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基于中国郑州雾霾期和降雪期高时间分辨率数据对二次无机气溶胶形成的深入了解。

Insight into the formation of secondary inorganic aerosol based on high-time-resolution data during haze episodes and snowfall periods in Zhengzhou, China.

机构信息

Research Institute of Environmental Science, College of Chemistry and Molecular Engineering, Zhengzhou University, Zhengzhou 450001, China.

Research Institute of Environmental Science, College of Chemistry and Molecular Engineering, Zhengzhou University, Zhengzhou 450001, China.

出版信息

Sci Total Environ. 2019 Apr 10;660:47-56. doi: 10.1016/j.scitotenv.2018.12.465. Epub 2019 Jan 4.

DOI:10.1016/j.scitotenv.2018.12.465
PMID:30639718
Abstract

Episodic haze is frequently observed in Zhengzhou, China. Such haze typically contains secondary inorganic aerosols. In this paper, we explore the formation mechanisms of sulfate, nitrate, and ammonium (SNA) in Zhengzhou from January 3 to 25, 2018 based on the results of a series of online instruments and a size-segregated filter sampler. Our results document the remarkable contributions of SNA to winter haze episodes in Zhengzhou, where they account for about 50% of PM mass concentration. SNA were mainly concentrated in droplet-mode particles, which increased remarkably with the aggravation of the haze episode. In addition, KNO and NaNO were formed in droplet-mode particles and coarse-mode particles respectively with increasing PM concentration. The atmosphere during the observation period was ammonia-rich, and the aerosol was acidic under high PM concentration. Homogeneous reactions dominated the formation of nitrate. HONO photolysis played a more important role in the origin of OH radicals when O decreased during haze episode. Under high relative humidity (RH), nitrate formation was influenced by heterogeneous hydrolysis reactions of NO. Sulfates were mainly formed through aqueous-phase reactions, especially when the RH was higher than 60%. Under these conditions, there were amounts of liquid water content existed in aerosols. Finally, we observed enhanced conversion of SO and NO during snowfall periods. This effect may be attributable to the higher RH and O levels despite the unfavorable effects of wet deposition and low concentrations of gaseous precursors.

摘要

中国郑州经常出现间歇性雾霾。这种雾霾通常含有二次无机气溶胶。本文基于一系列在线仪器和分级滤膜采样器的结果,探讨了 2018 年 1 月 3 日至 25 日郑州硫酸盐、硝酸盐和铵(SNA)的形成机制。研究结果表明,SNA 对郑州冬季雾霾事件有显著贡献,其占 PM 质量浓度的 50%左右。SNA 主要集中在液滴模态粒子中,随着雾霾事件的加剧,其浓度显著增加。此外,随着 PM 浓度的增加,KNO 和 NaNO 分别在液滴模态粒子和粗模态粒子中形成。观测期间大气中氨含量较高,在高 PM 浓度下气溶胶呈酸性。均相反应主导硝酸盐的形成。当 O 在雾霾事件中减少时,HONO 光解在 OH 自由基的起源中发挥了更重要的作用。在高相对湿度(RH)下,NO 的非均相水解反应影响硝酸盐的形成。硫酸盐主要通过水相反应形成,特别是在 RH 高于 60%时。在这些条件下,气溶胶中存在大量液态水含量。最后,我们观察到降雪期间 SO 和 NO 的转化率增强。尽管湿沉降和气体前体浓度较低会产生不利影响,但这种效应可能归因于较高的 RH 和 O 水平。

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