雾以及气象变量进行的同步观测,以确定巴伦支海和喀拉海的边界层稳定性。我们的研究结果表明,开放水域的气溶胶浓度最高,与波高密切相关,其次是风速、波陡和波龄。值得注意的是,在不稳定的海洋边界层条件下,这些相关性更强,反映了海雾的直接生成。通过分析海洋和大气变量的各种组合,我们发现波高雷诺数是大气海雾浓度的最有效指标,可解释不稳定条件下海雾浓度变化的 57%。我们的研究强调,需要综合考虑海况、风和边界层条件,以准确估计北极大气中的海雾浓度。
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引用次数: 0
Characteristics of light absorption and environmental effects of Brown carbon aerosol in Chongqing during summer and winter based on online measurement: Implications of secondary formation 基于在线测量的重庆夏季和冬季棕碳气溶胶的光吸收特征及环境效应:二次形成的影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-26 DOI: 10.1016/j.atmosenv.2024.120843
Hong Wu , Chao Peng , Tianyu Zhai , Jingcheng Deng , Peili Lu , Zhenliang Li , Yang Chen , Mi Tian , Zhier Bao , Xin Long , Fumo Yang , Chongzhi Zhai
Light-absorbing organic carbon (i.e., brown carbon, BrC) significantly contributes to light absorption and radiative forcing in the atmospheric particles. However, the secondary formation of BrC and optical properties of secondary BrC are poorly understood. In this study, we analyzed and evaluated the light absorption and environmental effects of BrC and secondary BrC from July 1st to 31st, 2022 (summer) and January 20th to February 20th, 2023 (winter) in Chongqing. BrC and secondary BrC light absorption were estimated via a seven-wavelength aethalometer and the statistical approach. The average values of secondary BrC light absorption (AbsBrC,sec,λ) accounted for 46.2–56.5% of AbsBrC. AbsBrC,370 and AbsBrC,sec,370 were significantly higher during winter (26.2 ± 13.2 and 9.1 ± 5.2 Mm−1 respectively) than that during summer (7.2 ± 4.1 and 5.2 ± 3.5 Mm−1 respectively) (p < 0.001), suggesting secondary formation played an essential role in BrC. A diurnal cycle of AbsBrC,sec,370 was explained by the photobleaching of light-absorbing chromophores under the oxidizing conditions in the daytime, and the formation of chromophores via aqueous reactions with NH4+ and NOx after sunset during winter. PSCF analysis showed that transport of anthropogenic emissions from the northeastern and southeastern areas of Chongqing was the important source of the secondary BrC in PP during winter. During winter, the average values of SFEBrC and SFEBrC,sec were 31.9 and 27.4 W g−1 lower than that during summer (64.7 and 44.5 W g−1), respectively. In contrast, J[NO2] values of SFEBrC and SFEBrC,sec decreased by 23.3% and 8.7% during winter higher than that during summer (19.9% and 5.6%), indicating that BrC and secondary BrC cause substantial radiative effects and atmospheric photochemistry. Overall, this study is helpful in understanding the characterization and secondary formation of BrC and accurately evaluating the environmental effects of BrC in Chongqing.
