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Assessing the importance of nitric acid and ammonia for particle growth in the polluted boundary layer† 评估硝酸和氨对污染边界层中颗粒物生长的重要性†。
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-25 DOI: 10.1039/D3EA00001J
Ruby Marten, Mao Xiao, Mingyi Wang, Weimeng Kong, Xu-Cheng He, Dominik Stolzenburg, Joschka Pfeifer, Guillaume Marie, Dongyu S. Wang, Miriam Elser, Andrea Baccarini, Chuan Ping Lee, Antonio Amorim, Rima Baalbaki, David M. Bell, Barbara Bertozzi, Lucía Caudillo, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Martin Heinritzi, Markus Lampimäki, Katrianne Lehtipalo, Hanna E. Manninen, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Maxim Philippov, Birte Rörup, Wiebke Scholz, Jiali Shen, Yee Jun Tham, António Tomé, Andrea C. Wagner, Stefan K. Weber, Marcel Zauner-Wieczorek, Joachim Curtius, Markku Kulmala, Rainer Volkamer, Douglas R. Worsnop, Josef Dommen, Richard C. Flagan, Jasper Kirkby, Neil McPherson Donahue, Houssni Lamkaddam, Urs Baltensperger and Imad El Haddad

Aerosols formed and grown by gas-to-particle processes are a major contributor to smog and haze in megacities, despite the competition between growth and loss rates. Rapid growth rates from ammonium nitrate formation have the potential to sustain particle number in typical urban polluted conditions. This process requires supersaturation of gas-phase ammonia and nitric acid with respect to ammonium nitrate saturation ratios. Urban environments are inhomogeneous. In the troposphere, vertical mixing is fast, and aerosols may experience rapidly changing temperatures. In areas close to sources of pollution, gas-phase concentrations can also be highly variable. In this work we present results from nucleation experiments at −10 °C and 5 °C in the CLOUD chamber at CERN. We verify, using a kinetic model, how long supersaturation is likely to be sustained under urban conditions with temperature and concentration inhomogeneities, and the impact it may have on the particle size distribution. We show that rapid and strong temperature changes of 1 °C min−1 are needed to cause rapid growth of nanoparticles through ammonium nitrate formation. Furthermore, inhomogeneous emissions of ammonia in cities may also cause rapid growth of particles.

尽管生长率和损耗率之间存在竞争,但气体到颗粒过程形成和生长的气溶胶是造成大城市烟雾和灰霾的主要因素。在典型的城市污染条件下,硝酸铵形成的快速增长速率有可能维持颗粒数量。这一过程需要气相氨和硝酸相对于硝酸铵饱和比的过饱和度。城市环境是不均匀的。在对流层中,垂直混合速度很快,气溶胶可能会经历快速变化的温度。在靠近污染源的地区,气相浓度也可能变化很大。在这项工作中,我们介绍了在欧洲核子研究中心的 CLOUD 实验室中进行的-10 °C和5 °C成核实验的结果。我们利用动力学模型验证了在温度和浓度不均匀的城市条件下,过饱和可能会持续多长时间,以及过饱和对粒径分布可能产生的影响。我们的研究表明,需要 1 °C min-1 的快速而强烈的温度变化,才能通过硝酸铵的形成导致纳米颗粒的快速增长。此外,城市中氨气的不均匀排放也可能导致颗粒的快速增长。
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引用次数: 0
Enhancing spatial inference of air pollution using machine learning techniques with low-cost monitors in data-limited scenarios† 在数据有限的情况下,利用机器学习技术和低成本监测器加强空气污染的空间推断†。
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-25 DOI: 10.1039/D3EA00126A
Leonardo Y. Kamigauti, Gabriel M. P. Perez, Thomas C. M. Martin, Maria de Fatima Andrade and Prashant Kumar

