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Isoprene oxidation by nitrate radical: Alkyl nitrate and secondary organic aerosol yields

机译：硝酸根对异戊二烯的氧化作用：硝酸烷基酯和二次有机气溶胶的产率

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Alkyl nitrates and secondary organic aerosol (SOA) produced during the oxidation of isoprene by nitrate radicals has been observed in the SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction Chamber) chamber. A 16 h dark experiment was conducted with temperatures at 289-301K, and maximum concentrations of 11 ppb isoprene, 62.4 ppb O_3 and 31.1 ppb NO _x. We find the yield of nitrates is 70±8% from the isoprene + NO_3 reaction, and the yield for secondary dinitrates produced in the reaction of primary isoprene nitrates with NO_3 is 40±20%. We find an effective rate constant for reaction of NO_3 with the group of first generation oxidation products to be 7×10~(-14) molecule~(-1) cm~3 s~(-1). At the low total organic aerosol concentration in the chamber (max=0.52 μgm~(-3)) we observed a mass yield (ΔSOA mass/Δisoprene mass) of 2% for the entire 16 h experiment. However a comparison of the timing of the observed SOA production to a box model simulation of first and second generation oxidation products shows that the yield from the first generation products was <0.7% while the further oxidation of the initial products leads to a yield of 14% (defined as ΔSOA/Δisoprene~(2x) where Δisoprene~(2x) is the mass of isoprene which reacted twice with NO_3). The SOA yield of 14% is consistent with equilibrium partitioning of highly functionalized C _5 products of isoprene oxidation.
机译：在SAPHIR（在大反应室中模拟大气光化学反应）室中，观察到了异戊二烯被硝酸根自由基氧化过程中产生的烷基硝酸盐和次级有机气溶胶（SOA）。在289-301K的温度下进行了16小时的黑暗实验，最大浓度为11 ppb异戊二烯，62.4 ppb O_3和31.1 ppb NO_x。我们发现，异戊二烯+ NO_3反应的硝酸盐产率为70±8％，而伯异戊二烯硝酸盐与NO_3反应的次硝酸盐产率为40±20％。我们发现，NO_3与第一代氧化产物的反应有效速率常数为7×10〜（-14）分子〜（-1）cm〜3 s〜（-1）。在室内低的总有机气溶胶浓度下（最大值= 0.52μgm〜（-3）），我们观察到整个16小时实验的质量收率（ΔSOA质量/Δ异戊二烯质量）为2％。但是，将观察到的SOA生产的时间与第一代和第二代氧化产物的盒模型模拟的时间比较表明，第一代产物的产率<0.7％，而初始产物的进一步氧化导致产率为14 ％（定义为ΔSOA/Δ异戊二烯〜（2x），其中Δisoprene〜（2x）是与NO_3反应两次的异戊二烯的质量）。 SOA产率为14％，与高功能化异戊二烯氧化C _5产物的平衡分配相一致。

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