Atmospheric Environment最新文献_第2页

The assessment of two smoke modelling systems for forecasting local air quality impacts from smouldering peat fires 评估用于预测泥炭燃烧对当地空气质量影响的两种烟雾模拟系统

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-17 DOI: 10.1016/j.atmosenv.2024.120940

Fabienne Reisen , Julie Noonan , Sean Gribben , Martin Cope , Jason Choi , Paul Torre , Darren Simon

On 17 March 2018 major grassland fires in south-west Victoria, Australia ignited several peat bogs. The peat fires smouldered for 40 days, generating substantial amounts of smoke. The surrounding communities were exposed to significant concentrations of fine particles (PM2.5), resulting in the need for active interventions (such as the relocation of schools) in order to protect vulnerable communities.

The peat fires provided a unique opportunity to review the capabilities of two air pollution forecasting models to assess the impact from the peat fires on nearby communities: the Air Quality Forecasting System (AQFx) and the Accident Reporting and Guiding Operational System (ARGOS). Both systems are used in Victoria to inform emergency management response strategies and community warnings.

A key configuration change was made to the smoke emissions module in AQFx from simulating emissions from a planned burn to a sub-surface peat fire. Emissions were derived by using heat maps generated from aerial imagery data and estimates of fuel load determined by the peat bulk density and depth of the peat.

The results indicated that AQFx successfully captured most smoke plume events during the simulation period, despite some errors in timing and magnitude. Accurate forecasting was most challenged by calm conditions, and meso-scale meteorological transition events. The ARGOS model performed better at capturing smoke plume dispersion during a meso-scale meteorological transition event due to meteorological forecasts being updated every 6 hours compared to a 24-hour update in AQFx. However, the source geometry in ARGOS meant that emission rates were concentrated within a small number of release points resulting in relatively narrow plumes with a likely overprediction of higher end PM2.5 concentrations. The AQFx system was better suited to area emissions.

The ARGOS and AQFx models showed different strengths in providing timely information to emergency response agencies to better manage smoke impacts from smouldering peat fires on communities. The ARGOS model can be set up quickly with preliminary emission estimates that can be adjusted as more accurate and updated information becomes available. Compared to the ARGOS model, AQFx is better suited for area emissions. Implementation of a rapid update cycle in AQFx would further improve forecasts especially during meteorological transition events.

2018 年 3 月 17 日，澳大利亚维多利亚州西南部的大型草原火灾引燃了多个泥炭沼泽。泥炭大火持续燃烧了 40 天，产生了大量烟雾。泥炭大火为我们提供了一个独特的机会，来审查两个空气污染预测模型的能力，以评估泥炭大火对附近社区的影响：空气质量预测系统（AQFx）和事故报告和指导操作系统（ARGOS）。AQFx 中的烟雾排放模块进行了关键配置更改，从模拟计划燃烧的排放改为模拟次表层泥炭火灾的排放。结果表明，尽管在时间和规模上存在一些误差，但 AQFx 成功捕捉到了模拟期间的大部分烟羽事件。在平静条件和中尺度气象过渡事件中，准确预报面临的挑战最大。与 AQFx 每 24 小时更新一次气象预报相比，ARGOS 模型每 6 小时更新一次气象预报，因此在中尺度气象转换事件中，ARGOS 模型在捕捉烟羽扩散方面表现更好。然而，ARGOS 中的烟源几何形状意味着排放率集中在少数几个排放点，导致烟羽相对狭窄，可能会对较高的 PM2.5 浓度预测过高。ARGOS 和 AQFx 模型在为应急响应机构提供及时信息以更好地管理泥炭燃烧产生的烟雾对社区的影响方面表现出不同的优势。ARGOS 模型可以快速建立初步排放估算，并可在获得更准确和更新的信息后进行调整。与 ARGOS 模型相比，AQFx 更适合区域排放。在 AQFx 中实施快速更新周期将进一步改进预测，尤其是在气象转换事件期间。

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引用次数: 0

Enhancing Uncrewed Aerial Vehicle Techniques for Monitoring Greenhouse Gas Plumes at Point Sources 加强无螺旋桨飞行器技术以监测点源温室气体羽流

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-16 DOI: 10.1016/j.atmosenv.2024.120924

Horim Kim , Keun Taek Kim , Sangjae Jeong , Young Su Lee , Xin Zhao , Jae Young Kim