Ensuring environmental justice necessitates equitable access to air quality data, particularly for vulnerable communities. However, traditional air quality data from reference monitors can be costly and challenging to interpret without in-depth knowledge of local meteorology. Low-cost monitors present an opportunity to enhance data availability in developing countries and enable the establishment of local monitoring networks. While machine learning models have shown promise in atmospheric dispersion modelling, many existing approaches rely on complementary data sources that are inaccessible in low-income areas, such as smartphone tracking and real-time traffic monitoring. This study addresses these limitations by introducing deep learning-based models for particulate matter dispersion at the neighbourhood scale. The models utilize data from low-cost monitors and widely available free datasets, delivering root mean square errors (RMSE) below 2.9 μg m−3 for PM1, PM2.5, and PM10. The sensitivity analysis shows that the most important inputs to the models were the nearby monitors' PM concentrations, boundary layer dissipation and height, and precipitation variables. The models presented different sensitivities to each road type, and an RMSE below the regional differences, evidencing the learning of the spatial dependencies. This breakthrough paves the way for applications in various vulnerable localities, significantly improving air pollution data accessibility and contributing to environmental justice. Moreover, this work sets the stage for future research endeavours in refining the models and expanding data accessibility using alternative sources.

要确保环境正义,就必须公平获取空气质量数据,尤其是对弱势社区而言。然而,来自参考监测仪的传统空气质量数据可能成本高昂,而且在没有深入了解当地气象学知识的情况下难以解读。低成本监测仪为提高发展中国家的数据可用性和建立当地监测网络提供了机会。虽然机器学习模型在大气扩散建模中大有可为,但许多现有方法依赖于低收入地区无法获得的补充数据源,如智能手机跟踪和实时交通监控。本研究通过引入基于深度学习的邻里尺度颗粒物扩散模型,解决了这些局限性。这些模型利用来自低成本监测仪和广泛可用的免费数据集的数据,使 PM1、PM2.5 和 PM10 的均方根误差(RMSE)低于 2.9 μg m-3。敏感性分析表明,对模型最重要的输入是附近监测站的 PM 浓度、边界层耗散和高度以及降水变量。模型对每种道路类型的敏感度不同,均方根误差低于区域差异,证明了对空间依赖性的学习。这一突破为在各种脆弱地区的应用铺平了道路,极大地改善了空气污染数据的可获取性,促进了环境正义。此外,这项工作还为今后利用其他来源完善模型和扩大数据可获取性的研究工作奠定了基础。
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引用次数: 0
What happens if we ‘burn all the carbon’? carbon reserves, carbon budgets, and policy options for governments† 如果我们 "烧光所有的碳 "会发生什么? 碳储备、碳预算和政府的政策选择†。
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-24 DOI: 10.1039/D3EA00107E
Kevin M. A. Parker and Michael R. Mainelli

Our estimates show that ‘proven reserves’ of fossil fuels in 2022, would generate an estimated 4777 Gt of CO2 after allowing for non-fuel uses. This quantity already could ‘bust CO2 budgets’ for IPCC RCP2.6, RCP4.5, and RCP6.0 and is approaching the range for RCP8.5. Notwithstanding these results, fossil fuel companies are still exploring and bringing new reserves onstream. We discuss the reasons behind this, and propose some policy options for governments as they address this situation.

我们的估算显示,2022 年化石燃料的 "探明储量 "在考虑非燃料用途后,估计将产生 4777 千兆吨二氧化碳。这一数量已经可以 "打破 "IPCC RCP2.6、RCP4.5 和 RCP6.0 的二氧化碳预算,并接近 RCP8.5 的范围。尽管得出了这些结果,化石燃料公司仍在勘探和开采新的储量。我们讨论了这背后的原因,并为政府应对这种情况提出了一些政策选择。
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引用次数: 0
Electrical charging of snow and ice in polar regions and the potential impact on atmospheric chemistry 极地冰雪电荷及其对大气化学的潜在影响
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-20 DOI: 10.1039/D3EA00084B
Kateryna Tkachenko and Hans-Werner Jacobi

