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由甲磺酸、三甲胺和水形成新颗粒并使其生长。

New particle formation and growth from methanesulfonic acid, trimethylamine and water.

作者信息

Chen Haihan, Ezell Michael J, Arquero Kristine D, Varner Mychel E, Dawson Matthew L, Gerber R Benny, Finlayson-Pitts Barbara J

机构信息

Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA.

出版信息

Phys Chem Chem Phys. 2015 May 28;17(20):13699-709. doi: 10.1039/c5cp00838g.

Abstract

New particle formation from gas-to-particle conversion represents a dominant source of atmospheric particles and affects radiative forcing, climate and human health. The species involved in new particle formation and the underlying mechanisms remain uncertain. Although sulfuric acid is commonly recognized as driving new particle formation, increasing evidence suggests the involvement of other species. Here we study particle formation and growth from methanesulfonic acid, trimethylamine and water at reaction times from 2.3 to 32 s where particles are 2-10 nm in diameter using a newly designed and tested flow system. The flow system has multiple inlets to facilitate changing the mixing sequence of gaseous precursors. The relative humidity and precursor concentrations, as well as the mixing sequence, are varied to explore their effects on particle formation and growth in order to provide insight into the important mechanistic steps. We show that water is involved in the formation of initial clusters, greatly enhancing their formation as well as growth into detectable size ranges. A kinetics box model is developed that quantitatively reproduces the experimental data under various conditions. Although the proposed scheme is not definitive, it suggests that incorporating such mechanisms into atmospheric models may be feasible in the near future.

摘要

由气体到颗粒的转化所导致的新颗粒形成是大气颗粒的主要来源,并且会影响辐射强迫、气候和人类健康。参与新颗粒形成的物种及其潜在机制仍不明确。尽管硫酸通常被认为是驱动新颗粒形成的因素,但越来越多的证据表明其他物种也参与其中。在此,我们使用新设计并经过测试的流动系统,研究了在2.3至32秒的反应时间内,甲磺酸、三甲胺和水形成颗粒及颗粒生长的情况,此时颗粒直径为2至10纳米。该流动系统有多个入口,便于改变气态前体的混合顺序。通过改变相对湿度、前体浓度以及混合顺序,来探究它们对颗粒形成和生长的影响,以便深入了解重要的机理步骤。我们发现水参与了初始团簇的形成,极大地促进了它们的形成以及生长到可检测的尺寸范围。我们开发了一个动力学箱式模型,该模型能定量再现各种条件下的实验数据。尽管所提出的方案并不确定,但它表明在不久的将来,将此类机制纳入大气模型可能是可行的。

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