The urgency of the global climate crisis necessitates advanced monitoring of greenhouse gases, with an emphasis on capturing their spatial and temporal variability. This study explores techniques to enhance plume detection and concentration measurements using uncrewed aerial vehicles (UAVs) for monitoring at point sources, specifically at an incineration stack. Through preliminary site investigations, our approach employed strategically designed flight paths and an autopilot system to optimize flight operations within the constraints of limited flight time due to battery capacity. We combined a UAV-mounted anemometer with a plume rise model to localize the plume center at a distance of 30 m from the stack center and evaluated its performance by comparing the model-based estimations at different altitudes and angular directions with the observation results. The comparison demonstrated that the results obtained by localizing the plume center using a plume rise model and a UAV-mounted anemometer aligned well with observations based on CO₂ concentration analysis. The comparative analysis showed a RMSE of 8.44 m and a MAE of 7.26 m for altitude, and a RMSE of 32.31

^{\circ}

and a MAE of 25.78

^{\circ}

for angular direction. Furthermore, we assessed the effectiveness of hovering UAV flights, in which a UAV remains stationary at a fixed point in the air, compared to non-hovering flights in capturing pollutant concentration. While both methods performed similarly in detecting the plume center, non-hovering flights underestimated the CO₂ concentration due to insufficient time for measurement despite a sensor response time of less than three seconds. Overall, our proposed hybrid monitoring strategy integrates non-hovering and hovering flights, enhancing both plume detection efficiency and concentration measurement accuracy at point sources.

全球气候危机的紧迫性要求对温室气体进行先进的监测，重点是捕捉其空间和时间变化。本研究探讨了利用无人驾驶飞行器（UAVs）加强羽流探测和浓度测量的技术，以监测点源，特别是焚烧烟囱。通过初步现场调查，我们的方法采用了战略性设计的飞行路径和自动驾驶系统，以便在电池容量导致飞行时间有限的限制条件下优化飞行操作。我们将无人飞行器安装的风速计与烟羽上升模型相结合，在距离烟囱中心 30 米处定位烟羽中心，并通过比较不同高度和角度方向上基于模型的估算结果与观测结果，对其性能进行评估。比较结果表明，使用烟羽上升模型和无人机安装的风速计定位烟羽中心所获得的结果与基于二氧化碳浓度分析的观测结果非常吻合。对比分析表明，高度的均方根误差为 8.44 米，最大误差为 7.26 米；角度方向的均方根误差为 32.31∘，最大误差为 25.78∘。此外，我们还评估了无人机悬停飞行与非悬停飞行在捕捉污染物浓度方面的效果，在悬停飞行中，无人机会静止在空中的一个固定点上。虽然这两种方法在检测烟羽中心方面表现相似，但非悬停飞行低估了二氧化碳浓度，原因是测量时间不足，尽管传感器的响应时间不到三秒。总之，我们提出的混合监测策略整合了非悬停和悬停飞行，提高了点源的羽流探测效率和浓度测量精度。

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引用次数: 0

Effect of ambient ozone and its interactions with ambient PM2.5 and temperature on peak expiratory flow in adults with asthma 环境臭氧及其与环境 PM2.5 和温度的相互作用对成人哮喘患者呼气流量峰值的影响

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-16 DOI: 10.1016/j.atmosenv.2024.120939

Dongxia Jiang , Ying Shang , Zhengxiong Li , Xianlin Mu , Xuehu Han , Xinzhuo Xie , Guanglong Fu , Yunshu Zhang , Shaodan Huang , Chun Chang

Numerous studies have linked air pollution to asthma. However, limited information exists on the effect of ambient ozone (O₃), or its interactions with fine particulate matter (PM_2.5) or temperature on peak expiratory flow (PEF) of in asthmatic adults. We conducted a longitudinal study including 99 adult asthma patients and documenting 7153 person-days PEF records. Utilizing linear mixed-effect and distributed non-linear models, we investigated the associations between ambient O₃ exposures over lag0-14 days with morning and evening PEF, as well as diurnal PEF variability. Findings revealed significant associations between ambient O₃ exposure with reduced morning and evening PEF, with varied associations for exposures across different lag days. Specifically, the most pronounced association with morning PEF was found for exposure at lag4, with a change of −0.211 (95%CI: −0.360, −0.062) L/min per 10 μg/m³ increase; for evening PEF, the strongest association was observed for exposure at lag0, with a change of −0.379 (95%CI: −0.721, −0.037) L/min per 10 μg/m³ increase. However, no significant association between O₃ and diurnal PEF variability was found. Furthermore, we observed significant interactions between O₃ and PM_2.5 exposures from lag6 to lag9 on morning and evening PEF, and significant interactions between O₃ and temperature from lag1 to lag11 on morning PEF and from lag0 to lag11 on evening PEF. Stronger associations between O₃ and PEF were observed in males, those aged over 40 years, overweight individuals, smokers and those with non-allergic asthma. These results underscore considering combined pollution and climate impacts in asthma management and supporting policies.