Charging of the ice–vapor interface is a well-studied topic in ice physics and atmospheric electrification. However, these effects were not yet considered to examine chemical processes in snow in polar regions because electric potentials at ice surfaces have so far been considered insufficient to initiate chemical reactions and processes. In this review, we analyze literature data to estimate levels of electrification in snow and other frozen objects that can be caused by different processes occurring at the Earth's surface. This analysis demonstrates that threshold values of electric field strength can be exceeded for the appearance of corona discharges and even for the formation of Rayleigh jets due to combined effects of different meteorological and physical processes. The accumulation of electrical charges can lead to different chemical modifications such as electroosmotic phenomena or the accumulation of impurities from the atmosphere in growing ice crystals. Moreover, highly energetic states that occur and dissipate in microseconds as “hot spots” have the potential to initiate free radical processes and even the production of charged aerosols. The review also discusses in detail selected field observations to point out how processes driven by electrical charging may help to interpret these observations, which are at least partly inconsistent with our present understanding of snow and ice chemistry. Finally, some approaches are presented how these effects can be studied in field and laboratory experiments. A further development of this new field at the intersection of ice physics and snow chemistry seems very promising for a better understanding of relevant chemical processes related to the cryosphere.

冰-水汽界面带电是冰物理学和大气电化研究的一个重要课题。然而,在研究极地地区雪的化学过程时,尚未考虑这些效应,因为迄今为止,冰表面的电势被认为不足以引发化学反应和化学过程。在本综述中,我们分析了文献数据,以估算地球表面发生的不同过程可能导致的雪和其他冰冻物体的电化水平。分析表明,在不同气象和物理过程的共同作用下,电场强度可能会超过电晕放电的临界值,甚至会形成瑞利喷流。电荷的积累会导致不同的化学变化,如电渗现象或大气中的杂质在生长的冰晶中积累。此外,作为 "热点 "出现并在微秒内消散的高能状态有可能引发自由基过程,甚至产生带电气溶胶。综述还详细讨论了部分实地观测结果,指出电荷驱动的过程如何有助于解释这些观测结果,这些观测结果至少部分与我们目前对冰雪化学的理解不一致。最后,还介绍了在实地和实验室实验中研究这些效应的一些方法。在冰物理和雪化学的交叉领域进一步发展这一新领域,对于更好地理解与冰冻圈有关的化学过程似乎大有希望。
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引用次数: 0
Oxidative potential of fine particulate matter emitted from traditional and improved biomass cookstoves† 传统炉灶和改良生物质炉灶排放的细颗粒物的氧化潜能†。
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-18 DOI: 10.1039/D3EA00135K
Bradley H. Isenor, Jillian P. Downey, Samuel A. Whidden, Megan M. Fitzgerald and Jenny P. S. Wong

Exposure to PM2.5 emitted from traditional biomass cookstoves is a significant health risk for nearly one-third of the global population. Improved cookstoves aim to reduce pollutant emissions, but there is limited evidence of whether PM2.5 toxicity is also reduced. Using the dithiothreitol (DTT) assay to measure the potential for PM2.5 chemical components to induce oxidative stress through antioxidant depletion and/or oxidant generation, we characterized the mass- and volume-normalized DTT activity of PM2.5 emitted from a traditional three-stone fire cookstove and three improved cookstoves burning wood or charcoal fuels. Although improved cookstoves typically yield lower PM2.5 mass concentrations compared to traditional three-stone cookstove, exposure to DTT active PM2.5 is not always reduced due to increases in mass-normalized DTT activity. A notable decrease in DTT active PM2.5 exposure (by 67%) was only observed for a forced-draft improved cookstove burning wood, where low PM2.5 mass concentration offsets the increased mass-normalized DTT activity. Additionally, elemental carbon and water-soluble organic matter were identified as key predictors of volume-normalized DTT activity. Compared to wood, the use of charcoal led to a 61–86% reduction in exposure to DTT active PM2.5, owing to both lower PM2.5 mass concentration and mass-normalized DTT activity. This further supports a proposed strategy whereby biomass fuel treatment can potentially reduce household exposure to toxic PM2.5. Collectively, our findings emphasized the need to consider not only the mass concentration but also the toxic properties of PM2.5 when evaluating the health impacts of cookstoves and fuels.