光吸收有机碳(即褐碳,BrC)对大气颗粒中的光吸收和辐射强迫有重要作用。然而,人们对褐碳的二次形成和二次褐碳的光学特性知之甚少。在本研究中,我们分析和评估了重庆地区2022年7月1日至31日(夏季)和2023年1月20日至2月20日(冬季)BrC和二次BrC的光吸收和环境效应。溴化碳和二次溴化碳的光吸收是通过七波长光度计和统计方法估算的。二次 BrC 光吸收的平均值(AbsBrC,sec,λ)占 AbsBrC 的 46.2-56.5%。冬季的 AbsBrC,370 和 AbsBrC,sec,370 分别为 26.2 ± 13.2 和 9.1 ± 5.2 Mm-1,明显高于夏季(分别为 7.2 ± 4.1 和 5.2 ± 3.5 Mm-1)(p <0.001),表明二次形成在 BrC 中起着重要作用。AbsBrC,sec,370的昼夜周期可解释为白天在氧化条件下光吸收发色团的光漂白,以及冬季日落后通过与NH4+和NOx的水反应形成发色团。PSCF分析表明,重庆东北部和东南部地区的人为排放物迁移是冬季PP中二次BrC的重要来源。冬季的 SFEBrC 和 SFEBrC,sec 平均值分别比夏季(64.7 W g-1 和 44.5 W g-1)低 31.9 W g-1 和 27.4 W g-1。相比之下,冬季 SFEBrC 和 SFEBrC,sec 的 J[NO2] 值下降了 23.3% 和 8.7%,高于夏季(19.9% 和 5.6%),这表明 BrC 和次级 BrC 对大气产生了巨大的辐射效应和光化学作用。总之,本研究有助于了解 BrC 的特征和二次形成,准确评估 BrC 在重庆的环境影响。
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引用次数: 0
Morphology and elemental composition of individual solid dust particles: From different sources to the atmosphere 单个固体尘埃粒子的形态和元素组成:从不同来源到大气层
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-26 DOI: 10.1016/j.atmosenv.2024.120842
Wenhua Wang , Mengyang Wang , Longyi Shao , Xiuyan Zhou , Zhe Zhao , Na Li , Hui Zhou , Weijun Li
This study investigates the morphology and elemental composition of individual solid dust particles from various sources (e.g., thermal power plant, domestic coal combustion, building construction dust, wind-blown dust, Asian dust storm, and road related dust) to the atmosphere under high and low relative humidity (RH) conditions in a coastal city of north China by using high-resolution electron microscopes. The results showed that distinct variations between dust particles from thermal power plant and domestic coal combustion, despite both using coal as fuel. Specifically, 88.6% (by number) of thermal power plant particles were spherical, whereas only 2 out of 347 particles from domestic coal combustion exhibited a spherical shape. Furthermore, domestic coal combustion particles showed a higher proportion of Ca-rich particles compared to those from thermal power plant. The wind-blown dust and Asian dust storm particles were mainly “Si + Al” subtype (52.0% v.s. 75.3%) and Si-dominant subtype (16.4% v.s. 11.7%) particles, which were mainly from crustal sources. However, wind-blown dust contained a higher fraction of Ca-rich (11.6%) and Fe-rich (5.3%) particles than Asian dust. The building construction dust particles primarily consisted of irregular Ca-dominant (39.4%) and “Ca + Si” subtype (29.8%) particles. Road related dust were also mainly Si-rich particles (52.9%), likely from re-suspended soil, along with a notable presence of spherical (8.0%) and Fe-rich particles (19.3%), possibly linked to vehicle emissions and brake wear. Additionally, relative number percentage of Na-rich particles and the average weigh ratios of Na in the atmospheric particles were higher than those from all above-mentioned source samples, suggesting that sea-salt related particles might be an important source of the atmospheric dust at the coastal city. The results indicated that Ca-rich particles were significantly modified by S and NaCl particles might lose Cl through heterogeneous reactions under higher RH.
本研究利用高分辨率电子显微镜,研究了中国北方某沿海城市在高相对湿度(RH)和低相对湿度(RH)条件下,不同来源(如火力发电厂、生活燃煤、建筑施工扬尘、风吹扬尘、亚洲沙尘暴和道路扬尘)的单个固体粉尘颗粒在大气中的形态和元素组成。结果表明,尽管都以煤为燃料,但火电厂和生活燃煤产生的粉尘颗粒之间存在明显差异。具体来说,88.6%(按数量计算)的火电厂颗粒呈球形,而在 347 个生活燃煤颗粒中,只有 2 个呈球形。此外,与火力发电厂的颗粒相比,国内燃煤颗粒中富含 Ca 的比例更高。风吹尘和亚洲沙尘暴颗粒主要是 "Si + Al "亚型(52.0% 对 75.3%)和以 Si-为主的亚型(16.4% 对 11.7%)颗粒,这些颗粒主要来自地壳。不过,与亚洲尘埃相比,风吹尘埃中富含钙(11.6%)和铁(5.3%)的颗粒比例更高。建筑施工尘粒主要由不规则的钙为主(39.4%)和 "钙+硅 "亚型(29.8%)颗粒组成。与道路相关的粉尘也主要是富含硅的颗粒(52.9%),可能来自重新悬浮的土壤,同时还存在明显的球形颗粒(8.0%)和富含铁的颗粒(19.3%),可能与汽车尾气排放和制动器磨损有关。此外,大气颗粒物中富含 Na 的相对数量百分比和 Na 的平均重量比均高于上述所有来源样本,这表明与海盐有关的颗粒物可能是沿海城市大气尘埃的一个重要来源。结果表明,在较高相对湿度条件下,富含 Ca 的颗粒物会受到 S 的明显修饰,NaCl 颗粒物可能会通过异相反应失去 Cl。
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引用次数: 0
In silico modelling of radiative efficiencies of anthropogenic greenhouse gases 人为温室气体辐射效率的硅学建模
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-25 DOI: 10.1016/j.atmosenv.2024.120839
Daniela Alvarado-Jiménez , Nicola Tasinato
