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
Atmospheric Chemistry and Physics Pub Date : 2024-11-01 Epub Date: 2024-11-21 DOI:10.5194/acp-24-12903-2024
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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引用次数: 0

Abstract

Formaldehyde (HCHO) is an important air pollutant with direct cancer risk and ozone-forming potential. HCHO sources are complex because HCHO is both directly emitted and produced from oxidation of most gas-phase reactive organic carbon. We update the secondary production of HCHO in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) in the Community Multiscale Air Quality (CMAQ) model. Production of HCHO from isoprene and monoterpenes is increased, correcting an underestimate in the current version. Simulated June-August surface HCHO during peak photochemical production (11:00-15:00 LT, local time) increased by 0.6 ppb (32 %) over the southeastern USA and by 0.2 ppb (13 %) over the contiguous USA. The increased HCHO compares more favorably with satellite-based observations from the TROPOspheric Monitoring Instrument (TROPOMI) and from aircraft-based observations. Evaluation against hourly surface observations indicates a missing nighttime sink that can be improved by increased nighttime deposition, which reduces June-August nocturnal (20:00-04:00 LT) surface HCHO by 1.1 ppb (36 %) over the southeastern USA and 0.5 ppb (29 %) over the contiguous USA. The ability of CRACMM to capture peak levels of HCHO at midday is improved, particularly at sites in the northeastern USA, while peak levels at sites in the southeastern USA are improved, although still lower than observed. Using established risk assessment methods, lifetime exposure of the population in the contiguous USA (~320 million) to ambient HCHO levels predicted here may result in 6200 lifetime cancer cases, with 40 % from controllable anthropogenic emissions of nitrogen oxides and reactive organic compounds. Chemistry updates will be available in CRACMM version 2 (CRACMM2) in CMAQv5.5.

群落区域大气化学多相机制(CRACMM)中甲醛化学生产和沉积损失的作用
甲醛(HCHO)是一种重要的空气污染物,具有直接致癌风险和臭氧形成潜力。HCHO的来源很复杂,因为HCHO既可以直接排放,也可以由大多数气相活性有机碳氧化产生。对社区多尺度空气质量(CMAQ)模式中社区区域大气化学多相机制(CRACMM)中HCHO的二次生成进行了更新。从异戊二烯和单萜烯中产生的HCHO增加了,纠正了当前版本中的低估。在光化学生产高峰期(当地时间11:00-15:00 LT),模拟的6 - 8月地面HCHO在美国东南部增加了0.6 ppb(32%),在美国邻近地区增加了0.2 ppb(13%)。增加的HCHO与对流层监测仪(TROPOMI)的卫星观测和飞机观测相比更为有利。对每小时地面观测的评估表明,缺失的夜间汇可以通过增加夜间沉积来改善,这使得6月至8月夜间(20:00-04:00 LT)的地面HCHO在美国东南部减少1.1 ppb(36%),在美国邻近地区减少0.5 ppb(29%)。CRACMM捕捉正午HCHO峰值水平的能力有所提高,特别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,尽管仍低于观测值。使用已建立的风险评估方法,美国邻近地区的人口(约3.2亿)终生暴露于本文预测的环境HCHO水平,可能导致6200例终生癌症病例,其中40%来自可控的氮氧化物和活性有机化合物的人为排放。化学更新将在CMAQv5.5中的CRACMM版本2 (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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