接触传统生物质炉灶排放的 PM2.5 对全球近三分之一人口的健康构成重大风险。改良炉灶的目的是减少污染物排放,但关于 PM2.5 的毒性是否也会降低的证据却很有限。我们使用二硫苏糖醇(DTT)测定法来测量 PM2.5 化学成分通过抗氧化剂消耗和/或氧化剂生成而诱发氧化应激的可能性,并对传统三石火灶和三种燃烧木材或木炭燃料的改良炉灶所排放的 PM2.5 的质量和体积归一化 DTT 活性进行了表征。虽然改良炉灶产生的 PM2.5 质量浓度通常低于传统的三石炉灶,但接触到的 DTT 活性 PM2.5 并不总是因为质量归一化 DTT 活性的增加而减少。只有在燃烧木材的强制通风改良炉灶中才能观察到 DTT 活性 PM2.5 暴露的显著减少(67%),在这种炉灶中,较低的 PM2.5 质量浓度抵消了质量归一化 DTT 活性的增加。此外,碳元素和水溶性有机物也是预测体积归一化 DTT 活性的关键因素。与木材相比,由于 PM2.5 的质量浓度和质量归一化 DTT 活性较低,使用木炭可使暴露于 DTT 活性 PM2.5 的程度降低 61-86%。这进一步支持了生物质燃料处理有可能减少家庭接触有毒PM2.5的建议策略。总之,我们的研究结果强调,在评估炉灶和燃料对健康的影响时,不仅要考虑PM2.5的质量浓度,还要考虑其毒性特性。
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引用次数: 0
Correction: Emerging investigator series: aqueous oxidation of isoprene-derived organic aerosol species as a source of atmospheric formic and acetic acids 更正:新晋调查员系列:作为大气甲酸和乙酸来源的异戊二烯衍生有机气溶胶物种的水氧化作用
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-17 DOI: 10.1039/D4EA90005G
Kelvin H. Bates, Daniel J. Jacob, James D. Cope, Xin Chen, Dylan B. Millet and Tran B. Nguyen

Correction for ‘Emerging investigator series: aqueous oxidation of isoprene-derived organic aerosol species as a source of atmospheric formic and acetic acids’ by Kelvin H. Bates et al., Environ. Sci.: Atmos., 2023, 3, 1651–1664, https://doi.org/10.1039/D3EA00076A.

对 Kelvin H. Bates 等人撰写的 "新锐调查员系列:异戊二烯衍生有机气溶胶物种的水氧化作用是大气中甲酸和乙酸的来源 "的更正,Environ.Sci:Atmos., 2023, 3, 1651-1664, https://doi.org/10.1039/D3EA00076A。
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引用次数: 0
Preliminary observation of strong NOx release over Qiyi Glacier in the northeast of the Tibetan Plateau† 青藏高原东北部七一冰川氮氧化物强烈释放的初步观测†。
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-16 DOI: 10.1039/D3EA00161J
Weili Lin, Feng Wang, Chunxiang Ye and Tong Zhu

NOx is released from sunlit snowpack surfaces, and this considerably influences the oxidizing capacity of the clean boundary layer atmosphere in Antarctic and Arctic regions and the potential interpretation of the historical atmospheric composition recorded in the ice core. The Tibetan Plateau is an important snow-covered region in the northern midlatitudes, with strong solar radiation and relatively high NO3 in snow/ice. Released NOx on the glacier surface of the Tibetan Plateau should be strong. To confirm this hypothesis, field observations were performed at 4600 m above the sea level in Qiyi Glacier in late August 2004. The surface ultraviolet-B (UVB) radiation level reached >4.5 W m−2 and was increased by the strong reflection of snow/ice and clouds against the Sun and strengthened by the topographical effect. The concentrations of NO3 and NH4+ in water from melting snow were hardly detected, but the average concentration (±1σ) of NO3 in snow samples was 8.7 ± 2.7 μmol L−1. Strong correlations were observed between NOx (NO2) mixing ratios and UVB radiation levels in the Tibetan glacier. Vertical experiments revealed a negative gradient of NOx (NO2) mixing ratios from the glacier snow surface to a height of 30 cm. As a result of the high levels of UV radiation and high NO3 concentrations in snow/ice, the mixing ratios of NOx released by fresh snow in Qiyi Glacier in late August reached several parts per billion (ppbv) and were approximately one order of magnitude higher than those observed in polar regions. This observation provides direct evidence to support the research hypothesis and confirms the release of high concentrations of NOx in the boundary layer of the highland glaciers and snow surfaces.

