The first UK measurements of nitryl chloride using a chemical ionization mass spectrometer in central London in the summer of 2012, and an investigation of the role of Cl atom oxidation

The first UK measurements of nitryl chloride using a chemical ionization mass spectrometer in central London in the summer of 2012, and an investigation of the role of Cl atom oxidation
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DOI:
10.1002/2014jd022629
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发表时间:
2015-06
期刊:
Journal of Geophysical Research: Atmospheres
影响因子:
--
通讯作者:
T. Bannan;A. M. Booth;A. Bacak;J. Muller;K. Leather;Michael Le Breton;B. Jones;D. Young;H. Coe;J. Allan;S. Visser;J. Slowik;M. Furger;A. Prevot;James D. Lee;R. Dunmore;J. Hopkins;J. Hamilton;A. Lewis;L. Whalley;T. Sharp;D. Stone;D. Heard;Z. Fleming;R. Leigh;D. Shallcross;C. Percival
T. Bannan;A. M. Booth;A. Bacak;J. Muller;K. Leather;Michael Le Breton;B. Jones;D. Young;H. Coe;J. Allan;S. Visser;J. Slowik;M. Furger;A. Prevot;James D. Lee;R. Dunmore;J. Hopkins;J. Hamilton;A. Lewis;L. Whalley;T. Sharp;D. Stone;D. Heard;Z. Fleming;R. Leigh;D. Shallcross;C. Percival
中科院分区:
其他
文献类型:
--
作者:
T. Bannan;A. M. Booth;A. Bacak;J. Muller;K. Leather;Michael Le Breton;B. Jones;D. Young;H. Coe;J. Allan;S. Visser;J. Slowik;M. Furger;A. Prevot;James D. Lee;R. Dunmore;J. Hopkins;J. Hamilton;A. Lewis;L. Whalley;T. Sharp;D. Stone;D. Heard;Z. Fleming;R. Leigh;D. Shallcross;C. Percival

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英国的第一个硝酰氯(ClNO2)测量是在2012年夏天的ClearfLo活动中使用化学电离质谱仪进行的,利用I−电离方案。ClNO2的浓度每晚都超过可检测限度(11 ppt),最高浓度为724 ppt。ClNO2的日变化曲线在凌晨4点到5点之间达到峰值,在日出后直接下降。在晚上8点和上午11点之间,通常观察到高于检测限的ClNO2浓度。ClNO2:N2O5的生产比例不同,这两种物质之间的正相关和负相关都有报道。ClNO2的光解和箱模型,利用修改后的主化学机制,包括氯化学计算氯原子浓度。使用低压激光诱导荧光和臭氧同时测量羟基自由基(OH),可以比较OH自由基、Cl原子和O3对三组测量的VOC(烷烃、烯烃和炔烃)氧化的相对重要性。对于一天的最大计算的Cl原子浓度,Cl原子在清晨是烷烃的主要氧化剂,并在整个一天,贡献了15%,3%和26%的烷烃,烯烃和炔烃的氧化,分别。
The first nitryl chloride (ClNO2) measurements in the UK were made during the summer 2012 ClearfLo campaign with a chemical ionization mass spectrometer, utilizing an I− ionization scheme. Concentrations of ClNO2 exceeded detectable limits (11 ppt) every night with a maximum concentration of 724 ppt. A diurnal profile of ClNO2 peaking between 4 and 5 A.M., decreasing directly after sunrise, was observed. Concentrations of ClNO2 above the detection limit are generally observed between 8 P.M. and 11 A.M. Different ratios of the production of ClNO2:N2O5 were observed throughout with both positive and negative correlations between the two species being reported. The photolysis of ClNO2 and a box model utilizing the Master Chemical Mechanism modified to include chlorine chemistry was used to calculate Cl atom concentrations. Simultaneous measurements of hydroxyl radicals (OH) using low pressure laser‐induced fluorescence and ozone enabled the relative importance of the oxidation of three groups of measured VOCs (alkanes, alkenes, and alkynes) by OH radicals, Cl atoms, and O3 to be compared. For the day with the maximum calculated Cl atom concentration, Cl atoms in the early morning were the dominant oxidant for alkanes and, over the entire day, contributed 15%, 3%, and 26% toward the oxidation of alkanes, alkenes, and alkynes, respectively.