Formation and Evolution of Catechol-Derived SOA Mass, Composition, Volatility, and Light Absorption
Formation and Evolution of Catechol-Derived SOA Mass, Composition, Volatility, and Light Absorption
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DOI：
10.1021/acsearthspacechem.2c00007
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发表时间：
2022-03
影响因子：
3.4
通讯作者：
C. Fredrickson;B. Palm;B. H. Lee;Xuan Zhang;J. Orlando;G. Tyndall;L. Garofalo;M. Pothier;D. Farmer;Z. Decker;M. A. Robinson;S. Brown;S. Murphy;Yingjie Shen;A. Sullivan;S. Schobesberger;J. Thornton
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文献类型：
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作者：
C. Fredrickson;B. Palm;B. H. Lee;Xuan Zhang;J. Orlando;G. Tyndall;L. Garofalo;M. Pothier;D. Farmer;Z. Decker;M. A. Robinson;S. Brown;S. Murphy;Yingjie Shen;A. Sullivan;S. Schobesberger;J. Thornton
从野火排放的酚类化合物有助于二次有机气溶胶（SOA）和棕色碳（BrC）的氧化引发的羟基（OH）和硝酸根（NO3）。我们进行了一组实验室室实验，研究邻苯二酚氧化OH和NO3的重点相关的SOA的形成和演变的条件下，有关的新鲜野火羽流。使用碘化物加合物高分辨率飞行时间化学电离质谱仪与气体和气溶胶过滤器入口耦合（FIGAERO-CIMS）测量气相和颗粒相的氧化产物以及SOA挥发性。硝基邻苯二酚（C6 H5 NO 4）是占主导地位的颗粒相化合物在OH-引发和NO3-引发的氧化，并强烈相关的颗粒在405 nm处的光吸收，与BrC一致。最大SOA的质量产率，范围从0.1至1.6的OH-和NO3-驱动的实验，分别与净形成的硝基邻苯二酚。气粒分配测量表明，OH引发实验中硝基邻苯二酚的有效饱和蒸气浓度c* 为12 μg m-3，NO3引发实验中为2.4 μg m-3，均远低于基团贡献法的估计值（1.8 × 102 ~ 8.5 × 108μg m-3）。在延长的光化学老化实验中，室中BrC的壁损失校正的光化学寿命分别为17.4 ± 0.8和12.4 ± 0.1 h，而颗粒硝基邻苯二酚的寿命分别为21 ± 8和6.9 ± 0.6 h（OH引发和NO3引发条件）。酚衍生的SOA和BrC演变野火羽的影响进行了讨论。
Phenolic compounds emitted from wildfires contribute to secondary organic aerosol (SOA) and brown carbon (BrC) upon oxidation initiated by hydroxyl (OH) and nitrate radicals (NO3). We conducted a set of laboratory chamber experiments to study catechol oxidation by OH and NO3with a focus on the associated SOA formation and evolution under conditions relevant to fresh wildfire plumes. Oxidation products in both gas and particle phases as well as SOA volatility were measured using an iodide-adduct high-resolution time-of-flight chemical ionization mass spectrometer coupled with the filter inlet for gases and aerosols (FIGAERO-CIMS). Nitrocatechol (C6H5NO4) was the dominant particle-phase compound in both OH-initiated and NO3-initiated oxidation and was strongly associated with particle light absorption at 405 nm, consistent with BrC. Maximum SOA mass yields, ranging from 0.1 to 1.6 for the OH- and NO3-driven experiments, respectively, varied with the net formation of nitrocatechol. Gas–particle partitioning measurements implied the effective saturation vapor concentration,c*, of nitrocatechol is 12 μg m–3for the OH-initiated experiment and 2.4 μg m–3for the NO3-initiated experiments, both far lower than group contribution method estimates, which ranged from 1.8 × 102to 8.5 × 108μg m–3. In extended photochemical aging experiments, wall-loss-corrected photochemical lifetimes of BrC in the chamber were 17.4 ± 0.8 and 12.4 ± 0.1 h, while particulate nitrocatechol had lifetimes of 21 ± 8 and 6.9 ± 0.6 h for OH-initiated and NO3-initiated conditions, respectively. Implications for phenolic-derived SOA and BrC evolution in wildfire plumes are discussed.