Heterogeneous uptake of gaseous nitric acid on dolomite (CaMg(CO3)2) and calcite (CaCO3) particles:: A knudsen cell study using multiple, single, and fractional particle layers

被引:28
作者
Johnson, ER
Sciegienka, J
Carlos-Cuellar, S
Grassian, VH [1 ]
机构
[1] Univ Iowa, Dept Chem, Iowa City, IA 52242 USA
[2] Univ Iowa, Environm Sci Program, Iowa City, IA 52242 USA
关键词
D O I
10.1021/jp0516285
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this study, the heterogeneous uptake of gaseous nitric acid on dolomite, CaMg(CO3)(2), and calcite, CaCO3, particles under dry conditions at 296 K was investigated. A Knudsen cell reactor was used to measure heterogeneous uptake coefficients for these reactions. Several different experiments were performed including those on many, single, and fractional layers of particles. For experiments using multiple particle layers, the Knudsen cell data were modeled to take into account gas diffusion into the underlying layers of the sample. From this analysis. initial heterogeneous uptake coefficients, gamma(o.t), were determined to be (5 +/- 2) x 10(-4) and (2 +/- 1) x 10(-3) for dolomite and calcite, respectively, at a nitric acid concentration of 6.5 x 10(10) molecules cm(-3). For experiments that employed single or fractional particle layers, the initial heterogeneous uptake coefficient was analyzed using a recent method described in the literature. Values of the initial heterogeneous uptake coefficient using this analysis were in agreement with the above analysis and determined to be (7 +/- 4) x 10(-4) and (2 +/- 0.4) x 10(-3) for CaMg(CO3)(2) and CaCO3, respectively. In addition, these results are compared to previous literature values.
引用
收藏
页码:6901 / 6911
页数:11
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