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OH 自由基与亚利桑那州试验尘的相互作用:吸收和产物。

Interaction of OH radicals with Arizona Test Dust: uptake and products.

机构信息

Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), CNRS, 45071 Orléans Cedex 2, France.

出版信息

J Phys Chem A. 2013 Jan 17;117(2):393-400. doi: 10.1021/jp311235h. Epub 2013 Jan 4.

Abstract

Kinetics and products of the interaction of OH radicals with solid films of Arizona Test Dust (ATD) were studied using a low pressure flow reactor (0.5-3 Torr) combined with a modulated molecular beam mass spectrometer for monitoring of the gaseous species involved. The reactive uptake coefficient of OH was measured from the kinetics of OH consumption on Pyrex rods coated with ATD as a function of OH concentration ((0.4-5.2) × 10(12) molecules cm(-3)), relative humidity (RH = 0.03-25.9%), temperature (T = 275-320 K), and UV irradiance intensity (J(NO(2)) = 0-0.012 s(-1)). Deactivation of ATD surface upon exposure to OH was observed. The initial uptake coefficient was found to be independent of temperature and irradiation conditions and to decrease with relative humidity: γ(0) = 0.2/(1 + RH(0.36)) (calculated using geometric surface area, with 30% estimated conservative uncertainty). H(2)O(2) and H(2)O were observed in the gas phase as products of the OH reaction with ATD surface with yields of (10 ± 3) and (98 ± 25) %, respectively.

摘要

使用低压流动反应器(0.5-3 托)结合调制分子束质谱仪研究了 OH 自由基与亚利桑那试验粉尘(ATD)固体膜的相互作用动力学和产物,用于监测涉及的气态物质。通过 OH 消耗动力学,从 Pyrex 棒上涂覆 ATD 的情况下,作为 OH 浓度((0.4-5.2)×10(12)分子 cm(-3))、相对湿度(RH = 0.03-25.9%)、温度(T = 275-320 K)和 UV 辐照度强度(J(NO(2))= 0-0.012 s(-1))的函数,测量 OH 的反应性摄取系数。发现暴露于 OH 时 ATD 表面失活。初始摄取系数被发现与温度和辐照条件无关,并随相对湿度而降低:γ(0)= 0.2/(1 + RH(0.36))(使用几何表面积计算,估计保守不确定性为 30%)。作为 OH 与 ATD 表面反应的产物,在气相中观察到 H2O2 和 H2O,产率分别为(10±3)%和(98±25)%。

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