Seasonal and geographical variability of nitryl chloride and its precursors in Northern Europe
Seasonal and geographical variability of nitryl chloride and its precursors in Northern Europe
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DOI：
10.1002/asl.844
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发表时间：
2018-08
影响因子：
3
通讯作者：
R. Sommariva;L. Hollis;T. Sherwen;A. Baker;S. Ball;B. Bandy;T. Bell;M. N. Chowdhury;R. Cordell;M. J. Evans;James D. Lee;C. Reed;C. Reeves;J. Roberts;Mingxi Yang;P. Monks
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文献类型：
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作者：
R. Sommariva;L. Hollis;T. Sherwen;A. Baker;S. Ball;B. Bandy;T. Bell;M. N. Chowdhury;R. Cordell;M. J. Evans;James D. Lee;C. Reed;C. Reeves;J. Roberts;Mingxi Yang;P. Monks
2014-2016年，在英国的三个对比鲜明的地点进行了硝酰氯（ClNO 2）及其前体（O3，NO2，颗粒氯化物）的测量：莱斯特，Penlee Point和Weybourne。在所有地点和每个季节都观察到ClNO 2，最高浓度在格林尼治标准时间00：00至04：00之间。夜间ClNO 2浓度的中位数介于检测限（4.2 ppt）和139 ppt之间。一个明确的季节性周期，在春季和冬季的最大值，并在同一季节的位置之间的显着差异进行了观察。氯化物颗粒的主要来源是海盐气溶胶（包括距离海岸约200公里的莱斯特）。在一般情况下，ClNO 2水平控制的O3和NO2的浓度，而不是通过吸收和反应的N2 O 5与颗粒氯化物。在这些条件下，ClNO 2的季节性和地理分布可以用影响N2 O 5前体形成的O3限制和NO2限制机制来解释。中等分辨率（2° × 2.5°）的全球版本的GEOS‐Chem模型无法完全捕捉到观测到的ClNO 2的季节性，主要是因为该模型高估了前体物质的浓度，特别是夜间O3的浓度。更高分辨率（0.25° × 0.3125°）版本的GEOS‐Chem显示与观测结果的一致性更好，尽管它仍然高估了夏季的ClNO 2浓度。
Measurements of nitryl chloride (ClNO2) and its precursors (O3, NO2, particulate chloride) were made in 2014–2016 at three contrasting locations in the United Kingdom: Leicester, Penlee Point and Weybourne. ClNO2 was observed at all sites and in every season, with the highest concentrations between 00:00 and 04:00 GMT. The median nocturnal concentration of ClNO2 ranged between the detection limit (4.2 ppt) and 139 ppt. A clear seasonal cycle, with maxima in spring and winter, and significant differences between locations in the same season were observed. The main source of particulate chloride was sea salt aerosol (including at Leicester, ∼200 km from the coast). In general, ClNO2 levels were controlled by the concentrations of O3 and NO2, rather than by the uptake and reaction of N2O5 with particulate chloride. Under these conditions, the seasonality and geographical distribution of ClNO2 can be explained in terms of O3‐limited and NO2‐limited regimes affecting the formation of the N2O5 precursor. A global version of the GEOS‐Chem model at medium resolution (2° × 2.5°) was not able to fully capture the observed seasonality of ClNO2, mostly because the model overestimated the concentrations of the precursors, particularly of nocturnal O3. A higher‐resolution (0.25° × 0.3125°) version of GEOS‐Chem showed better agreement with the observations, although it still overestimated ClNO2 concentrations during summer.