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春季/夏季首尔都会区大气硫酸盐形成:痕量金属离子的影响。

Atmospheric sulfate formation in the Seoul Metropolitan Area during spring/summer: Effect of trace metal ions.

机构信息

Department of Environmental Health Sciences, Graduate School of Public Health, Seoul National University, 08826, Seoul, Republic of Korea.

Department of Atmospheric Sciences, Yonsei University, 03722, Seoul, Republic of Korea.

出版信息

Environ Pollut. 2022 Dec 15;315:120379. doi: 10.1016/j.envpol.2022.120379. Epub 2022 Oct 12.

Abstract

Despite the effort to control SO emission, sulfate is still one of the major inorganic components of PM in urban area. Moreover, there is still a lack of understanding of the sulfate formation mechanism via SO oxidation under various ambient conditions. In this study, we focus on sulfate formation during a haze pollution episode in the spring/summertime of 2016 in Seoul Metropolitan Area (SMA). During the pollution episode, PM mass concentration exceeded over 60 μg m, and sulfate accounted for about 25% of the total PM mass concentration. A sharp increase of sulfur oxidation ratio (SOR) values along with aerosol liquid water content (AWC) under humid conditions could be ascribed to an apparent contribution of aqueous-phase oxidation of SO of sulfate formation during the pollution period. Comparisons of SOR values with four representative oxidants for the aqueous-phase oxidation (i.e., NO, HO, O, and TMIs) indicated that TMIs concentration, especially for Mn (II), showed the best positive correlation. Furthermore, for calculating the sulfate production rate, the contribution of TMIs concentration was found to be dominant within the pH range in SMA (2.1-3.0), which was determined by the chemical composition and derived AWC. These results imply that not only the SO emission but also other chemical components (e.g., TMI and nitrate) would play a critical combined role in sulfate formation under urban haze condition.

摘要

尽管努力控制 SO 排放,但硫酸盐仍然是城市地区 PM 中主要的无机成分之一。此外,对于在各种环境条件下通过 SO 氧化形成硫酸盐的机制,我们仍然缺乏了解。在本研究中,我们关注了 2016 年春季/夏季首尔都会区(SMA)雾霾污染期间硫酸盐的形成。在污染期间,PM 质量浓度超过 60μg/m,硫酸盐约占总 PM 质量浓度的 25%。在潮湿条件下,随着气溶胶液水含量(AWC)的增加,硫氧化比(SOR)值急剧上升,这可能归因于在污染期间硫酸盐形成过程中 SO 的水相氧化对硫酸盐形成的明显贡献。将 SOR 值与四种代表性的水相氧化剂(即 NO、HO、O 和 TMIs)进行比较表明,TMIs 浓度,特别是 Mn(II),表现出最好的正相关。此外,对于计算硫酸盐生成速率,在 SMA 的 pH 值范围内(2.1-3.0),TMIs 浓度的贡献是主要的,这是由化学成分和推导的 AWC 决定的。这些结果表明,不仅 SO 排放,而且其他化学成分(例如 TMI 和硝酸盐)在城市雾霾条件下对硫酸盐的形成将发挥关键的综合作用。

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