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含二元羧酸气溶胶对N2O5的反应性摄取。颗粒相、组成和硝酸盐含量的影响。

Reactive uptake of N2O5 by aerosols containing dicarboxylic acids. Effect of particle phase, composition, and nitrate content.

作者信息

Griffiths Paul T, Badger Claire L, Cox R Anthony, Folkers Mareike, Henk Hartmut H, Mentel Thomas F

机构信息

Centre for Atmospheric Science, Department of Chemistry, Lensfield Road, University of Cambridge, Cambridge, CB2 1EW, United Kingdom.

出版信息

J Phys Chem A. 2009 Apr 30;113(17):5082-90. doi: 10.1021/jp8096814.

Abstract

Reactive uptake coefficients for loss of N(2)O(5) to micron-size aerosols containing oxalic malonic, succinic, and glutaric acids, and mixtures with ammonium hydrogen sulfate and ammonium sulfate, are presented. The uptake measurements were made using two different systems: atmospheric pressure laminar flow tube reactor (Cambridge) and the Large Indoor Aerosol Chamber at Forschungszentrum Juelich. Generally good agreement is observed for the data recorded using the two techniques. Measured uptake coefficients lie in the range 5 x 10(-4)-3 x 10(-2), dependent on relative humidity, on particle phase, and on particle composition. Uptake to solid particles is generally slow, with observed uptake coefficients less than 1 x 10(-3), while uptake to liquid particles is around an order of magnitude more efficient. These results are rationalized using a numerical model employing explicit treatment of both transport and chemistry. Our results indicate a modest effect of the dicarboxylic acids on uptake and confirm the strong effect of particle phase, liquid water content, and particulate nitrate concentrations.

摘要

本文给出了N₂O₅与含有草酸、丙二酸、琥珀酸和戊二酸的微米级气溶胶以及与硫酸氢铵和硫酸铵混合物反应的摄取系数。摄取测量使用了两种不同的系统:大气压层流管反应器(剑桥)和于利希研究中心的大型室内气溶胶室。对于使用这两种技术记录的数据,总体上观察到了良好的一致性。测量的摄取系数范围为5×10⁻⁴ - 3×10⁻²,这取决于相对湿度、颗粒相和颗粒组成。对固体颗粒的摄取通常较慢,观察到的摄取系数小于1×10⁻³,而对液体颗粒的摄取效率大约高一个数量级。使用一个对传输和化学过程都进行显式处理的数值模型对这些结果进行了合理化分析。我们的结果表明二元羧酸对摄取有适度影响,并证实了颗粒相、液态水含量和颗粒硝酸盐浓度的强烈影响。

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