Novel Analysis to Quantify Plume Crosswind Heterogeneity Applied to Biomass Burning Smoke
Novel Analysis to Quantify Plume Crosswind Heterogeneity Applied to Biomass Burning Smoke
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DOI：
10.1021/acs.est.1c03803
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发表时间：
2021-12-07
影响因子：
11.4
通讯作者：
Brown, Steven S.
中科院分区：
文献类型：
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作者：
Decker, Zachary C. J.;Wang, Siyuan;Brown, Steven S.
我们提出了一种新的方法，高斯边缘到中心非均质性观测模型（GOMECH）来量化羽流的水平化学结构。GOMECH将观测到的短寿命排放物或产物与长寿命示踪剂（如CO）进行拟合，以提供羽流宽度(w（i)/w(CO)）和中心(b（i)/w(CO)）的相对度量。为了验证GOMECH，我们研究了Fire - aq（火灾对区域到全球环境和空气质量的影响，2019年野火烟雾研究）期间采样的烟羽中的OH和NO3氧化过程。对430个侧风断面的分析表明，亚硝酸盐（HONO）是OH的主要来源，比CO更窄(w(HONO)/w(CO) = 0.73-0.84 +/- 0.01)，羟基氧化产物马来酸酐在羽流边缘增强（w（马来酸酐）/w(CO) = 1.06-1.12 +/- 0.01）。NO3生成[P(NO3)]主要发生在烟羽中心(w(P（NO3))/w(CO) = 0.91 ~ 1.00 +/- 0.01）。对OH和NO3反应强烈的酚类排放物比CO排放物窄(w（苯酚）/w(CO) = 0.96 +/- 0.03, w（儿茶酚）/w(CO) = 0.91 +/- 0.01, w（甲基儿茶酚）/w(CO) = 0.84 +/- 0.01)，表明羽流边缘的酚类排放物损失最大。而其氧化产物硝基酚气溶胶在羽流中心最大(w（nitrophenolicaerosol)/w(CO) = 0.95 +/- 0.02）。在一项大型羽流案例研究中，GOMECH表明硝基儿茶酚气溶胶与P（NO3）的关系最为密切。最后，我们用一个大涡模拟模型证实了GOMECH，该模型表明，在我们的案例研究中，大部分（55%）硝基儿茶酚是通过NO3产生的。
We present a novel method, the Gaussian observational model for edge to center heterogeneity (GOMECH), to quantify the horizontal chemical structure of plumes. GOMECH fits observations of short-lived emissions or products against a long-lived tracer (e.g., CO) to provide relative metrics for the plume width (w(i)/w(CO)) and center (b(i)/w(CO)). To validate GOMECH, we investigate OH and NO3 oxidation processes in smoke plumes sampled during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality, a 2019 wildfire smoke study). An analysis of 430 crosswind transects demonstrates that nitrous acid (HONO), a primary source of OH, is narrower than CO (w(HONO)/w(CO) = 0.73-0.84 +/- 0.01) and maleic anhydride (an OH oxidation product) is enhanced on plume edges (w(maleicanhydride)/w(CO) = 1.06-1.12 +/- 0.01). By contrast, NO3 production [P(NO3)] occurs mainly at the plume center (w(P(NO3))/w(CO) = 0.91-1.00 +/- 0.01). Phenolic emissions, highly reactive to OH and NO3, are narrower than CO (w(phenol)/w(CO) = 0.96 +/- 0.03, w(catechol)/w(CO) = 0.91 +/- 0.01, and w(methylcatechol)/w(CO) = 0.84 +/- 0.01), suggesting that plume edge phenolic losses are the greatest. Yet, nitrophenolic aerosol, their oxidation product, is the greatest at the plume center (w(nitrophenolicaerosol)/w(CO) = 0.95 +/- 0.02). In a large plume case study, GOMECH suggests that nitrocatechol aerosol is most associated with P(NO3). Last, we corroborate GOMECH with a large eddy simulation model which suggests most (55%) of nitrocatechol is produced through NO3 in our case study.