大量研究表明，空气污染与哮喘有关。然而，有关环境臭氧（O3）或其与细颗粒物（PM2.5）或温度的相互作用对成人哮喘患者呼气流量峰值（PEF）的影响的信息却很有限。我们进行了一项纵向研究，研究对象包括 99 名成人哮喘患者，记录了 7153 人天的 PEF。利用线性混合效应和分布式非线性模型，我们研究了滞后 0-14 天的环境 O3 暴露与早晚 PEF 之间的关系，以及 PEF 的昼夜变化。研究结果表明，暴露于环境中的臭氧与早晚血压下降之间存在明显的联系，不同滞后天数的暴露量之间存在不同的联系。具体来说，滞后 4 天的暴露量与早晨 PEF 的关系最为明显，每增加 10 μg/m3 的变化为-0.211（95%CI：-0.360，-0.062）升/分钟；对于晚间 PEF，滞后 0 天的暴露量与之关系最为密切，每增加 10 μg/m3 的变化为-0.379（95%CI：-0.721，-0.037）升/分钟。然而，我们没有发现臭氧与昼夜肺活量变异性之间有明显的关联。此外，我们还观察到，从滞后期6到滞后期9，O3和PM2.5暴露对早晨和傍晚的PEF有明显的交互作用；从滞后期1到滞后期11，O3和温度对早晨的PEF有明显的交互作用；从滞后期0到滞后期11，O3和温度对傍晚的PEF有明显的交互作用。在男性、40 岁以上者、超重者、吸烟者和非过敏性哮喘患者中，观察到 O3 与 PEF 之间的关联性更强。这些结果表明，在哮喘管理和支持政策中应考虑污染和气候的综合影响。

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引用次数: 0

Fragrance, volatile organic compound, and particulate matter emissions from incense burning: Observations and risk assessments for household rooms and temples in Japan 焚香产生的香气、挥发性有机化合物和微粒物质排放：对日本家庭房间和寺庙的观察和风险评估

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-14 DOI: 10.1016/j.atmosenv.2024.120930

Saria Hoshino , Kazushi Noro , Qi Wang , Takashi Amagai

In Japanese society, incense is often burned indoors for its fragrance and as a part of Buddhist rituals. However, fragrances and volatile organic compounds (VOCs) emitted by incense burning can adversely affect human health. Japanese products are not required to disclose fragrances included; therefore, the number of these compounds to which users are exposed is unclear. This study aimed to evaluate the human health risks associated with incense burning in household rooms and temples. Chamber tests demonstrated that incense sticks used in the home contained higher concentrations of fragrance than those used in temples. Consequently, the level of fragrance contained in smoke from incense used in the home (1,100–9,200 μg stick⁻¹) was greater than that from temple incense smoke (15–84 μg stick⁻¹). The concentration of VOCs derived from the pyrolysis of incense ranged from 840 to 2,900 μg stick⁻¹, which was higher than the fragrance emission concentrations. Field observations in three temples and four rooms revealed that incense burning during memorial services presented a benzene cancer risk of 3.7–5.2 × 10⁻⁶ for monks. The seating position of the monk should be at least 11 m from the incense to reduce the cancer risk of benzene to a value below 1 × 10⁻⁶.

在日本社会，人们经常在室内焚香，以获取香味，并将其作为佛教仪式的一部分。然而，焚香时散发出的香味和挥发性有机化合物（VOC）会对人体健康产生不利影响。日本的产品并不要求公开所含的香料，因此，使用者接触到的这些化合物的数量并不清楚。这项研究旨在评估在家庭房间和寺庙中焚香对人体健康造成的风险。室温测试表明，家庭中使用的香棒比寺庙中使用的香棒含有更高浓度的香料。因此，家用香烟所含的香味水平（1,100-9,200 微克香棒-1）高于寺庙香烟所含的香味水平（15-84 微克香棒-1）。沉香热解产生的挥发性有机化合物的浓度范围为 840 至 2,900 微克/支-1，高于香味排放浓度。对三座寺庙和四间房的实地观察表明，僧侣在追悼会上焚香引发苯癌的风险为 3.7-5.2 × 10-6。僧侣的坐姿应距离香炉至少 11 米，才能将苯的致癌风险降至 1 × 10-6 以下。

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引用次数: 0

137Cs in outdoor air due to Chernobyl-contaminated wood combustion for residential heating in Thessaloniki, North Greece 希腊北部塞萨洛尼基因居民取暖燃烧受切尔诺贝利污染的木材而导致室外空气中的 137Cs