Radiative efficiency (RE) is a climate metric adopted in international reports on climate change to quantify the greenhouse capacity of gases, and hence to guide decision-making processes and drive transitions in the production and utilization of chemicals in different application fields. Key quantities for the determination of the RE of a gas are the atmospheric irradiance profile and the infrared (IR) absorption cross section spectrum. The latter is usually measured experimentally, even though acquiring high-quality IR spectra can pose severe challenges, sometimes limiting the accuracy or the accessible spectral range. While computational quantum chemistry methods have emerged as valuable tools to simulate IR absorption properties, their application to REs estimation is still limited to the use of the double-harmonic approximation, which presents fundamental limitations. In this work, a cost-effective quantum chemical (QC) workflow including non-empirical anharmonic contributions to spectral properties and an automatic identification of conformer distribution is presented for the accurate evaluation of REs using a range of atmospheric irradiance profiles. Different levels of theory are considered, according to the current state-of-the-art, and the accuracy of the QC RE tool is demonstrated with reference to a number of representative halocarbons widely used in refrigeration, manufacturing, and pharmaceutical fields. The results show that REs can be computed with an average accuracy of 5% using double-hybrid functionals, which overshoot the widely used B3LYP method. Finally, the QC methodology is applied to determine the REs of selected halocarbons for which data is limited, or to address some contradictory results appeared in the literature for some species. The outcomes of this work demonstrate that QC anharmonic IR cross section spectra can be used to estimate REs with an accuracy on par with that of experimental measurements, hence applicable to challenging cases for providing data for policymakers as well for screening purposes when seeking new replacement compounds.
辐射效率(RE)是气候变化国际报告中采用的一种气候指标,用于量化气体的温室效应能力,从而指导决策过程,推动不同应用领域化学品生产和利用的转型。确定气体 RE 的关键量是大气辐照度曲线和红外线(IR)吸收截面光谱。后者通常是通过实验测量的,尽管获取高质量的红外光谱会带来严峻的挑战,有时会限制精确度或可获取的光谱范围。虽然计算量子化学方法已成为模拟红外吸收特性的重要工具,但其在 REs 估算中的应用仍局限于使用双谐波近似,这带来了根本性的限制。在这项工作中,介绍了一种经济有效的量子化学(QC)工作流程,其中包括对光谱特性的非经验非谐波贡献和构象分布的自动识别,以便利用一系列大气辐照度剖面准确评估 REs。根据当前最先进的理论,考虑了不同的理论水平,并参考了广泛应用于制冷、制造和制药领域的一些具有代表性的卤化碳,展示了 QC RE 工具的准确性。结果表明,使用双杂交函数计算 REs 的平均准确度为 5%,超过了广泛使用的 B3LYP 方法。最后,QC 方法被用于确定数据有限的某些卤化碳的 REs,或解决文献中出现的某些物种的矛盾结果。这项工作的成果表明,QC 非谐波红外截面光谱可用于估算 REs,其精确度与实验测量结果相当,因此适用于具有挑战性的情况,为决策者提供数据,并在寻找新的替代化合物时用于筛选目的。
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引用次数: 0
Total deposition of sulphur to coniferous forests in Sweden - Taking canopy exchange into account 瑞典针叶林的硫沉积总量--考虑树冠交换因素
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-25 DOI: 10.1016/j.atmosenv.2024.120840
G. Pihl Karlsson , P.E. Karlsson , S. Hellsten , H. Danielsson , V. Kronnäs , C. Akselsson
In the low deposition situation of today at many of the long-term Swedish forest monitoring sites, the deposition measured as precipitation to the open field, i.e. bulk deposition of oxidized sulphur (S) is often higher or equal to deposition of S sampled under the forest canopies, i.e. as throughfall. This suggests that the total S deposition estimated using throughfall is underestimated. The reason for this is direct exchange of S with the forest canopies, leading to an underestimation which becomes evident in low-deposition areas. We describe a new method to estimate the dry deposition of S to coniferous forest based on measurements with Teflon string samplers as surrogate surfaces, in combination with measurements of the net throughfall for sodium (throughfall subtracted with wet deposition). The wet deposition was estimated from bulk deposition measurements on the open field, corrected for dry deposition to the collectors. The method was applied for Norway spruce forests at monitoring sites across Sweden during nine years 2014–2022, and total deposition was calculated based on wet deposition and the estimated dry deposition. The estimated annual total deposition of S as a mean value for coniferous forests ranged between 0.8 and 5.2 kg S ha−1 yr−1 with lowest values in northern Sweden and highest in southwest Sweden. The share of dry deposition of the total S deposition was between 20 and 53%. The mean annual deposition of S measured as throughfall during 2014–2022 for three different regions in Sweden was between 16 and 41% lower compared to the corresponding total deposition estimated with the new method. The canopy exchange of S was analyzed on a monthly basis as the difference between the estimated total deposition and the measured throughfall deposition of S. At most sites, there was a canopy uptake of S during the summer months and a leakage of S during the winter months. This indicates that the canopy exchange of S is a phenomenon that involves some biological activity.
