Brownwood Bellamy, Turdziladze Avtandil, Hohaus Thorsten, Wu Rongrong, Mentel Thomas F, Carlsson Philip T M, Tsiligiannis Epameinondas, Hallquist Mattias, Andres Stefanie, Hantschke Luisa, Reimer David, Rohrer Franz, Tillmann Ralf, Winter Benjamin, Liebmann Jonathan, Brown Steven S, Kiendler-Scharr Astrid, Novelli Anna, Fuchs Hendrik, Fry Juliane L
Chemistry Department and Environmental Studies Program, Reed College, Portland, Oregon 97202, United States.
Institute for Energy and Climate (IEK-8), Forschungszentrum Jülich, Jülich 52428, Germany.
ACS Earth Space Chem. 2021 Apr 15;5(4):785-800. doi: 10.1021/acsearthspacechem.0c00311. Epub 2021 Mar 11.
Alkyl nitrate (AN) and secondary organic aerosol (SOA) from the reaction of nitrate radicals (NO) with isoprene were observed in the Simulation of Atmospheric PHotochemistry In a large Reaction (SAPHIR) chamber during the NOIsop campaign in August 2018. Based on 15 day-long experiments under various reaction conditions, we conclude that the reaction has a nominally unity molar AN yield (observed range 90 ± 40%) and an SOA mass yield of OA + organic nitrate aerosol of 13-15% (with ∼50 μg m inorganic seed aerosol and 2-5 μg m total organic aerosol). Isoprene (5-25 ppb) and oxidant (typically ∼100 ppb O and 5-25 ppb NO) concentrations and aerosol composition (inorganic and organic coating) were varied while remaining close to ambient conditions, producing similar AN and SOA yields under all regimes. We observe the formation of dinitrates upon oxidation of the second double bond only once the isoprene precursor is fully consumed. We determine the bulk partitioning coefficient for ANs ( ∼ 10 m μg), indicating an average volatility corresponding to a C hydroxy hydroperoxy nitrate.
2018年8月“NO异戊二烯”活动期间,在大型反应大气光化学模拟(SAPHIR)腔室中观测到了硝酸烷基酯(AN)以及硝酸根自由基(NO)与异戊二烯反应生成的二次有机气溶胶(SOA)。基于在各种反应条件下进行的为期15天的实验,我们得出结论,该反应的标称AN摩尔产率为1(观测范围为90±40%),OA + 有机硝酸气溶胶的SOA质量产率为13 - 15%(有50μg/m³无机种子气溶胶和2 - 5μg/m³总有机气溶胶)。异戊二烯(5 - 25 ppb)和氧化剂(通常为100 ppb O₃和5 - 25 ppb NO)浓度以及气溶胶组成(无机和有机涂层)发生变化,同时保持接近环境条件,在所有情况下都产生了相似的AN和SOA产率。只有在异戊二烯前体完全消耗后,我们才观测到第二个双键氧化时二硝酸酯的形成。我们确定了ANs的整体分配系数(~10 m³/μg),表明其平均挥发性对应于一种C₅羟基氢过氧硝酸盐。