Parameterizations of US wildfire and prescribed fire emission ratios and emission factors based on FIREX-AQ aircraft measurements-猫眼课题宝

DOI：

10.5194/acp-24-929-2024

发表时间：

2024-01

期刊：

Atmospheric Chemistry and Physics

影响因子：

6.3

通讯作者：

中科院分区：

地球科学1区

文献类型：

作者：

G. Gkatzelis;M. Coggon;C. Stockwell;R. Hornbrook;H. Allen;E. Apel;M. Bela;Donald R. Blake;I. Bourgeois;S. S. Brown-S.;P. Campuzano‐Jost;J. S. St. Clair;James. H. Crawford;J. Crounse;D. Day;J. Digangi;G. Diskin;Alan Fried;J. Gilman;Hongyu Guo;J. W. Hair;H. Halliday;T. Hanisco;R. Hannun;A. Hills;L. G. Huey;J. Jimenez;J. Katich;A. Lamplugh;Young Ro Lee;Jin Liao;J. Lindaas;S. Mckeen;T. Mikoviny;B. Nault;J. Neuman;J. Nowak;D. Pagonis;J. Peischl;A. Perring;F. Piel;P. Rickly;M. A. Robinson;A. Rollins;T. Ryerson;Melinda (Mindy) Schueneman;R. Schwantes;J. Schwarz;K. Sekimoto;Vanessa Selimovic;Taylor J. Shingler;David J. Tanner;L. Tomsche;Krystal T. Vasquez;P. Veres;R. Washenfelder;P. Weibring;P. Wennberg;Armin Wisthaler;G. Wolfe;C. Womack;Lu Xu;Katherine Ball;R. Yokelson;C. Warneke

抽象的。在 2019 年 NOAA/NASA 火灾对区域到全球环境和空气质量影响活动 (FIREX-AQ) 期间，对美国野火和规定火灾的非甲烷有机气体 (NMOG)、甲烷、氮氧化物、还原氮物种和气溶胶排放进行了广泛的机载测量。在这里，我们报告了在 NASA DC-8 研究飞机上测量的 9 场野火和一场指定火灾（涵盖一系列植被类型）的化合物的大气增强比 (ER) 和推断排放因子 (EF)。我们使用光化学代理来识别年轻烟雾并减少化学降解对排放计算的影响。根据 FIREX-AQ 观测计算出的 ER 和 EF 的一致性在 2 倍以内，与之前实验室和现场研究报告的 80% 以上的含碳和氮物种的值一致。野火排放的参数化基于 NMOG 与活性氮氧化物 (NOy) 总和与改良燃烧效率 (MCE) 以及指示火焰/阴燃燃烧的其他化学特征的相关性，包括一氧化碳 (CO)、二氧化氮 (NO2) 和黑碳气溶胶。主要 NMOG EF 之和与 MCE 相关，R2 为 0.68，斜率为 -296 ± 51 g kg−1，与之前的研究一致。 NMOG 混合比总和与 CO 相关性良好，R2 为 0.98，NMOG 的斜率为 137 ± 4 ppbv 每百万分之一体积 (ppmv) CO，表明可以根据 CO 估算主要 NMOG 排放量。单个含氮物种与 NO2、NOy 和黑碳的相关性优于与 CO 的相关性。新鲜羽流中一半以上的 NOy 是 NO2，R2 为0.95，NO2 与 NOy 的比率为 0.55 ± 0.05 ppbv ppbv−1，这突出表明在采样的火羽流中已经发生了快速光化学反应。 NOy 与 NMOG 总量的比率遵循实验室实验中观察到的趋势，并且随着 MCE 呈指数增加，这是由于在有焰燃烧期间，关键氮物种的排放量增加，而在较高 MCE 下 NMOG 的排放量减少。这些参数化将为火羽化学和演化的建模和卫星研究提供更准确的边界条件，以预测顺风形成的二次污染物（包括臭氧和二次有机气溶胶）。

Abstract. Extensive airborne measurements of non-methane organic gases (NMOGs), methane, nitrogen oxides, reduced nitrogen species, and aerosol emissions from US wild and prescribed fires were conducted during the 2019 NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality campaign (FIREX-AQ). Here, we report the atmospheric enhancement ratios (ERs) and inferred emission factors (EFs) for compounds measured on board the NASA DC-8 research aircraft for nine wildfires and one prescribed fire, which encompass a range of vegetation types. We use photochemical proxies to identify young smoke and reduce the effects of chemical degradation on our emissions calculations. ERs and EFs calculated from FIREX-AQ observations agree within a factor of 2, with values reported from previous laboratory and field studies for more than 80 % of the carbon- and nitrogen-containing species. Wildfire emissions are parameterized based on correlations of the sum of NMOGs with reactive nitrogen oxides (NOy) to modified combustion efficiency (MCE) as well as other chemical signatures indicative of flaming/smoldering combustion, including carbon monoxide (CO), nitrogen dioxide (NO2), and black carbon aerosol. The sum of primary NMOG EFs correlates to MCE with an R2 of 0.68 and a slope of −296 ± 51 g kg−1, consistent with previous studies. The sum of the NMOG mixing ratios correlates well with CO with an R2 of 0.98 and a slope of 137 ± 4 ppbv of NMOGs per parts per million by volume (ppmv) of CO, demonstrating that primary NMOG emissions can be estimated from CO. Individual nitrogen-containing species correlate better with NO2, NOy, and black carbon than with CO. More than half of the NOy in fresh plumes is NO2 with an R2 of 0.95 and a ratio of NO2 to NOy of 0.55 ± 0.05 ppbv ppbv−1, highlighting that fast photochemistry had already occurred in the sampled fire plumes. The ratio of NOy to the sum of NMOGs follows trends observed in laboratory experiments and increases exponentially with MCE, due to increased emission of key nitrogen species and reduced emission of NMOGs at higher MCE during flaming combustion. These parameterizations will provide more accurate boundary conditions for modeling and satellite studies of fire plume chemistry and evolution to predict the downwind formation of secondary pollutants, including ozone and secondary organic aerosol.

Parameterizations of US wildfire and prescribed fire emission ratios and emission factors based on FIREX-AQ aircraft measurements

文献摘要

相似文献