Summertime NO x measurements during the CHABLIS campaign: can source and sink estimates unravel observed diurnal cycles?

Summertime NO x measurements during the CHABLIS campaign: can source and sink estimates unravel observed diurnal cycles?
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夏布利 (Chablis) 活动期间的夏季氮氧化物测量:源和汇估算能否揭示观测到的昼夜循环?

DOI:
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发表时间:
2009
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影响因子:
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通讯作者:
J. Plane
J. Plane
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作者:
S. Bauguitte;W. Bloss;M. J. Evans;R. Salmon;P. Anderson;A. Jones;James D. Lee;A. Saiz‐Lopez;H. Roscoe;E. Wolff;J. Plane

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NOx 测量是在 2005 年 1 月 1 日至 2 月 10 日的南方夏季期间在南极洲沿海哈雷研究站进行的。观察到明显的 NOx 昼夜周期,在格林尼治标准时间 04:00 至 05:00 之间测得的最低浓度接近仪器检测限 (5 pptv)。 NOx 浓度在 19:00–20:00 GMT 之间达到峰值 (24 pptv),大约在当地太阳正午后 5 小时。基于雪中硝酸盐光解和化学损失产生的氮氧化物浓度的优化盒模型得出平均中午排放率为 3.48 × 108 摩尔 cm−2 s−1,假设边界层混合高度为 100 m,氮氧化物寿命相对较短,约为 6.4 小时。该排放率与研究期结束时 3 天的直接测量值(范围为 2.1 至 12.6 × 108 molec cm−2 s−1)进行比较。通过各种传统的 HOx 和卤素氧化过程对 NO2 最大损失率的计算表明,NOx 的寿命主要由卤素处理控制,即 BrNO3 和 INO3 气相形成及其随后的异质吸收。此外,卤氧化物的存在会降低 NO/NO2 比率,从而显着扰乱 NOx 浓度。我们得出的结论是,在南极洲沿海,由于卤素硝酸盐水解导致的氮氧化物损失更快,从而降低了积雪排放的氮氧化物的潜在臭氧生产效率。
NOx measurements were conducted at the Halley Research Station, coastal Antarctica, during the austral summer period 1 January–10 February 2005. A clear NOx diurnal cycle was observed with minimum concentrations close to instrumental detection limit (5 pptv) measured between 04:00–05:00 GMT. NOx concentrations peaked (24 pptv) between 19:00–20:00 GMT, approximately 5 h after local solar noon. An optimised box model of NOx concentrations based on production from in-snow nitrate photolysis and chemical loss derives a mean noon emission rate of 3.48 × 108 molec cm−2 s−1, assuming a 100 m boundary layer mixing height, and a relatively short NOx lifetime of ~6.4 h. This emission rate compares to directly measured values ranging from 2.1 to 12.6 × 108 molec cm−2 s−1 made on 3 days at the end of the study period. Calculations of the maximum rate of NO2 loss via a variety of conventional HOx and halogen oxidation processes show that the lifetime of NOx is predominantly controlled by halogen processing, namely BrNO3 and INO3 gas-phase formation and their subsequent heterogeneous uptake. Furthermore the presence of halogen oxides is shown to significantly perturb NOx concentrations by decreasing the NO/NO2 ratio. We conclude that in coastal Antarctica, the potential ozone production efficiency of NOx emitted from the snowpack is mitigated by the more rapid NOx loss due to halogen nitrate hydrolysis.
DOI: 10.1038/nature07035
发表时间: 2008-06-26
期刊: NATURE
影响因子: 64.8
作者:
Read, Katie A.;Mahajan, Anoop S.;Plane, John M. C.
通讯作者: Plane, John M. C.