Skipper T Nash, D'Ambro Emma L, Wiser Forwood C, McNeill V Faye, Schwantes Rebecca H, Henderson Barron H, Piletic Ivan R, Baublitz Colleen B, Bash Jesse O, Whitehill Andrew R, Valin Lukas C, Mouat Asher P, Kaiser Jennifer, Wolfe Glenn M, St Clair Jason M, Hanisco Thomas F, Fried Alan, Place Bryan K, Pye Havala O T
Oak Ridge Institute for Science and Education, Office of Research and Development, US Environmental Protection Agency, Research Triangle Park, North Carolina, USA.
Office of Research and Development, US Environmental Protection Agency, Research Triangle Park, North Carolina, USA.
Atmos Chem Phys. 2024 Nov;24(22):12903-12924. doi: 10.5194/acp-24-12903-2024. Epub 2024 Nov 21.
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.
甲醛(HCHO)是一种重要的空气污染物,具有直接致癌风险和形成臭氧的潜力。甲醛的来源很复杂,因为甲醛既直接排放,又由大多数气相活性有机碳氧化产生。我们更新了社区多尺度空气质量(CMAQ)模型中社区区域大气化学多相机制(CRACMM)里甲醛的二次生成。异戊二烯和单萜烯生成甲醛的量有所增加,纠正了当前版本中的低估情况。在美国东南部,模拟的6月至8月光化学生成高峰期(当地时间上午11:00至下午15:00)地表甲醛增加了0.6 ppb(32%),在美国本土增加了0.2 ppb(13%)。增加后的甲醛与对流层监测仪器(TROPOMI)基于卫星的观测结果以及基于飞机的观测结果相比更相符。根据每小时的地表观测进行评估表明,存在一个夜间汇缺失的问题,可以通过增加夜间沉降来改善,这会使美国东南部6月至8月夜间(当地时间20:00至04:00)地表甲醛减少1.1 ppb(36%),美国本土减少0.5 ppb(29%)。CRACMM捕捉中午甲醛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也有所改善,尽管仍低于观测值。使用既定的风险评估方法,美国本土(约3.2亿人)终身暴露于此处预测的环境甲醛水平可能导致6200例终身癌症病例,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的CRACMM版本2(CRACMM2)中提供。