Mass spectrometry of interfacial layers during fast aqueous aerosol/ozone gas reactions of atmospheric interest
Mass spectrometry of interfacial layers during fast aqueous aerosol/ozone gas reactions of atmospheric interest
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DOI：
10.1016/j.cplett.2008.02.075
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发表时间：
2008-04-10
影响因子：
2.8
通讯作者：
Colussi, A. J.
中科院分区：
文献类型：
--
作者：
Enami, S.;Vecitis, C. D.;Colussi, A. J.
用静电喷射阴离子的在线质谱仪研究了O-3(G)作用1ms时水相微滴界面层中硫酸盐和碘的氧化反应。S(IV)Na_2SO_3微滴的氧化损失与[S(IV)][O-3(G)]成正比，最高可达90%的转化率。在等摩尔(Na2SO3+NaI)微滴的界面层中，I-比HSO3-更丰富，在大溶液中转化为O-3(AQ)的活性比HSO3-高3倍，但它被转化为I-3(-)和I03-+一种持久的IS03-中间体。这些观察揭示了在以前的快速气液反应处理中没有考虑到的意外的界面梯度、反应模式和传输现象。(C)2008爱思唯尔B.V.保留所有权利。
The oxidations of sulfate and iodide in the interfacial layers of aqueous microdroplets exposed to O-3( g) for 1 ms are investigated by online mass spectrometry of the electrostatically ejected anions. S(IV) oxidation losses in Na2SO3 microdroplets are proportional to [ S( IV)] [ O-3( g)] up to similar to 90% conversion. I- is more abundant than HSO3- in the interfacial layers of equimolar (Na2SO3 + NaI) microdroplets and similar to 3 times more reactive than HSO3- toward O-3(aq) in bulk solution, but it is converted with minimal loss to I-3(-) and IO3- plus a persistent ISO3- intermediate. These observations reveal unanticipated interfacial gradients, reactivity patterns and transport phenomena that had not been taken into account in previous treatments of fast gas - liquid reactions. (c) 2008 Elsevier B. V. All rights reserved.