The heterogeneous reaction of HNO3 on mineral dust and γ-alumina surfaces: a combined Knudsen cell and DRIFTS study
文献信息
Sabine Seisel, Christoph Börensen, Rainer Vogt, Reinhard Zellner
The kinetics of the interaction of HNO3 with natural mineral dusts (Saharan, Chinese and Arizona dust) and γ-alumina surfaces has been studied at T = 298 K using a Knudsen cell reactor coupled to a mass spectrometer for kinetic studies on the gas uptake as well as DRIFT spectroscopy for studies of the surface products. The uptake of HNO3 on each surface was found to be fast with initial uptake coefficients of γ ≈ 0.1. Nitrate and water have been identified as reaction products. The formation rate of surface nitrate, however, was slower with uptake coefficients ranging from 8 × 10−3 < γ < 5.4 × 10−2 depending on the chemical nature of the surface. From these results a two-step mechanism for the reactive uptake of HNO3 onto mineral oxides, consisting of fast adsorption of gas-phase HNO3 followed by a slower surface reaction of HNO3(ads) with surface OH-groups is inferred. Furthermore, it was found that the reactivity of mineral dust towards HNO3 decreased with increasing exposure. However, the original reactivity could be recovered by water exposure and may therefore be conserved under atmospheric conditions.
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