Kinetics of NO2 uptake on methane flame soot

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• 作者：V. V. Zelenov ; E. V. Aparina ; S. A. Kashtanov…
• 关键词：chemistry of the troposphere ; NO2 ; methane soot ; uptake coefficient ; Langmuir coefficient ; desorption rate constant ; adsorption heat ; rate constant ; activation energy
• 刊名：Russian Journal of Physical Chemistry B, Focus on Physics
• 出版年：2016
• 出版时间：January 2016
• 年：2016
• 卷：10
• 期：1
• 页码：172-178
• 全文大小：659 KB
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• 作者单位：V. V. Zelenov (1)
  E. V. Aparina (1)
  S. A. Kashtanov (2)
  E. V. Shardakova (1)
  
  1. Tal’roze Institute for Energy Problems of Chemical Physics (Chernogolovka Branch), Russian Academy of Sciences, Chernogolovka, Moscow oblast, Russia
  2. Institute of Chemical Physics, Russian Academy of Sciences, Chernogolovka, Moscow oblast, Russia
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Physical Chemistry
  Russian Library of Science
  
• 出版者：MAIK Nauka/Interperiodica distributed exclusively by Springer Science+Business Media LLC.
• ISSN：1990-7923

文摘

The dependences of the initial NO₂ uptake coefficient γ on a methane soot coating at 255 K on the NO₂ concentration (1.3 × 1012–3.3 × 1013 cm–3) and time t were studied using a flow reactor with a mobile insert and mass spectrometric recording of gaseous reagents and products: 1/γ(t) = 1/γ₀ + at, where γ₀ and a are the parameters that depend on the NO₂ concentration; γ₀ = γ₀ ini/(1 + k _L [NO₂], a= k [NO₂], with the constants γ₀ ini = (4.8 ± 2) × 10–4, K _L = (8.2 ± 3) × 10–13 cm3, and k = (2.3 ± 0.1) × 10–10 cm3 s–1. The elementary parameters that determine the uptake were evaluated on the basis of the Langmuir adsorption model: desorption rate constant k _d = (52 ± 20) s–1, adsorption heat Q _ad = (38 ± 8) kJ mol–1, rate constant of the unimolecular heterogeneous conversion of NO₂ into the product k _r = (2.5 ± 1.3) × 10–2 s–1, and its activation energy E _a = (19 ± 10) kJ mol–1. The laboratory data were extrapolated, based on the uptake coefficient, to the limiting tropospheric NO₂ concentrations in remote marine (1 ppb) and polluted industrial regions (40 ppb).