Partitioning of Organonitrates in the Production of Secondary Organic Aerosols from α-Pinene Photo-Oxidation.
Partitioning of Organonitrates in the Production of Secondary Organic Aerosols from α-Pinene Photo-Oxidation.
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α-蒎烯光氧化生成二次有机气溶胶过程中有机硝酸盐的分配情况
DOI：
10.1021/acs.est.1c08380
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发表时间：
2022-05-03
影响因子：
11.4
通讯作者：
Martin, Scot T.
中科院分区：
文献类型：
--
作者：
Aruffo, Eleonora;Wang, Junfeng;Ye, Jianhuai;Ohno, Paul;Qin, Yiming;Stewart, Matthew;McKinney, Karena;Di Carlo, Piero;Martin, Scot T.
二次有机气溶胶（SOA）产生的化学途径受到氮氧化物（NOx）浓度的影响，包括有机硝酸盐（ON）的产生。本文在环境室中进行了一系列实验，研究了α-蒎烯在<1至24 ppb NOx条件下光氧化产生和分配总有机硝酸酯的情况。采用激光诱导荧光（LIF）法测定气相和颗粒相有机硝酸盐（分别为gON和pON）。采用在线气溶胶质谱法同时表征了颗粒相组成和颗粒质量浓度。pON浓度的LIF和MS测量值在0.3 ~ 1.1 μg - m-3范围内的Pearson相关系数为0.91。当NOx浓度为1 ~ 6 ppb时，随着NOx浓度的增加，SOA粒子质量浓度的产率从0.02提高到0.044。当NOx浓度为bb60 ppb时，产率稳步下降，在NOx浓度为24 ppb时产率仅为0.034。相比之下，在不同的NOx浓度范围内，pON的产率从0.002稳步增加到0.022。氮化镓的产率也由0.005提高到0.148。气粒分配比（pON/(pON + gON)）强烈依赖于NOx浓度，当NOx浓度从<1 ppb增加到24 ppb时，pON/(pON + gON)从0.27变化到0.13。在大气中，通常在清洁和污染条件之间存在一个交叉点，该交叉点强烈影响SOA的产生，本文的结果定量地确定了6 ppb NOx是在这些研究条件下α-蒎烯光氧化的点，包括有机硝酸盐的产生和分配。由于pON挥发性的变化，SOA产率和分配比作为NOx的函数的趋势发生了变化。生物源和人为排放之间的相互作用已被研究，确定有机硝酸盐气体到颗粒的分配强烈依赖于NOx浓度。
The chemical pathways for the production of secondary organic aerosols (SOA) are influenced by the concentration of nitrogen oxides (NOx), including the production of organonitrates (ON). Herein, a series of experiments conducted in an environmental chamber investigated the production and partitioning of total organonitrates from α-pinene photo-oxidation from <1 to 24 ppb NOx. Gas-phase and particle-phase organonitrates (gON and pON, respectively) were measured by laser-induced fluorescence (LIF). The composition of the particle phase and the particle mass concentration were simultaneously characterized by online aerosol mass spectrometry. The LIF and MS measurements of pON concentrations had a Pearson correlation coefficient of 0.91 from 0.3 to 1.1 μg m–3. For 1–6 ppb NOx, the yield of SOA particle mass concentration increased from 0.02 to 0.044 with NOx concentration. For >6 ppb NOx, the yield steadily dropped, reaching 0.034 at 24 ppb NOx. By comparison, the yield of pON steadily increased from 0.002 to 0.022 across the range of investigated NOx concentrations. The yield of gON likewise increased from 0.005 to 0.148. The gas-to-particle partitioning ratio (pON/(pON + gON)) depended strongly on the NOx concentration, changing from 0.27 to 0.13 as the NOx increased from <1 to 24 ppb. In the atmosphere, there is typically a cross-over point between clean and polluted conditions that strongly affects SOA production, and the results herein quantitatively identify 6 ppb NOx as that point for α-pinene photo-oxidation under these study conditions, including the production and partitioning of organonitrates. The trends in SOA yield and partitioning ratio as a function of NOx occur because of the changes in pON volatility. The interaction between biogenic and anthropogenic emissions has been investigated, identifying that organonitrate gas-to-particle partitioning strongly depends on NOx concentration.
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