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-13 DOI: 10.1016/j.atmosenv.2024.120929

S. Stoulos , E. Ioannidou , P. Koseoglou , E. Vagena , A. Ioannidou

Wood combustion was the key heating source in Greece during the first years at the beginning of the financial crisis. Signals of ¹³⁷Cs were detected in Thessaloniki during the winter of 2013–2014 on weekends and holidays when the residents were at home burning the biggest amount of wood all day. ¹³⁷Cs signals were >6–21 μBq m⁻³ detected using high-volume air filters and γ-spectrometry. No signals have been detected since then, as gas has replaced oil for residential heating, reducing forest wood. Besides, signal <6 μBq m⁻³ is undetectable because this is the minimum detectable activity. ⁴⁰K concentrations were also measured, revealing a constant value of 143 ± 16 μBq m⁻³. The Cs-to-K ratio in air was 0.04–0.14 compared to 0.05 ± 0.01 measured before and after. Higher levels were measured when the air temperature was the lowest, but no correlation was observed with wind or pressure. Simulations using the HYSLIT model were applied on the dates on which the ratio was the highest. The model confirms the experimental results observed. ¹³⁷Cs signals detected and related to the Chernobyl-contaminated biomass used for central heating indicate that contaminated forest ecosystems remain a source of unwanted radioactivity in the environment.

在金融危机爆发的最初几年，木材燃烧是希腊的主要供暖来源。塞萨洛尼基在 2013-2014 年冬季的周末和节假日检测到了 137Cs 信号，当时居民整天都在家燃烧大量木材。使用高容量空气过滤器和 γ 光谱仪检测到的 137Cs 信号为 6-21 μBq m-3。此后，由于天然气已取代石油用于居民取暖，减少了森林木材，因此没有再检测到任何信号。此外，6 μBq m-3 信号是检测不到的，因为这是最低检测活性。对 40K 浓度也进行了测量，结果显示其恒定值为 143 ± 16 μBq m-3。空气中的铯-钾比率为 0.04-0.14，而前后测得的比率为 0.05 ± 0.01。气温最低时测得的浓度水平较高，但与风力或气压没有相关性。使用 HYSLIT 模型对比率最高的日期进行了模拟。该模型证实了观察到的实验结果。检测到的 137Cs 信号与用于集中供暖的切尔诺贝利污染生物质有关，这表明受污染的森林生态系统仍然是环境中不必要的放射性来源。

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引用次数: 0

Exploring fine-aerosol episodes in urban Seoul during the cold season of the 2021 SIJAQ campaign: Measurement evidences of heterogeneous reactions on black carbon particles 探索 2021 年 SIJAQ 活动寒冷季节首尔市区的细微气溶胶事件：黑碳颗粒异质反应的测量证据

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-13 DOI: 10.1016/j.atmosenv.2024.120926

Saehee Lim , Min-Suk Bae , Jihi Jang , Anubhav Kumar Dwivedi , Junsu Gil , Joo ae Kim , Meehye Lee , Sea-Ho Oh , Sun-A Shin , Lim-Seok Chang

Significant PM_2.5 pollution has been prevalent on a regional scale in East Asia including a megacity Seoul in South Korea. Here, we explore fine-aerosol episodes occurred in Seoul during the Satellite Integrated Joint monitoring of Air Quality (SIJAQ) campaign from October to November of the 2021, focusing on experimental evidences of heterogeneous reactions to form secondary aerosol under a highly oxidized atmospheric condition.

At this urban site in Seoul, vehicle exhaust was the clear source of fresh emissions, leading to a high level of NO and small refractory black carbon (rBC) particles (mass median diameter of 162 nm ± 16 nm) in the morning time. The hourly mass concentration of PM_2.5 ranged from 5.3 μg m⁻³ to 146.1 μg m⁻³, averaging at 24.5 ± 22.2 μg m⁻³. During the campaign, the most intense episode, EP3 (November 18–21), recorded an average PM_2.5 concentration of 72.5 ± 38.2 μg m⁻³, peaking at 146.1 μg m⁻³, was characterized by relatively higher temperature (∼12 °C) and relative humidity (67 %) on average thoroughly governed by continental migratory high and westerly winds. While the average NO₃⁻ concentration was 27.7 μg m⁻³, four times the whole campaign's average, EP3 was highlighted by a high morning NO₂/NO_x ratio and significantly elevated daytime and nighttime O_x (O₃+NO₂) concentrations compared to non-episode days. Throughout the entire campaign, NO_z surrogate (NO_2(CL)-NO_2(T)), O_x, and F_{moderate + thick} (the combined number fractions of moderately and thickly coated-rBC particles) tended to increase with the PM_2.5 concentration. During the daytime, as PM_2.5 increased, F_{moderate + thick} showed a monotonic increase, accompanied by RH rising from 54 ± 16% to 63 ± 11%. In contrast, at nighttime of humid condition with RH often exceeding 70% the enhancement of F_{moderate + thick} was more sensitive to condensable gas levels than RH. Given that high levels of PM_2.5 (>60 μg m⁻³) were observed only during EP3, enhanced levels of NO_z surrogate, O_x, F_{moderate + thick,} and RH were evident characteristics of EP3. Such chemical and meteorological conditions suggest that the chemically enhanced oxidation state was evident during EP3, which promoted the formation of secondary aerosols on primary particles including rBC, especially under conditions of elevated RH. Considering the recent trend of increasing number of vehicles and rising atmospheric O₃ concentrations in East Asia, future studies should be well designed to investigate the detailed mechanisms involved in heterogeneous reactions that lead to the formation of secondary aerosols.

