Formation and transport of oxidized reactive nitrogen, ozone, and secondary organic aerosol in Tokyo

Formation and transport of oxidized reactive nitrogen, ozone, and secondary organic aerosol in Tokyo
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DOI:
10.1029/2008jd010134
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发表时间:
2008-11
影响因子:
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通讯作者:
Y. Kondo;Y. Morino;M. Fukuda;Y. Kanaya;Y. Miyazaki;N. Takegawa;H. Tanimoto;R. McKenzie;P. Johns
Y. Kondo;Y. Morino;M. Fukuda;Y. Kanaya;Y. Miyazaki;N. Takegawa;H. Tanimoto;R. McKenzie;P. Johns
中科院分区:
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文献类型:
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作者:
Y. Kondo;Y. Morino;M. Fukuda;Y. Kanaya;Y. Miyazaki;N. Takegawa;H. Tanimoto;R. McKenzie;P. Johns

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[1]在2003-2004年的不同季节,对东京市中心附近的主要活性氮物种(NOy)i(NOx、过氧酰基硝酸盐、HNO 3和颗粒硝酸盐(NO3−))、总活性氮(NOy)、挥发性有机化合物、OH和HO 2以及有机气溶胶进行了测量,以研究涉及活性氮和O3氧化形式的过程。一般来说,氮氧化物构成了整个季节的NOy占主导地位的部分。NOx/NOy和HNO 3/NOy比值在夏季最低和最高,分别是由于季节性高OH浓度。在夏季和秋季,随着NOx/NOy比值的降低,排放后残留在大气中的NOy分数(RNOy)逐渐降低。Ox = O3 + NO2的平均季节日变化可能受背景O3水平、光化学O3形成和垂直输送的控制。2004年8月中旬,在停滞的情况下,牛在中午出现大幅增长。用箱形模型计算的原地生产率太慢,无法解释观察到的增加。高Ox可能是由于前几天的Ox在边界层(BL)的上部积累,然后在日出后通过混合向下输送到表面附近。考虑到Ox与二次有机气溶胶(SOA)之间的密切相关性,很可能SOA也积累在海陆风环流过程中的BL。
[1] Measurements of the major reactive nitrogen species (NOy)i (NOx, peroxyacyl nitrates, HNO3, and particulate nitrate (NO3−)), total reactive nitrogen (NOy), volatile organic compounds, OH and HO2, and organic aerosol were made near the urban center of Tokyo in different seasons of 2003–2004 to study the processes involving oxidized forms of reactive nitrogen and O3. Generally, NOx constituted the dominant fraction of NOy throughout the seasons. The NOx/NOy and HNO3/NOy ratios were lowest and highest, respectively, in summer, owing to the seasonally high OH concentration. The fraction of NOy that remained in the atmosphere after emission (RNOy) decreased with the decrease in the NOx/NOy ratio in summer and fall. It is likely that the median seasonal-diurnal variations of Ox = O3 + NO2 were controlled by those of the background O3 levels, photochemical O3 formation, and vertical transport. Ox showed large increases during midday under stagnant conditions in mid-August 2004. Their in situ production rates calculated by a box model were too slow to explain the observed increases. The high Ox was likely due to the accumulation of Ox from previous days in the upper part of the boundary layer (BL) followed by transport down to near the surface by mixing after sunrise. Considering the tight correlation between Ox and secondary organic aerosol (SOA), it is likely that SOA also accumulated during the course of sea-land breeze circulation in the BL.