氮氧化物从阳光照射的雪层表面释放出来,这在很大程度上影响了南极和北极地区清洁边界层大气的氧化能力,以及对冰芯中记录的历史大气成分的潜在解释。青藏高原是北半球中纬度地区重要的积雪区,太阳辐射强烈,雪/冰中的 NO3- 含量相对较高。青藏高原冰川表面释放的氮氧化物应该很强。为了证实这一假设,2004 年 8 月下旬在海拔 4600 米的七一冰川进行了实地观测。地表紫外线-B(UVB)辐射水平达到 4.5 W m-2,由于冰雪和云层对太阳的强烈反射以及地形效应,辐射水平有所提高。融化的雪水中几乎检测不到 NO3- 和 NH4+ 的浓度,但雪样中 NO3- 的平均浓度(±1σ)为 8.7 ± 2.7 μmol L-1。在西藏冰川中观察到氮氧化物(二氧化氮)混合比与紫外线辐射水平之间存在很强的相关性。垂直实验显示,从冰川雪面到 30 厘米高处,氮氧化物(二氧化氮)混合比呈负梯度。由于高水平的紫外线辐射和雪/冰中高浓度的 NO3-,8 月下旬七一冰川新雪释放的氮氧化物混合比达到十亿分之几(ppbv),比极地地区观测到的混合比高约一个数量级。这一观测结果为支持研究假设提供了直接证据,证实了高原冰川和雪面边界层释放出高浓度的氮氧化物。
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引用次数: 0
The potential environmental and climate impacts of stratospheric aerosol injection: a review† 平流层气溶胶注入对环境和气候的潜在影响:综述†
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-15 DOI: 10.1039/D3EA00134B
Han N. Huynh and V. Faye McNeill

Given the rise in global mean temperature as a direct consequence of increasing levels of greenhouse gases (GHG) in the atmosphere, a variety of climate engineering approaches, including stratospheric aerosol injection (SAI), have been proposed. Often criticized as a distraction from global efforts towards reducing GHG emissions, SAI aims to increase the Earth's albedo by seeding aerosols in the lower stratosphere. Inspired in part by observations of temporary cooling of the Earth's surface following major volcanic eruptions which introduced significant loadings of sulfate particles into the stratosphere, SAI has been explored extensively in modeling studies. The cooling effect may be accompanied by other significant consequences including stratospheric heating, stratospheric ozone (O3) depletion, and reduced global mean precipitation. In order to understand the potential environmental and climate impacts of SAI, we review the state of the knowledge regarding these issues, starting from an aerosol science perspective. We summarize aerosol radiative properties and the role they play in defining the optimal chemical and physical aerosol characteristics for SAI, and their implications for lower stratospheric warming. We then review in depth the impacts of stratospheric aerosol heterogeneous chemistry on global O3 levels. We review SAI modeling studies as well as their uncertainties, in comparison to the observed environmental and climate impacts of volcanically derived sulfate aerosols, including impacts on global temperature, stratospheric warming, and hydrological cycle. We also briefly discuss the current governance and economic considerations of the application of SAI and raise essential questions from both research and social standpoints that should be addressed before SAI is deployed for climate change mitigation.

