Volatility basis-set approach simulation of organic aerosol formation in East Asia: implications for anthropogenic–biogenic interaction and controllable amounts
Volatility basis-set approach simulation of organic aerosol formation in East Asia: implications for anthropogenic–biogenic interaction and controllable amounts
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DOI：
10.5194/acp-14-9513-2014
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发表时间：
2014-04
影响因子：
6.3
通讯作者：
H. Matsui;M. Koike;Y. Kondo;A. Takami;J. Fast;Y. Kanaya;M. Takigawa
中科院分区：
文献类型：
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作者：
H. Matsui;M. Koike;Y. Kondo;A. Takami;J. Fast;Y. Kanaya;M. Takigawa
抽象的。采用挥发性基组方法对东亚及其外流区进行了有机气溶胶(OA)模拟。模式模拟通过与东京及其周围地区(2003年和2004年夏季在小叶和溪西)以及东亚外流区(2009年春季在福岛和和岛)的气溶胶质谱仪测量的光学系数进行比较来评估模式模拟。对有机蒸气老化过程的模拟相当好地再现了所有地点观测到的OA的质量浓度、时间变化和形成效率。由于在没有老化过程的模拟中严重低估了OA的质量，有机蒸汽的氧化对于东亚地区合理的OA模拟是必不可少的。在考虑老化过程的情况下，整个东亚地区边界层中模拟的OA浓度从0.2 4μg m−3增加到1.2 8 ppm。由人为和生物来源相互作用形成的骨性关节炎也因老化过程而增强。在整个东亚地区，可控性OA的比例估计为总OA的87%，这表明我们模拟中的大部分OA是人为形成的(来自可控燃烧源)。很大一部分生物性继发性骨关节炎(78%)是在人为因素的影响下形成的。这些分数高于人为排放的分数。这些较高的可控组分的一个重要原因是较高的氧化剂浓度，以及考虑到人为来源导致的较快的OA前体的氧化速度。在东亚地区，有机蒸气的老化过程增加了可控酸的含量(从0.18到1.12μg m−3)和比例(从75%到87%)。
Abstract. Organic aerosol (OA) simulations using the volatility basis-set approach were made for East Asia and its outflow region. Model simulations were evaluated through comparisons with OA measured by aerosol mass spectrometers in and around Tokyo (at Komaba and Kisai in summer 2003 and 2004) and over the outflow region in East Asia (at Fukue and Hedo in spring 2009). The simulations with aging processes of organic vapors reproduced the mass concentrations, temporal variations, and formation efficiencies of observed OA at all of the sites reasonably well. As OA mass was severely underestimated in the simulations without the aging processes, the oxidations of organic vapors are essential for reasonable OA simulations over East Asia. By considering the aging processes, simulated OA concentrations increased from 0.24 to 1.28 μg m−3 in the boundary layer over the whole of East Asia. OA formed from the interaction of anthropogenic and biogenic sources was also enhanced by the aging processes. The fraction of controllable OA was estimated to be 87% of total OA over the whole of East Asia, which indicated that most of the OA in our simulations were formed anthropogenically (from controllable combustion sources). A large portion of biogenic secondary OA (78% of biogenic secondary OA) was formed through the influence of anthropogenic sources. These fractions were higher than the fraction of anthropogenic emissions. An important reason for these higher controllable fractions was higher oxidant concentrations and the resulting faster oxidation rates of OA precursors by considering anthropogenic sources. Both the amounts (from 0.18 to 1.12 μg m−3) and the fraction (from 75 to 87%) of controllable OA were increased by aging processes of organic vapors over East Asia.