Nitrate formation from heterogeneous uptake of dinitrogen pentoxide during a severe winter haze in southern China
Nitrate formation from heterogeneous uptake of dinitrogen pentoxide during a severe winter haze in southern China
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中国南方严重冬季雾霾期间五氧化二氮的异质吸收形成硝酸盐
DOI：
10.5194/acp-18-17515-2018
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发表时间：
2018-08
影响因子：
6.3
通讯作者：
Zhou Y.
中科院分区：
文献类型：
--
作者：
Yun H.;Wang W.;Wang T.;Xia M.;Yu C.;Wang Z.;C. N. Poon S.;Yue D.;Zhou Y.
硝酸盐（NO3-）已成为我国雾霾天细颗粒物（PM2.5）的主要组成成分。然而，五氧化二氮（N2 O 5）在硝酸盐形成中的非均相反应的作用并没有得到很好的限制。2017年1月，中国南方的珠江三角洲（PRD）发生了一次严重的雾霾事件，期间在珠江三角洲西部的一个半农村地区（鹤山）观测到高水平的PM2.5（约400 µg m−3）和O3（约160 ppbv）。硝酸盐浓度达到108 µg m−3（1小时时间分辨率），硝酸盐对PM2.5的贡献接近40%。同时增加NO3-和ClNO 2（在1分钟的时间分辨率的最大值为8.3 ppbv），观察在日落后的头几个小时，表明强烈的N2 O 5的非均匀吸收气溶胶。根据测量数据，在日落后的凌晨（2至6小时），通过N2 O 5非均相反应生成NO3-的可能性估计为29.0至77.3 µg m−3，这可以完全解释在同一时间段内测量到的NO3-浓度的增加。利用主化学反应机理（MCM v3.3.1）建立的化学箱模型计算了白天由OH+NO2气相反应生成硝酸的过程，并以测量数据为约束条件。通过N2 O 5化学形成的综合夜间硝酸盐与白天形成的硝酸相当或甚至更高。这项研究证实，N2 O 5的非均相化学是一个显着的来源，气溶胶硝酸盐在中国南方的雾霾天。
Nitrate (NO3-) has become a major component of fine particulate matter (PM2.5) during hazy days in China. However, the role of the heterogeneous reactions of dinitrogen pentoxide (N2O5) in nitrate formation is not well constrained. In January 2017, a severe haze event occurred in the Pearl River Delta (PRD) of southern China during which high levels of PM2.5 (∼400 µg m−3) and O3 (∼160 ppbv) were observed at a semi-rural site (Heshan) in the western PRD. Nitrate concentrations reached 108 µg m−3 (1 h time resolution), and the contribution of nitrate to PM2.5 was nearly 40 %. Concurrent increases in NO3- and ClNO2 (with a maximum value of 8.3 ppbv at a 1 min time resolution) were observed in the first several hours after sunset, indicating an intense N2O5 heterogeneous uptake by aerosols. The formation potential of NO3- via N2O5 heterogeneous reactions was estimated to be between 29.0 and 77.3 µg m−3 in the early hours (2 to 6 h) after sunset based on the measurement data, which could completely explain the measured increase in the NO3- concentration during the same time period. Daytime production of nitric acid from the gas-phase reaction of OH+NO2 was calculated with a chemical box model built using the Master Chemical Mechanism (MCM v3.3.1) and constrained by the measurement data. The integrated nocturnal nitrate formed via N2O5 chemistry was comparable to or even higher than the nitric acid formed during the day. This study confirms that N2O5 heterogeneous chemistry was a significant source of aerosol nitrate during hazy days in southern China.
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