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中国南方背景大气中高浓度颗粒结合咪唑的洞察:潜在来源及影响因素

Insights into high concentrations of particle-bound imidazoles in the background atmosphere of southern China: Potential sources and influencing factors.

作者信息

He Chunqian, Wang Hao, Gong Daocheng, Lv Shaojun, Wu Gengchen, Wang Ruiwen, Chen Yaqiu, Ding Yaozhou, Li Yanlei, Wang Boguang

机构信息

Institute for Environmental and Climate Research, Jinan University, Guangzhou, China; Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, China.

Institute for Environmental and Climate Research, Jinan University, Guangzhou, China; Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, China; Australia-China Centre for Air Quality Science and Management (Guangdong), Guangzhou, China.

出版信息

Sci Total Environ. 2022 Feb 1;806(Pt 4):150804. doi: 10.1016/j.scitotenv.2021.150804. Epub 2021 Oct 12.

Abstract

Imidazoles are important constituents in atmospheric brown carbon and have gained increasing attention in the past decade. Although imidazoles have been studied widely in laboratories, the sparse field observations severely limit the understanding of imidazole's abundance and sources in the atmosphere. In this study, we measured particle-bound imidazoles and their precursors at a background forest site in the Nanling Mountains of southern China. The average concentration of imidazoles (4.17 ± 3.76 ng/m) was found to be significantly higher than other background sites worldwide. Further analyses revealed that a majority of imidazoles (59.1%) at the site originated from secondary formation through reactions of dicarbonyls (e.g., glyoxal and methylglyoxal) and reduced nitrogen species, with relatively minor contributions from regional transport (32.8%) and biomass burning (8.1%). In addition, the key factors influencing secondary formation of imidazoles, such as relative humidity, water-soluble inorganic ions, and pH, were analyzed. Our results indicated that the secondary formation of imidazoles can be greatly enhanced under high humidity conditions, particularly during fog events. Overall, this study offers valuable insights into potential sources and influencing factors of ambient imidazoles in background atmospheres.

摘要

咪唑是大气棕碳的重要组成部分,在过去十年中受到越来越多的关注。尽管咪唑已在实验室中得到广泛研究,但稀疏的实地观测严重限制了对大气中咪唑丰度和来源的了解。在本研究中,我们在中国南方南岭山区的一个背景森林站点测量了颗粒态咪唑及其前体。发现咪唑的平均浓度(4.17±3.76纳克/立方米)显著高于全球其他背景站点。进一步分析表明,该站点大部分咪唑(59.1%)源自二羰基化合物(如乙二醛和甲基乙二醛)与还原态氮物种反应的二次生成,区域传输(32.8%)和生物质燃烧(8.1%)的贡献相对较小。此外,还分析了影响咪唑二次生成的关键因素,如相对湿度、水溶性无机离子和pH值。我们的结果表明,在高湿度条件下,尤其是在雾天期间,咪唑的二次生成会大大增强。总体而言,本研究为背景大气中环境咪唑的潜在来源和影响因素提供了有价值的见解。

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