包括韩国特大城市首尔在内的东亚地区普遍存在严重的 PM2.5 污染。在此，我们探讨了 2021 年 10 月至 11 月空气质量卫星综合联合监测（SIJAQ）活动期间首尔发生的微细气溶胶事件，重点是在高度氧化的大气条件下异质反应形成二次气溶胶的实验证据。在首尔的这个城市站点，汽车尾气是明显的新鲜排放源，导致早晨出现大量氮氧化物和小难熔黑碳（rBC）颗粒（质量中值直径为 162 nm ± 16 nm）。PM2.5 的每小时质量浓度从 5.3 μg m-3 到 146.1 μg m-3 不等，平均为 24.5 ± 22.2 μg m-3。在这次活动中，强度最大的 EP3 阶段（11 月 18-21 日）的 PM2.5 平均浓度为 72.5 ± 38.2 μg m-3，峰值为 146.1 μg m-3，受大陆性偏高和西风的影响，平均温度（12 °C）和相对湿度（67%）相对较高。虽然 NO3- 的平均浓度为 27.7 μg m-3，是整个活动平均值的四倍，但与非活动日相比，EP3 的突出特点是早晨 NO2/NOx 比率较高，白天和夜间 Ox（O3+NO2）浓度显著升高。在整个活动期间，NOz 代用值（NO2(CL)-NO2(T)）、Ox 和 Fmoderate + thick（中等和较厚包覆-红细胞颗粒的综合数量分数）趋向于随 PM2.5 浓度的增加而增加。在白天，随着 PM2.5 的增加，Fmoderate + thick 呈单调增加，同时相对湿度从 54 ± 16% 上升到 63 ± 11%。相反，在夜间潮湿的条件下，相对湿度往往超过 70%，中浓氨的增强对可凝性气体水平比相对湿度更敏感。鉴于只有在 EP3 期间才观测到高水平的 PM2.5（60 μg m-3），NOz 替代物、Ox、Fmoderate + thick 和相对湿度水平的增强是 EP3 的明显特征。这些化学和气象条件表明，在 EP3 期间，化学氧化状态明显增强，这促进了包括 rBC 在内的初级粒子上二次气溶胶的形成，尤其是在相对湿度升高的条件下。考虑到近来东亚地区车辆数量增加和大气中臭氧浓度上升的趋势，未来的研究应精心设计，以调查导致二次气溶胶形成的异质反应的详细机制。

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引用次数: 0

Pollution status, phase partitioning, potential sources, and health impacts of polybrominated diphenyl ethers in Hangzhou offices 杭州办公室多溴联苯醚的污染状况、相分配、潜在来源和对健康的影响

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-13 DOI: 10.1016/j.atmosenv.2024.120906

Mantong Jin, Jingjing Guo, Ziyu Xu, Liwei Sun, Shunfei Zhang

Polybrominated diphenyl ethers (PBDEs) have persistence and toxicities, so exposure to PBDEs is associated with various health hazards. Thus, it is crucial to study the pollution status of PBDEs in office microenvironments, which are the primary active places for people working in offices. We collected 80 samples (air, particulate matter, and dust) from 10 offices in Hangzhou and detected the congeners of PBDEs using GC-ECD. Median concentrations of total PBDEs in particle phase, gas phase, and dust were 108.28 pg/m³, 35.63 pg/m³ and 59.22 ng/g, respectively. BDE-209 was the primary congener in various media. The particle size distribution was bimodal and was primarily distributed in the ＜1.1 and > 7 μm particle size segment. We predicted the concentration of PBDEs in different phases to better explore the fate of released PBDEs. The measured value of the equilibrium coefficient between gas and dust indicated that PDBEs in the gas-phase were transferred into the dust. The predicted

