Atmospheric OH reactivity in the western United States determined from comprehensive gas-phase measurements during WE-CAN
Atmospheric OH reactivity in the western United States determined from comprehensive gas-phase measurements during WE-CAN
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美国西部大气 OH 反应性通过 WE-CAN 期间的综合气相测量确定
DOI：
10.1039/d2ea00063f
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Apel, Eric C.
中科院分区：
文献类型：
--
作者：
Permar, Wade;Jin, Lixu;Peng, Qiaoyun;O'Dell, Katelyn;Lill, Emily;Selimovic, Vanessa;Yokelson, Robert J.;Hornbrook, Rebecca S.;Hills, Alan J.;Apel, Eric C.
野火烟雾含有许多不同的活性有机气体，其中许多只是最近才被确定和量化。因此，它们作为氧化剂汇的相对重要性受到很大限制，导致在全球化学传输模型（CTM）和明确的化学机制中的代表性不完整。利用西部野火云化学实验，气溶胶吸收和氮（WE-CAN）飞机活动期间进行的160个气相测量，我们计算了美国西部野火排放，烟雾年龄>3天，烟雾影响和低/无烟雾影响的城市大气以及清洁的自由对流层的OH反应性（OHR）。在野火排放量中，VOC占计算OHR总量的80%以上，目前在常用的GEOS-Chem CTM中，至少有一半的现场VOC OHR未用于生物质燃烧（BB）排放。为了提高OHR的代表性，我们建议CTM为BB实施含呋喃的物质、丁二烯和单萜。主化学机制（MCM）被发现占88%的挥发性有机化合物OHR在野火排放量，并捕捉其观察到的衰减在老化的头几个小时，表明大多数已知的挥发性有机化合物OH汇包括在明确的机制。我们发现，BB烟雾提高了平均总OHR的53%，相对于低/无烟雾的城市背景，主要是由于挥发性有机化合物和CO的增加，从而促进城市臭氧的产生。这项工作突出了白天BB烟羽氧化最重要的VOC种类，并提供了一个路线图，其中物种应优先在下一代CTM，以更好地预测下风向空气质量和BB烟对健康的影响。
Wildfire smoke contains numerous different reactive organic gases, many of which have only recently been identified and quantified. Consequently, their relative importance as an oxidant sink is poorly constrained, resulting in incomplete representation in both global chemical transport models (CTMs) and explicit chemical mechanisms. Leveraging 160 gas-phase measurements made during the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) aircraft campaign, we calculate OH reactivities (OHRs) for western U.S. wildfire emissions, smoke aged >3 days, smoke-impacted and low/no smoke-impacted urban atmospheres, and the clean free troposphere. VOCs were found to account for ∼80% of the total calculated OHR in wildfire emissions, with at least half of the field VOC OHR not currently implemented for biomass burning (BB) emissions in the commonly used GEOS-Chem CTM. To improve the representation of OHR, we recommend CTMs implement furan-containing species, butadienes, and monoterpenes for BB. The Master Chemical Mechanism (MCM) was found to account for 88% of VOC OHR in wildfire emissions and captures its observed decay in the first few hours of aging, indicating that most known VOC OH sinks are included in the explicit mechanisms. We find BB smoke enhanced the average total OHR by 53% relative to the low/no smoke urban background, mainly due to the increase in VOCs and CO thus promoting urban ozone production. This work highlights the most important VOC species for daytime BB plume oxidation and provides a roadmap for which species should be prioritized in next-generation CTMs to better predict the downwind air quality and health impacts of BB smoke.
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基于 WE-CAN 飞机测量的美国西部野火痕量有机气体排放
DOI：
10.1029/2020jd033838
发表时间：
2021
期刊：
Journal of Geophysical Research: Atmospheres
影响因子：
--
作者：
Permar, Wade;Wang, Qian;Selimovic, Vanessa;Wielgasz, Catherine;Yokelson, Robert J.;Hornbrook, Rebecca S.;Hills, Alan J.;Apel, Eric C.;Ku, I‐Ting;Zhou, Yong
通讯作者：
Zhou, Yong
行星边界层中总 VOC 反应性 2. 确定臭氧产生对 VOC 和 NO x 敏感性的新指标
影响因子：
--
作者：
Frank Kirchner;F. Jeanneret;A. Clappier;Bernd Krüger;Hubert van den Bergh;B. Calpini
通讯作者：
B. Calpini
影响因子：
3.8
作者：
B. Palm;Xiaoxi Liu;J. Jimenez;J. Thornton
通讯作者：
B. Palm;Xiaoxi Liu;J. Jimenez;J. Thornton
DOI：
10.1029/2020jd033730
发表时间：
2021-06
期刊：
Journal of Geophysical Research: Atmospheres
影响因子：
--
作者：
J. Lindaas;Ilana B. Pollack;Julieta Juncosa Calahorrano;K. O’Dell;L. Garofalo;M. Pothier;D. Farmer;S. Kreidenweis;T. Campos;F. Flocke;A. Weinheimer;D. Montzka;G. Tyndall;E. Apel;A. Hills;R. Hornbrook;B. Palm;Q. Peng;J. Thornton;W. Permar;C. Wielgasz;Lu Hu;J. Pierce;J. Collett;A. Sullivan;E. Fischer
通讯作者：
J. Lindaas;Ilana B. Pollack;Julieta Juncosa Calahorrano;K. O’Dell;L. Garofalo;M. Pothier;D. Farmer;S. Kreidenweis;T. Campos;F. Flocke;A. Weinheimer;D. Montzka;G. Tyndall;E. Apel;A. Hills;R. Hornbrook;B. Palm;Q. Peng;J. Thornton;W. Permar;C. Wielgasz;Lu Hu;J. Pierce;J. Collett;A. Sullivan;E. Fischer
DOI：
10.1021/acsearthspacechem.0c00058
发表时间：
2020-07
期刊：
--
影响因子：
--
作者：
Jia Jiang;W. Carter;D. Cocker;K. Barsanti
通讯作者：
Jia Jiang;W. Carter;D. Cocker;K. Barsanti