Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)

IF 5.2 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, Havala O. T. Pye
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Abstract

Abstract. Formaldehyde (HCHO) is an important air pollutant due to its direct health effects as an air toxic that contributes to elevated cancer risk, its role in ozone formation, and its role as a product from oxidation of most gas phase reactive organic carbon. We make several updates affecting secondary production of HCHO in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) in the Community Multiscale Air Quality (CMAQ) model. Secondary HCHO from isoprene and monoterpenes is increased, correcting an underestimate in the current version. Simulated 2019 June–August surface HCHO during peak photochemical production (11 am–3 pm) increased by 0.6 ppb (32 %) over the southeastern US and by 0.2 ppb (13 %) over the entire contiguous US. The increased HCHO compares more favorably with satellite-based observations from TROPOMI and observations from an aircraft campaign. Evaluation against hourly surface observations indicates a missing nighttime sink for HCHO which can be ameliorated by adding bidirectional exchange of HCHO and a leaf wetness dependent deposition process which increases nighttime deposition, decreasing 2019 June–August nocturnal (8 pm–4 am) surface HCHO by 1.1 ppb (36 %) over the southeastern US and 0.5 ppb (29 %) over the entire contiguous US. The ability of CRACMM to capture peak levels of HCHO at midday is improved, particularly at sites in the northeastern US, while peak levels at southeastern US sites are improved though still lower than observed. Using established risk assessment methods, lifetime exposure of the contiguous U.S. population (~320 million) to ambient HCHO levels predicted here may result in 6200 lifetime cancer cases, 40 % of which are from controllable anthropogenic emissions of nitrogen oxides and reactive organic compounds. Chemistry updates will be available in CRACMM version 2 (CRACMM2) in CMAQv5.5.
共同体区域大气化学多相机制(CRACMM)中化学品生产和沉积损失对甲醛的作用
摘要甲醛(HCHO)是一种重要的空气污染物,因为它作为一种空气有毒物质会直接影响健康,导致癌症风险升高,它在臭氧形成中的作用,以及它作为大多数气相活性有机碳氧化产物的作用。我们对共同体多尺度空气质量(CMAQ)模型中的共同体区域大气化学多相机制(CRACMM)中影响 HCHO 二次生成的部分进行了更新。增加了异戊二烯和单萜烯产生的二次 HCHO,纠正了当前版本中的低估。在光化学生成高峰期(上午 11 点至下午 3 点),模拟的 2019 年 6-8 月地表 HCHO 在美国东南部增加了 0.6 ppb(32%),在整个美国毗连地区增加了 0.2 ppb(13%)。增加的 HCHO 与 TROPOMI 卫星观测数据和飞机观测数据相比更为接近。根据每小时地表观测数据进行的评估表明,夜间缺少 HCHO 吸收汇,但可以通过增加 HCHO 的双向交换和叶片湿度依赖性沉积过程来改善,从而增加夜间沉积,使美国东南部地区 2019 年 6-8 月夜间(晚 8 点至早 4 点)地表 HCHO 减少 1.1 ppb(36%),整个美国毗连地区减少 0.5 ppb(29%)。CRACMM 捕获正午 HCHO 峰值水平的能力有所提高,尤其是在美国东北部的站点,而美国东南部站点的峰值水平有所提高,但仍低于观测值。使用既定的风险评估方法,美国毗连地区人口(约 3.2 亿)终生暴露于此处预测的环境 HCHO 水平可能会导致 6200 例癌症病例,其中 40% 来自可控的人为氮氧化物和活性有机化合物排放。化学更新将在 CMAQv5.5 中的 CRACMM 第 2 版 (CRACMM2) 中提供。
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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