在瑞典许多长期森林监测点目前的低沉积情况下,以降水形式测量的空地沉积物(即氧化硫(S)的大量沉积)往往高于或等于在林冠下采样的 S 沉积物(即直降)。这表明,用直流降雨量估算的 S 沉积总量被低估了。其原因在于 S 与林冠的直接交换,从而导致低估,这在低沉积区尤为明显。我们介绍了一种估算针叶林 S 干沉降量的新方法,该方法基于以聚四氟乙烯绳采样器为替代表面的测量结果,并结合钠净通过量的测量结果(通过量减去湿沉降量)。湿沉降量是根据空地上的大量沉降测量结果估算的,并对采集器上的干沉降量进行了校正。该方法适用于 2014-2022 年九年期间瑞典各地监测点的挪威云杉林,并根据湿沉降量和估计的干沉降量计算出总沉降量。针叶林中估计的 S 年总沉积量的平均值介于 0.8 至 5.2 kg S ha-1 yr-1 之间,瑞典北部的沉积量最低,瑞典西南部的沉积量最高。干沉积物占总 S 沉积物的比例在 20% 到 53% 之间。与采用新方法估算的相应总沉积量相比,2014-2022 年期间瑞典三个不同地区通过降雨量测量的 S 年平均沉积量减少了 16% 至 41%。根据估算的总沉积量与测量的 S 径流沉积量之差,按月对 S 的冠层交换量进行了分析。这表明,树冠层的 S 交换现象涉及某种生物活动。
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引用次数: 0
A comprehensive evaluation of the atmospheric impacts and health risks of cooking fumes from different cuisines 全面评估不同菜系烹饪油烟对大气的影响和健康风险
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-24 DOI: 10.1016/j.atmosenv.2024.120837
Junfeng Zhang , Wenjiao Duan , Shuiyuan Cheng , Chuanda Wang
Pollutants emitted by catering enterprises pose a significant threat to the environment and public health. In this study, based on a systematic analysis of volatile organic compound (VOC) emission characteristics of different cuisines, the contribution of cooking emissions from catering enterprises to the PM2.5 and O3 concentrations in the atmosphere was evaluated using generation potential calculations and WRF-CAMx simulations. The health exposure risks of VOCs in kitchen breathing areas and those of PM2.5 and O3 contributed by the catering enterprises were evaluated. The generation potential calculation results showed that the catering enterprises exhibit 2.21–5.00 gO3/gVOCs of ozone formation potential (OFP) and 0.07–0.21 gSOA/gVOCs of secondary organic aerosol production potential (SOAP). The WRF-CAMx simulation results indicated that cooking emissions from catering enterprises contribute 0.36–1.91 μg/m3 and 0.05–0.21 μg/m3 to PM2.5 and maximum daily 8-h average (MDA8) concentrations of O3. The health exposure risks of PM2.5 and O3 were higher in catering enterprises in southern cities than in northern cities and were higher in urban areas than in suburban areas. The average hazardous VOCs (HVOCs) concentrations ranged from 53 ± 16 to 357 ± 31 μg/m3 in kitchen breathing areas. Acrolein was the primary contributor to the hazard index (HI) of all VOC species, accounting for 50.9%–99.5%. The total incremental lifetime carcinogenic risk (ILCR) of all cuisines exceeded the acceptable thresholds of 1.00 × 10−6. These findings provide insights that can aid in the formation and implementation of pollutant mitigation strategies in the catering industry.