C_{g - p r e}

value of PBDEs was smaller than the measured value

C_{g}

, especially BDE-209. The measured concentration of low-brominated PBDEs in particles was higher than the predicted concentration, which may be because the non-equilibrium model did not consider the dry and wet deposition of particles. The PBDE concentrations in the materials were in the following order: mouse pad < cable shell < plastic folder < eco-board. The analysis of indoor sources of PBDEs demonstrated that plastic folders, eco-boards, and mouse pads and cable shells may be potential sources of PBDEs in the air, dust, and particles, respectively. The HQ of PBDEs in Hangzhou offices was far less than 1, indicating that the health risk was within the acceptable range.

多溴联苯醚具有持久性和毒性，因此接触多溴联苯醚会对健康造成各种危害。因此，研究办公室微环境中多溴联苯醚的污染状况至关重要，因为办公室是人们工作的主要活动场所。我们从杭州的 10 家办公室采集了 80 份样本（空气、颗粒物和粉尘），并使用气相色谱-电化学方法检测了多溴联苯醚的同系物。颗粒物、气相和粉尘中多溴联苯醚总浓度的中位数分别为 108.28 皮克/立方米、35.63 皮克/立方米和 59.22 纳克/克。BDE-209 是各种介质中的主要同系物。粒径分布呈双峰型，主要分布在＜1.1 和 > 7 μm 粒径段。我们预测了多溴联苯醚在不同相中的浓度，以便更好地探索释放出的多溴联苯醚的归宿。气体和粉尘之间平衡系数的测量值表明，气相中的多溴联苯醚被转移到了粉尘中。多溴联苯醚的预测 Cg-pre 值小于实测值 Cg，尤其是 BDE-209。颗粒中低溴多溴联苯醚的实测浓度高于预测浓度，这可能是因为非平衡模型没有考虑颗粒的干湿沉降。材料中的多溴联苯醚浓度依次为：鼠标垫；电缆外壳；塑料文件夹；环保板。对室内多溴联苯醚来源的分析表明，塑料文件夹、环保板、鼠标垫和电缆外壳可能分别是空气、灰尘和微粒中多溴联苯醚的潜在来源。杭州办公室多溴联苯醚的 HQ 值远小于 1，表明其健康风险在可接受范围之内。

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引用次数: 0

Aerosol retrievals derived from a low-cost Calitoo sun-photometer taken on board a research vessel 研究船上使用的低成本 Calitoo 太阳光度计得出的气溶胶检索结果

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-12 DOI: 10.1016/j.atmosenv.2024.120888

Rosa D. García , África Barreto , Celia Rey , Eugenio Fraile-Nuez , Alba González-Vega , Sergio F. León-Luis , Antonio Alcantara , A. Fernando Almansa , Carmen Guirado-Fuentes , Pablo González-Sicilia , Victoria E. Cachorro , Frederic Bouchar

This study presents a comprehensive 5-year period assessment of aerosol optical depth (AOD) and Å ngströn Exponent (AE) data from a hand-held Calitoo sun photometer on board the Ángeles Alvariño research vessel. Observations spanned March 2018 to September 2023, focusing on key maritime regions such as the Canary Islands, coasts of North Africa, the Mediterranean, Portugal, the Cantabrian, and the Bay of Biscay. The Calitoo device measures solar irradiance at three wavelengths (465, 540, and 619 nm). Uncertainty analysis for Calitoo AOD retrievals was performed using the Monte Carlo method, yielding an expanded uncertainty (U

{_{A}_{O}}_{D}

) ranging between 0.008 and 0.050 with a mean and standard deviation of 0.032 ± 0.008 for the three wavelengths. Our results also highlight the remarkable calibration stability of the Calitoo (

<

2.6%) over this 5-year period. Calitoo AOD values were assessed using reference AOD data from Santa Cruz de Tenerife (the Canary Islands), El Arenosillo (Huelva), and Palma de Mallorca (the Balearic Islands) AERONET (Aerosol Robotic Network) stations. The comparison revealed a good agreement with correlation coefficients ranging from 0.727 to 0.917 and mean bias ranging from -0.030 to -0.001. Additionally, the Calitoo AOD data were compared with MODIS (Moderate Resolution Imaging Spectroradiometer) and CAMS-ECMWF (Copernicus Atmosphere Monitoring Service-European Centre for Medium-Range Weather Forecasts) aerosol products obtaining that Calitoo AOD values were generally lower, showing negative mean bias of -0.063 and -0.024, respectively.