鉴于全球平均气温上升是大气中温室气体(GHG)含量增加的直接后果,人们提出了各种气候工程方法,包括平流层气溶胶注入(SAI)。平流层气溶胶注入通常被批评为分散全球减少温室气体排放努力的注意力,其目的是通过在低平流层播撒气溶胶来增加地球的反照率。在某种程度上,SAI 的灵感来自于对大面积火山爆发后地球表面暂时冷却的观测,这些火山爆发向平流层引入了大量的硫酸盐颗粒,SAI 在建模研究中得到了广泛的探讨。降温效应可能伴随着其他重大后果,包括平流层升温、平流层臭氧(O3)耗竭和全球平均降水量减少。为了了解 SAI 对环境和气候的潜在影响,我们从气溶胶科学的角度出发,回顾了有关这些问题的知识现状。我们总结了气溶胶的辐射特性及其在确定 SAI 的最佳化学和物理气溶胶特性方面所起的作用,以及它们对低平流层变暖的影响。然后,我们深入回顾了平流层气溶胶异质化学对全球臭氧水平的影响。我们回顾了 SAI 模型研究及其不确定性,并将其与观测到的火山衍生硫酸盐气溶胶对环境和气候的影响(包括对全球气温、平流层变暖和水文循环的影响)进行对比。我们还简要讨论了当前应用 SAI 的治理和经济考虑因素,并从研究和社会角度提出了在部署 SAI 以减缓气候变化之前应解决的基本问题。
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引用次数: 0
The mobility virtual environment (MoVE): an open source framework for gathering and visualizing atmospheric observations using multiple vehicle-based sensors 移动虚拟环境(MoVE):利用多个车载传感器收集和可视化大气观测数据的开源框架
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-12 DOI: 10.1039/D2EA00106C
Marc D. Compere, Kevin A. Adkins, Avinash Muthu Krishnan, Ronny Schroeder and Curtis N. James

Uncrewed Aircraft Systems (UAS) are becoming prevalent in a wide variety of meteorological investigations. UAS fill an important atmospheric observational gap, namely observations between ground-based sensors and higher altitudes where manned aircraft can safely operate. This paper explores the hardware and software design used for a multi-vehicle atmospheric data collection campaign. The Mobility Virtual Environment (MoVE) is a software framework designed specifically to collect data from multiple vehicles and present a coherent, summary view of a complex scenario. Using both a 2D map and a live updating table, multiple vehicles can be monitored simultaneously to make real-time decisions and quickly assess the mission's effectiveness. MoVE is the software framework used to gather live telemetry inputs before, during, and after flight. MoVE is also the set of tools used to post-process multiple data logs from days of flight experiments into 3D and 4D visualizations over the surrounding terrain. The results are visualizations of otherwise invisible quantities like T, P, RH, and especially vector wind velocities, , captured during flight with drone-based sensors. The open-source software and procedures described here can help the atmospheric research, and broader scientific community, achieve greater understanding when using drone-based sensors.

无螺旋桨飞机系统(UAS)正在广泛应用于各种气象调查。无人机系统填补了一个重要的大气观测空白,即在地面传感器和有人驾驶飞机可以安全运行的更高海拔之间进行观测。本文探讨了用于多飞行器大气数据收集活动的硬件和软件设计。移动虚拟环境(MoVE)是一个软件框架,专门用于收集多飞行器的数据,并提供复杂场景的连贯、汇总视图。通过使用二维地图和实时更新表格,可以同时监测多辆飞行器,从而做出实时决策并快速评估任务的有效性。MoVE 是用于在飞行前、飞行中和飞行后收集实时遥测输入的软件框架。MoVE 也是一套工具,用于将多日飞行实验的多个数据日志后处理成周围地形的三维和四维可视化图像。其结果是在飞行过程中利用无人机传感器捕捉到的温度、湿度、相对湿度,特别是矢量风速等不可见量的可视化。这里介绍的开源软件和程序可以帮助大气研究和更广泛的科学界在使用无人机传感器时获得更深入的理解。
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引用次数: 0
Environmental Science: Atmospheres is four and so much more 环境科学:环境科学:大气是四种,还有更多
Q3 ENVIRONMENTAL SCIENCES Pub Date : 2024-01-10 DOI: 10.1039/D3EA90050A
Neil M. Donahue

A graphical abstract is available for this content

本内容有图解摘要
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引用次数: 0
期刊
Environmental science: atmospheres
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