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N₂O₅与矿物尘埃颗粒非均相反应的动力学及机理

Kinetics and mechanism of the heterogeneous reaction of N2O5 with mineral dust particles.

作者信息

Tang M J, Thieser J, Schuster G, Crowley J N

机构信息

Max Planck Institute for Chemistry, Atmospheric Chemistry Division, Mainz, Germany.

出版信息

Phys Chem Chem Phys. 2012 Jun 28;14(24):8551-61. doi: 10.1039/c2cp40805h. Epub 2012 May 21.

Abstract

The heterogeneous interaction of N2O5 with Saharan dust particles was investigated using aerosol flow tubes with detection of N2O5 by cavity-ring-down spectroscopy. The uptake coefficient, γ, was determined to be 0.02 ± 0.01 on airborne Saharan dust particles, independent of relative humidity (RH, 0-67%) and initial N2O5 concentration (5 × 10(11)-3 × 10(13) molecule cm(-3)). Analysis of gas- and particulate phase products suggests that N2O5 undergoes heterogeneous hydrolysis forming particulate nitrate. The independence of γ on the initial N2O5 concentration indicates that, on the seconds time scale of these experiments, the heterogeneous reaction of N2O5 with dust particles is not restricted to the external particle surface but internal reactive sites are also available. The particles could be deactivated with respect to N2O5 uptake only when pre-treated with very high levels of HNO3.

摘要

利用气溶胶流管并通过腔衰荡光谱法检测N2O5,研究了N2O5与撒哈拉沙尘颗粒的非均相相互作用。在空气中的撒哈拉沙尘颗粒上,摄取系数γ被确定为0.02±0.01,与相对湿度(RH,0 - 67%)和初始N2O5浓度(5×10(11) - 3×10(13)分子 cm(-3))无关。对气相和颗粒相产物的分析表明,N2O5发生非均相水解形成颗粒硝酸盐。γ对初始N2O5浓度的独立性表明,在这些实验的秒级时间尺度上,N2O5与沙尘颗粒的非均相反应不仅限于颗粒外表面,内部反应位点也可用。只有在经过非常高浓度的HNO3预处理后,颗粒对N2O5的摄取才会失活。

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