The aerosol characterizations using AE vs. AOD plots in the three maritime study regions using 5-years of non-routine Calitoo data are similar to the corresponding aerosol characterizations performed with simultaneous AERONET-Cimel data.

These findings underscore Calitoo’s reliability for aerosol studies in regions where AERONET instruments or other aerosol networks are unavailable. Likewise, given the low cost of Calitoo photometers, they could be deployed onboard a large number of merchant and passenger ships or in other remote or under-monitored areas, providing near real-time AOD/AE data to enhance our understanding of aerosols processes or for model or satellite assimilation/validation.

本研究对安赫尔斯-阿尔瓦里尼奥号研究船上的手持式 Calitoo 太阳光度计提供的气溶胶光学深度（AOD）和 Å ngströn 指数（AE）数据进行了为期 5 年的综合评估。观测时间跨度为 2018 年 3 月至 2023 年 9 月，重点是加那利群岛、北非海岸、地中海、葡萄牙、坎塔布连和比斯开湾等主要海洋区域。Calitoo 设备可测量三种波长（465、540 和 619 纳米）的太阳辐照度。使用蒙特卡洛方法对 Calitoo AOD 数据进行了不确定性分析，得出三个波长的扩展不确定性（UAOD）在 0.008 和 0.050 之间，平均值和标准偏差为 0.032 ± 0.008。我们的结果还突显了 Calitoo 在这 5 年中出色的校准稳定性（2.6%）。利用圣克鲁斯-德特内里费（加那利群岛）、埃尔阿雷诺西约（韦尔瓦）和帕尔马-德马略卡（巴利阿里群岛）AERONET（气溶胶机器人网络）站的参考气溶胶数据，对 Calitoo 的 AOD 值进行了评估。比较结果表明，两者的相关系数在 0.727 至 0.917 之间，平均偏差在-0.030 至-0.001 之间，具有良好的一致性。此外，将 Calitoo 的 AOD 数据与 MODIS（中分辨率成像分光仪）和 CAMS-ECMWF （哥白尼大气监测服务-欧洲中期天气预报中心）的气溶胶产品进行比较后发现，Calitoo 的 AOD 值普遍较低，平均偏差分别为-0.063 和-0.024。在三个海洋研究区域，使用 Calitoo 5 年非例行数据绘制的 AE vs. AOD 图进行的气溶胶特征描述与使用 AERONET-Cimel 同步数据进行的相应气溶胶特征描述相似。同样，鉴于 Calitoo 光度计的低成本，可以将其部署在大量商船和客船上或其他偏远或监测不足的地区，提供近乎实时的 AOD/AE 数据，以加深我们对气溶胶过程的了解，或用于模型或卫星同化/验证。

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引用次数: 0

Reaction between peracetic acid and carbonyl oxide: Quantitative kinetics and insight into implications in the atmosphere 过乙酸与羰基氧化物之间的反应：定量动力学和对大气中影响的见解

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-12 DOI: 10.1016/j.atmosenv.2024.120928

Chao-Lu Xie , Hao Yang , Bo Long

Peracetic acid (PAA, CH₃C(O)OOH) is one of the most abundant organic peroxyacid in the atmosphere. PAA is often assumed to be removed by hydroxyl radical in the gas phase of troposphere, but its reaction rate is quite low. Here, we investigated the new reaction between PAA and carbonyl oxide (CH₂OO) by using quantum chemical methods, reaction kinetics in combination with atmospheric modeling. We first performed W3X-L calculations close to CCSDT(Q)/CBS accuracy with the reaction systems containing eight carbon and oxygen atoms. The present findings show that the post-CCSD(T) contribution is about 0.50 kcal/mol, which is important for obtaining quantitative relative enthalpy of activation at 0 K. We find that the recrossing effect reduces the rate constant by an order of magnitude for the mechanism of the hydrogen-shift coupled carbon-oxygen addition at low temperature. The calculated results reveal that the anharmonicity increases the rate constants of CH₂OO + CH₃C(O)OOH by a factor of 6.27 at 298 K. The present findings uncover that the PAA + CH₂OO reaction is a dominant pathway for PAA sinks in the gas phase of troposphere at the lower nighttime OH concentrations at 298 K, since the rate of PAA + CH₂OO is even an order of magnitude higher than the rate of the PAA + OH reaction. Moreover, atmospheric modeling simulations unveil that CH₂OO can make certain contribution to the reduction of PAA in the Amazon.