餐饮企业排放的污染物对环境和公众健康构成重大威胁。本研究在系统分析不同菜系挥发性有机化合物(VOC)排放特征的基础上,利用生成潜力计算和 WRF-CAMx 模拟,评估了餐饮企业烹饪排放对大气中 PM2.5 和 O3 浓度的贡献。评估了厨房呼吸区挥发性有机化合物的健康暴露风险以及餐饮企业产生的 PM2.5 和 O3 的健康暴露风险。生成潜势计算结果显示,餐饮企业的臭氧形成潜势(OFP)为 2.21-5.00 gO3/gVOCs,二次有机气溶胶生成潜势(SOAP)为 0.07-0.21 gSOA/gVOCs。WRF-CAMx 模拟结果表明,餐饮企业的烹饪排放对 PM2.5 和臭氧的最大日 8 小时平均浓度(MDA8)分别有 0.36-1.91 μg/m3 和 0.05-0.21 μg/m3 的贡献。南方城市餐饮企业的 PM2.5 和 O3 健康暴露风险高于北方城市,市区高于郊区。厨房呼吸区的有害挥发性有机化合物(HVOCs)平均浓度介于 53 ± 16 至 357 ± 31 μg/m3 之间。在所有挥发性有机化合物种类中,丙烯醛是造成危害指数(HI)的主要因素,占 50.9%-99.5%。所有菜肴的终生总致癌风险增量(ILCR)都超过了 1.00 × 10-6 的可接受阈值。这些研究结果有助于餐饮业制定和实施污染物缓解战略。
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引用次数: 0
Controls on the stable Mo isotopic composition of inner-continental precipitation 内大陆降水稳定钼同位素组成的控制因素
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-24 DOI: 10.1016/j.atmosenv.2024.120838
E.M. O'Sullivan , A.K.C. Kaufmann , C. Rosca , M.G. Babechuk , M.C. Pierret , N.H. Waber , T.F. Nägler
The molybdenum (Mo) isotope budget of the surface environment has been well characterized in recent decades, facilitating accurate mass balance modeling of the ancient redox-driven Mo cycle. One yet unresolved component is the range of possible processes and sources that result in isotopically heavy river waters relative to continental sources. Following a recent hypothesis that isotopically heavy δ98Mo of precipitation may control the final δ98Mo of river water relative to its continental source bedrock, we investigated the δ98Mo composition of 19 snow samples from three locations in Central Europe: the Swiss Alps (“Alpine” samples) from the Hochalpine Forschungsstation Jungfraujoch (HFSJ) in both summer and winter, the Swiss Jura Mountains in winter and the French Vosges Mountains in winter. Stream waters from two snowmelt-fed streams were additionally collected from the Alpine site. Snow sample δ98Mo compositions were highly variable, ranging from −0.03 to +1.93 ‰, with no clear mixing trends indicating complex sources, source pathways, or post-depositional processing. Only the winter snow samples from the high-altitude HFSJ site had δ98Mo values consistently heavier than typical continental crust. The δ98Mo results were coupled with radiogenic Sr isotopic, major ion, and trace element compositions as tracers for three major sources of airborne ion inputs: sea salt, mineral dust, and anthropogenic aerosols. We found that the most likely source of Mo to precipitation in the lower elevation Vosges and Jura Mountains samples was isotopically light soil mineral dust, which reflected the underlying bedrock sources, with a likely additional anthropogenic component. The isotopically heavy winter snow samples at the elevated HFSJ site were attributed to a higher input of carbonate mineral dust from long-distance transport of carbonate-rich Saharan dust, which was overwritten in the summer by an influx of low elevation sources transported upwards during higher vertical thermal mixing. Finally, we concluded that precipitation has a negligible direct effect on the overall Mo content and isotopic composition of inner continental European streams and rivers relative to other sources, such as bedrock weathering. Future time-series studies may augment these conclusions to show possible heterogeneity of precipitation as well as the addition of sample sites closer to marine sources, where a larger flux of isotopically heavy marine aerosols to streams might be expected.
