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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetics of surface-bound benzo[a]pyrene and ozone on solid organic and salt aerosols
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Kinetics of surface-bound benzo[a]pyrene and ozone on solid organic and salt aerosols

机译：固体有机和盐气溶胶表面结合的苯并[a] and和臭氧的动力学

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An aerosol flow tube apparatus was developed to perform the first kinetic study of the oxidation of particulate-bound BaP on solid organic and salt aerosols by gas-phase ozone. The studies on azelaic acid aerosols were performed with submonolayer coatings of BaP under both dry (RH < 1%) and high relative humidity (RH similar to 72%) conditions. The reaction exhibited pseudo-first-order kinetics for BaP loss and the pseudo-first-order rate coefficients displayed a Langmuir-Hinshelwood dependence on gas-phase ozone concentration. Under high relative humidity conditions the kinetics were faster but also displayed a similar functional dependence on the gas-phase ozone concentration. By assuming Langmuir-Hinshelwood behavior, the following parameters were obtained: ozone-surface equilibrium constant K-O3(< 1% RH) = (1.2 +/- 0.4) x 10(-15) cm(-1), K-O3(72% RH) = (2.8 +/- 1.4) x 10(-15) cm(-3), the maximum pseudo-first-order rate coefficient k(max)(I) (< 1% RH) = (0.048 +/- 0.008) s(-1), k(max)(I)(72% RH) = (0.060 +/- 0.018) s(-1). Uptake coefficients were extracted from the pseudofirst-order rate coefficients and a slight trend of decreasing uptake coefficients with increasing ozone concentration was observed. In contrast to the behavior on azelaic acid aerosols, no reaction was observed between ozone and BaP adsorbed to solid NaCl particles. These results are compared to previous studies, which have been performed on different substrates, and their atmospheric implications are discussed. We conclude that a strong substrate effect prevails in this reaction with the kinetics proceeding faster on surfaces best able to adsorb ozone.
机译：开发了一种气溶胶流量管设备，以进行通过气相臭氧对固体有机和盐气溶胶上结合的BaP进行氧化的第一动力学研究。壬二酸气雾剂的研究是在干燥（相对湿度<1％）和相对湿度较高（相对于72％相对湿度）的条件下，用BaP亚单层涂层进行的。该反应表现出BaP损失的拟一级动力学，拟一级速率系数显示Langmuir-Hinshelwood对气相臭氧浓度的依赖性。在较高的相对湿度条件下，动力学更快，但对气相臭氧浓度也显示出类似的功能依赖性。通过假设Langmuir-Hinshelwood行为，获得以下参数：臭氧表面平衡常数K-O3（<1％RH）=（1.2 +/- 0.4）x 10（-15）cm（-1），K-O3 （72％RH）=（2.8 +/- 1.4）x 10（-15）cm（-3），最大伪一阶速率系数k（max）（I）（<1％RH）=（0.048 +/- 0.008）s（-1），k（max）（I）（72％RH）=（0.060 +/- 0.018）s（-1）。从伪一级速率系数中提取了吸收系数，并观察到随着臭氧浓度的增加，吸收系数有轻微的下降趋势。与壬二酸气溶胶的行为相反，臭氧和吸附在固体NaCl颗粒上的BaP之间没有反应。将这些结果与以前在不同基材上进行的研究进行了比较，并讨论了它们对大气的影响。我们得出结论，在该反应中普遍存在较强的底物效应，在最能吸附臭氧的表面上动力学进行得更快。

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