过乙酸（PAA，CH3C(O)OOH）是大气中含量最高的有机过氧酸之一。人们通常认为 PAA 在对流层气相中会被羟基自由基清除，但其反应速率相当低。在此，我们采用量子化学方法、反应动力学和大气模型相结合的方法研究了 PAA 和羰基氧化物（CH2OO）之间的新反应。我们首先对含有八个碳原子和氧原子的反应体系进行了接近 CCSDT(Q)/CBS 精确度的 W3X-L 计算。本研究结果表明，CCSD(T) 后贡献约为 0.50 kcal/mol，这对于获得 0 K 时的定量相对活化焓非常重要。我们发现，对于低温下氢移耦合碳氧加成的机理而言，交叉效应将速率常数降低了一个数量级。计算结果显示，在 298 K 时，非谐波使 CH2OO + CH3C(O)OOH 的速率常数增加了 6.27 倍。本研究结果发现，在 298 K 的较低夜间 OH 浓度条件下，PAA + CH2OO 反应是对流层气相中 PAA 吸收的主要途径，因为 PAA + CH2OO 的速率甚至比 PAA + OH 反应的速率高出一个数量级。此外，大气模型模拟显示，CH2OO 对亚马逊河流域 PAA 的减少有一定的贡献。

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引用次数: 0

Development of an online cloud fog monitor: Design, laboratory, and field deployment at an unoccupied coastal site in Eastern China 开发在线云雾监测仪：设计、实验室和在中国东部沿海无人区的实地部署

IF 4.2 2区环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES

Atmospheric Environment

Pub Date : 2024-11-12 DOI: 10.1016/j.atmosenv.2024.120927

Ping Du , Xinghui Liu , Xiaoling Nie , Tao Li , Haoran He , Jianing Zhang , Xinfeng Wang , Yan Wang , Jianmin Chen

Online detection of cloud water chemistry is a pressing issue in atmospheric outfield observation, with online detection modules representing a significant development direction for cloud water observation. Addressing the common problem of time-delayed errors in manual detection, particularly in the context of cloud water acidity, has remained challenging, with limited understanding and effective solutions available. We developed an Online Cloud Fog Monitor (OCFM) featuring automatic pH and electrical conductivity (EC) detection capabilities, and conducted comprehensive laboratory and field tests. The OCFM utilizes a peristaltic pump, water pipe, and diversion chamber to direct cloud samples to distinct detection chambers, enabling real-time analysis. The diversion chamber is equipped with dual liquid level sensors to segregate and preserve samples once the volume exceeds a predetermined threshold. Calibration results indicate that the instrument's background metal elements do not affect cloud water analysis, and detection occurs within the designed response time. Field tests demonstrate that the OCFM can collect over 50 ml of cloud water, with a response accuracy exceeding 63.6%, though influenced by meteorological conditions. The time-delay error for pH was notably larger than for EC. Comparative analysis with the Caltech Active Strand Cloudwater Collector (CASCC) revealed that the OCFM's sampling process does not introduce errors, and the online detection accuracy of pH and EC is comparable to manual methods. Additionally, water-soluble ions in samples collected by the OCFM showed no significant differences compared to those collected by CASCC. Overall, the OCFM effectively replaces manual testing, mitigating time-delay errors in chemical property testing. The introduction of this cloud water detector promises to significantly reduce labor costs and economic consumption associated with cloud water observation, thereby facilitating long-term, multi-site observation of cloud water chemistry.

云水化学在线探测是大气外场观测中的一个紧迫问题，在线探测模块是云水观测的一个重要发展方向。解决人工检测中常见的延时误差问题，尤其是云水酸度方面的问题，仍然具有挑战性，人们对这一问题的理解和有效解决方案都很有限。我们开发了一种在线云雾监测仪（OCFM），具有自动 pH 值和导电率（EC）检测功能，并进行了全面的实验室和实地测试。OCFM 利用蠕动泵、水管和分流室将云雾样本导入不同的检测室，从而实现实时分析。分流室配备了双液面传感器，一旦体积超过预定阈值，就会隔离并保存样本。校准结果表明，仪器的本底金属元素不会影响云水分析，检测也在设计的响应时间内完成。现场测试表明，OCFM 可以采集 50 毫升以上的云水，响应精度超过 63.6%，但会受到气象条件的影响。pH 值的延时误差明显大于 EC 值。与加州理工学院主动式云水采集器（CASCC）的比较分析表明，OCFM 的采样过程不会产生误差，pH 值和 EC 值的在线检测精度与人工方法相当。此外，OCFM 采集的样本中的水溶性离子与 CASCC 采集的样本相比没有明显差异。总之，OCFM 能有效取代人工检测，减少化学性质检测中的时间延迟误差。这种云水检测器的引入有望大幅降低与云水观测相关的人工成本和经济消耗，从而促进对云水化学的长期、多站点观测。

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引用次数: 0