近几十年来,地表环境的钼(Mo)同位素预算已经得到了很好的表征,有助于对古代氧化还原驱动的钼循环进行精确的质量平衡建模。一个尚未解决的问题是,与大陆来源相比,导致河水同位素偏重的可能过程和来源范围。根据最近提出的一个假设,即降水中同位素重的δ98Mo可能会控制河水相对于其大陆源基岩的最终δ98Mo,我们调查了中欧三个地点的 19 个雪样的δ98Mo组成:瑞士阿尔卑斯山("阿尔卑斯山 "样本),来自少女峰研究站(HFSJ)的夏季和冬季样本;瑞士汝拉山脉的冬季样本;法国孚日山脉的冬季样本。此外,还在阿尔卑斯山采集了两条融雪溪流的溪水。雪样中的δ98Mo成分变化很大,从-0.03到+1.93 ‰不等,没有明显的混合趋势,这表明雪样的来源、来源途径或沉积后处理都很复杂。只有来自高海拔 HFSJ 站点的冬雪样本的 δ98Mo 值始终重于典型的大陆地壳。δ98Mo结果与放射性Sr同位素、主要离子和痕量元素组成相结合,作为空气中离子输入的三个主要来源的示踪剂:海盐、矿物尘埃和人为气溶胶。我们发现,在海拔较低的孚日山脉和汝拉山脉样本中,降水中最有可能的钼元素来源是同位素轻的土壤矿物尘埃,这反映了下层基岩的来源,可能还有人为成分。高海拔地区 HFSJ 的冬雪样本中同位素含量较高,这是因为富含碳酸盐的撒哈拉尘埃长距离迁移产生了较多的碳酸盐矿物尘埃,而在夏季,这些碳酸盐尘埃被在较高的垂直热混合过程中向上迁移的低海拔来源的流入所覆盖。最后,我们得出结论,相对于基岩风化等其他来源,降水对欧洲大陆内部溪流和河流的总体钼含量和同位素组成的直接影响微乎其微。未来的时间序列研究可能会增强这些结论,以显示降水可能存在的异质性,并增加更靠近海洋源的样本点,因为在这些样本点,可能会有更多同位素重的海洋气溶胶流向溪流。
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引用次数: 0
Comparative analysis of winter composite-PM2.5 in Central Indo Gangetic Plain cities: Combined organic and inorganic source apportionment and characterization, with a focus on the photochemical age effect on secondary organic aerosol formation 印度河平原中部城市冬季综合 PM2.5 比较分析:有机和无机源的综合分配和特征描述,重点关注光化学年龄对二次有机气溶胶形成的影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-21 DOI: 10.1016/j.atmosenv.2024.120827
Akanksha Lakra , Ashutosh Kumar Shukla , Himadri Sekhar Bhowmik , Amit Kumar Yadav , Vaishali Jain , Vishnu Murari , Sreenivas Gaddamidi , Vipul Lalchandani , Sachchida Nand Tripathi
To gain insights into air quality dynamics, a high-end instrument such as High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) alongside an Aethalometer was used to measure the Composite PM2.5 (C-PM2.5) in Lucknow and Kanpur during winter. It encompasses non-refractive PM2.5 (NR-PM2.5) and Black Carbon (BC) mass concentrations. Significant variation was noted in average C-PM2.5 concentrations at both sites, as 168.8 ± 61.3 μg m−3 in Lucknow and 90.7 ± 25.7 μg m−3 in Kanpur. Organics emerged as the predominant component, constituting ∼55%–65% of the C-PM2.5 mass, followed by inorganics (24% and 30%) and BC (20% and 8%). The present study employs Positive Matrix Factorization (PMF) on combined organic and inorganic source apportionment, resolving eight and seven source factors at Lucknow and Kanpur, respectively. Both sites exhibit significant contributions from solid-fuel combustion organic aerosol (SFC-OA), with ∼11% in Lucknow and 8% in Kanpur. However, SFC-OA mass concentration in Lucknow, at 24.67 μg m-³, is nearly double that in Kanpur (12.05 μg m-³). This was likely due to domestic coal burning in the nearby households, unregulated open burning, and burning of garbage on roadsides. The study shows that both sites were affected by oxidized biomass burning OA (O-BBOA) emissions, with increased concentration during the night due to dark oxidation by NO3 radicals. The diurnal variation of secondary organic aerosols (SOA), such as O-BBOA and semi-volatile oxygenated OA (SVOOA), shows increasing concentration during daytime hours. Therefore, the photochemical aging (ta) role in SOA formation was analyzed, and it was revealed that the formation might primarily be driven by photochemical oxidation. Additionally, two inorganic-rich factors, sulfate and nitrate-related OA (SO4-OA and NO3-OA) at both sites and additional ammonium chloride-related OA (NH4Cl-OA) resolved at Lucknow. Our study shows that NO3-OA and SO4-OA formation was dominated by aqueous phase processes due to high relative humidity and decline in concentration with increasing ta (ta > 30 h) during winter.
