Johnson Elizabeth R, Sciegienka Joanna, Carlos-Cuellar Sofia, Grassian Vicki H
Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, USA.
J Phys Chem A. 2005 Aug 11;109(31):6901-11. doi: 10.1021/jp0516285.
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.
在本研究中,对296K干燥条件下气态硝酸在白云石(CaMg(CO3)2)和方解石(CaCO3)颗粒上的非均相吸收进行了研究。使用克努森池反应器测量这些反应的非均相吸收系数。进行了几个不同的实验,包括对多层、单层和部分单层颗粒的实验。对于使用多层颗粒的实验,对克努森池数据进行建模,以考虑气体扩散到样品的下层。通过该分析,在硝酸浓度为6.5×10(10)分子·cm(-3)时,白云石和方解石的初始非均相吸收系数γ(o,t)分别确定为(5±2)×10(-4)和(2±1)×10(-3)。对于采用单层或部分单层颗粒的实验,使用文献中描述的最新方法分析初始非均相吸收系数。使用该分析得到的初始非均相吸收系数值与上述分析一致,CaMg(CO3)2和CaCO3的初始非均相吸收系数分别确定为(7±4)×10(-4)和(2±0.4)×10(-3)。此外,将这些结果与先前文献值进行了比较。