Aqueous-phase reactions occurred in the PM2.5 cumulative explosive growth during the heavy pollution episode (HPE) in 2016 Beijing wintertime

Lingyan Wu, Junying Sun, Xiaoye Zhang, Yangmei Zhang, Yaqiang Wang, J. Zhong, Yun Yang
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引用次数: 19

Abstract

Abstract A heavy pollution episode (HPE) that lasted for seven days occurred over the North China Plain in December 2016. An in situ Ambient Ion Monitor was applied to analyze the chemical composition of PM2.5 (fine particulate matter with diameters less than 2.5 µm) and gaseous HONO concentration during that event. A representative explosive growth in the pollution cumulative stage was selected to investigate the pollution mechanism during the HPE in Beijing. PM2.5 cumulative explosive growth processes were observed to occur commonly under high relative humidity (RH) condition. Our results demonstrated that the aqueous-phase oxidation of SO2 by NO2 to sulfate could contribute to the cumulative explosive growth. Nitrate produced by secondary formation was another factor in the growth of PM2.5. Depending on the relative humidity, temperature, and chemical species, the deliquescence relative humidity was calculated to 82%, 81%, and 83% for (NH4)2SO4, NH4NO3, and NH4Cl, respectively. The preexisting PM2.5 surface changed from solid to liquid when RH > 81%. Coincidentally, both the sulfur oxidation ratio (SOR) and reaction product HONO displayed an evident exponential relationship with RH and increased more quickly when RH was larger than 80%. In addition, sufficiently excessive NO2 made the aqueous-phase oxidation of SO2 efficiently proceed even at relative low SO2 concentrations (below 15 µg m−3). Potential H+ in the reactions was neutralized by NH3, resulting in fully neutralized PM2.5 during HPE. The chemical evolution of these reactions was discussed in detail in this study.
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2016年北京冬季重污染事件(HPE)期间PM2.5累积爆发性增长发生了水相反应
2016年12月,华北平原发生了一次持续7天的重污染事件。使用现场环境离子监测仪分析了该事件期间PM2.5(直径小于2.5µm的细颗粒物)的化学成分和气态HONO浓度。选取具有代表性的污染累积阶段的爆发性增长为研究对象,探讨了北京HPE期间的污染机制。在高相对湿度条件下,PM2.5的累积爆发性生长过程较为常见。研究结果表明,NO2水相氧化SO2生成硫酸盐有助于累积爆发性生长。次生形成产生的硝酸盐是PM2.5增长的另一个因素。根据相对湿度、温度和化学物质的不同,计算得出(NH4)2SO4、NH4NO3和NH4Cl的潮解相对湿度分别为82%、81%和83%。当相对湿度> 81%时,原有PM2.5表面由固体变为液体。巧合的是,硫氧化比(SOR)和反应产物HONO均与RH呈明显的指数关系,且当RH大于80%时,其增加速度更快。此外,足够过量的NO2使SO2的水相氧化即使在相对较低的SO2浓度(低于15µg m−3)下也能有效地进行。反应中的电位H+被NH3中和,导致HPE过程中PM2.5完全中和。本文详细讨论了这些反应的化学演化过程。
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