为了深入了解空气质量动态,我们使用高分辨率飞行时间气溶胶质谱仪(HR-ToF-AMS)等高端仪器和空气热量计来测量勒克瑙和坎普尔冬季的复合 PM2.5(C-PM2.5)。它包括非折射性 PM2.5(NR-PM2.5)和黑碳(BC)的质量浓度。两个地点的 C-PM2.5 平均浓度存在显著差异,勒克瑙为 168.8 ± 61.3 μg m-3,坎普尔为 90.7 ± 25.7 μg m-3。有机物是主要成分,占 C-PM2.5 质量的 55% 至 65%,其次是无机物(24% 和 30%)和 BC(20% 和 8%)。本研究采用正矩阵因子法(PMF)对有机和无机源进行综合分配,分别解决了勒克瑙和坎普尔的 8 个和 7 个源因子问题。这两个地点的固体燃料燃烧有机气溶胶(SFC-OA)贡献都很大,勒克瑙为 11%,坎普尔为 8%。然而,勒克瑙的 SFC-OA 质量浓度为 24.67 μg m-³,几乎是坎普尔(12.05 μg m-³)的两倍。这可能是由于附近家庭的燃煤、无管制的露天焚烧和路边的垃圾焚烧造成的。研究表明,这两个地点都受到氧化生物质燃烧 OA(O-BBOA)排放的影响,由于 NO3 自由基的暗氧化作用,夜间浓度增加。二次有机气溶胶(SOA),如 O-BBOA 和半挥发性含氧 OA(SVOOA)的昼夜变化显示,白天浓度增加。因此,分析了光化学老化(ta)在 SOA 形成中的作用,结果表明 SOA 的形成可能主要由光化学氧化作用驱动。此外,两个地点的硫酸盐和硝酸盐相关 OA(SO4-OA 和 NO3-OA)以及勒克瑙的氯化铵相关 OA(NH4Cl-OA)这两个富含无机物的因素也得到了解决。我们的研究表明,由于冬季相对湿度高,NO3-OA 和 SO4-OA 的形成主要是水相过程,而且浓度随着 ta 的增加(ta > 30 小时)而下降。
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引用次数: 0
Well-planned greenery improves air urban quality - Modelling the effect of altered airflow and pollutant deposition 规划合理的绿化可改善城市空气质量--模拟气流和污染物沉积变化的影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-21 DOI: 10.1016/j.atmosenv.2024.120829
Malin S.M. Gustafsson , Jenny Lindén , Emelie M.M. Johansson , Ågot K. Watne , Johan Uddling , Daniel Sjölie , Håkan Pleijel
Urban air quality is influenced by vegetation through alterations in airflow and pollutant deposition processes. We investigated these interactions by integrating the Vegetation Impact Dynamic Assessment model (VIDA) with the Large-Eddy Simulation model PALM. Our analysis focus on nitrogen dioxide (NO₂) and particulate matter (PM) concentrations at the local scale, considering three tree genera. Our findings reveal the necessity of accounting for both gaseous pollutants and particles separately due to their differing mechanisms of deposition onto leaves. The coupled PALM-VIDA model demonstrates a significant reduction in PM levels across the modelling domain and within street canyons when deposition to vegetation is incorporated. Reduction in NO₂ through deposition to vegetation is lower but human NO2 exposure can still be decreased if tree species selection and placement leads to desirable effects on air flow. Sparse tree arrangements or species with sparse crowns facilitate ventilation and are often better at reducing NO₂ concentrations in street canyons compared to denser vegetation with higher deposition but negative effects on ventilation. Our study informs urban planning and green infrastructure design, underscoring the multifaceted role of urban greenery in air pollution mitigation strategies. Its main conclusion is that both deposition processes and the influence of air mixing and ventilation need to be considered to accurately assess the effects of urban trees on local air quality. Ill-considered placement and species selection may cause a net increase in pollutants underneath the trees. However, careful planning can address this risk and instead improve overall air quality.
