The heterogeneous reaction of HNO3 on mineral dust and γ-alumina surfaces: a combined Knudsen cell and DRIFTS study

文献信息

发布日期 2004-10-29
DOI 10.1039/B410793D
影响因子 3.676
作者

Sabine Seisel, Christoph Börensen, Rainer Vogt, Reinhard Zellner


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摘要

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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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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