植被通过改变气流和污染物沉积过程影响城市空气质量。我们将植被影响动态评估模型(VIDA)与大埃迪模拟模型 PALM 相结合,对这些相互作用进行了研究。我们的分析重点是当地范围内的二氧化氮(NO₂)和颗粒物(PM)浓度,并考虑了三种树属。我们的研究结果表明,由于气态污染物和颗粒物在叶片上的沉积机制不同,因此有必要将它们分开计算。PALM-VIDA 耦合模型显示,如果将植被上的沉积物考虑在内,整个建模域和街道峡谷内的可吸入颗粒物水平会显著降低。通过沉积到植被上减少的 NO₂ 较少,但如果树种的选择和摆放能对气流产生理想的影响,仍可减少人类的 NO2 暴露。稀疏的树木排列或树冠稀疏的树种有利于通风,与沉积物较高但对通风有负面影响的茂密植被相比,稀疏的树木排列或树冠稀疏的树种通常能更好地降低街道峡谷中的二氧化氮浓度。我们的研究为城市规划和绿色基础设施设计提供了信息,强调了城市绿化在空气污染缓解战略中的多方面作用。研究的主要结论是,要准确评估城市树木对当地空气质量的影响,必须同时考虑沉积过程以及空气混合和通风的影响。考虑不周的位置和树种选择可能会导致树下污染物的净增加。不过,精心规划可以解决这一风险,从而改善整体空气质量。
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引用次数: 0
Impact of the 2020 COVID-19 lockdown on the concentration of non-methane volatile organic compounds in a UK urban atmosphere 2020 年 COVID-19 封锁对英国城市大气中非甲烷挥发性有机化合物浓度的影响
IF 4.2 2区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-09-21 DOI: 10.1016/j.atmosenv.2024.120836
Emmanuel Bernard , Rebecca L. Cordell , Robert S. Blake , Michael J. Wilde , Paul S. Monks
The changes in air quality brought about by the COVID-19 lockdowns can provide valuable insight into how longer-term reductions in emissions might affect atmospheric composition. In urban Leicester UK, the 2020 COVID “lockdown” brought about several notable changes in atmospheric composition, including a considerable decrease (20–60%) in concentrations of non-methane volatile organic compounds (NMVOCs). Given their varied emission sources and lifetimes, NMVOC data can give valuable insights into how behavioural change impact atmospheric composition. The total concentration of 48 NMVOCs at roadside (RS) sites decreased from a pre-lockdown (sampled 16th-24th March 2020) concentration of 181.3 ± 41.4 μg/m3 to 82.0 ± 12.8 μg/m3 during lockdown (LD, sampled 18th-21st May 2020), before rebounding to a concentration of 236.3 ± 23.9 μg/m3 post lockdown (post-LD, sampled 14th-17th Sept 2020). A similar pattern was observed at urban background (UB) sites with concentrations reducing during lockdown to 96.8 ± 39.5 μg/m3 from a pre-lockdown (pre-LD) concentration of 123.2 ± 24.6 μg/m3 and then increasing to 168.6 ± 29.1 μg/m3 post-LD.
Generally, despite the decrease in NMVOC concentrations during the LD, an increase in O3 level was observed. This was attributed to decreased emissions of NOx and the subsequent repartioning of Ox. This research assessed the quantitative effect of changes in vehicular and related anthropogenic emissions on air quality, providing valuable insights for the formulation of future air pollution controls.
COVID-19 禁排带来的空气质量变化可以为了解长期减排如何影响大气成分提供有价值的见解。在英国莱斯特市,2020 年 COVID "禁排 "使大气成分发生了一些显著变化,包括非甲烷挥发性有机化合物 (NMVOC) 的浓度大幅下降(20-60%)。由于非甲烷挥发性有机化合物的排放源和生命周期各不相同,因此非甲烷挥发性有机化合物数据可以为了解行为变化如何影响大气成分提供有价值的信息。路边(RS)站点的 48 种 NMVOCs 总浓度从封锁前(2020 年 3 月 16 日至 24 日采样)的 181.3 ± 41.4 μg/m3 降至封锁期间(LD,2020 年 5 月 18 日至 21 日采样)的 82.0 ± 12.8 μg/m3,然后反弹至封锁后(LD 后,2020 年 9 月 14 日至 17 日采样)的 236.3 ± 23.9 μg/m3。城市本底(UB)站点也观察到类似的模式,在封锁期间,浓度从封锁前(LD 前)的 123.2 ± 24.6 μg/m3 降至 96.8 ± 39.5 μg/m3,然后在 LD 后升至 168.6 ± 29.1 μg/m3。这归因于氮氧化物排放量的减少以及随后氧化物的重新生成。这项研究评估了车辆和相关人为排放物的变化对空气质量的定量影响,为制定未来的空气污染控制措施提供了宝贵的见解。
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引用次数: 0
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