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2017年1月中国南方严重雾霾期间有机气溶胶及其前体物的特征分析

Characterization of organic aerosols and their precursors in southern China during a severe haze episode in January 2017.

作者信息

Chang Di, Wang Zhe, Guo Jia, Li Tao, Liang Yiheng, Kang Lingyan, Xia Men, Wang Yaru, Yu Chuan, Yun Hui, Yue Dingli, Wang Tao

机构信息

Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hong Kong, China.

Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hong Kong, China.

出版信息

Sci Total Environ. 2019 Nov 15;691:101-111. doi: 10.1016/j.scitotenv.2019.07.123. Epub 2019 Jul 9.

Abstract

The rapid industrialization and economic development in the Pearl River Delta (PRD) region of southern China have led to a substantial increase in anthropogenic emissions and hence frequent haze pollution over the past two decades. In early January 2017, a severe regional haze pollution episode was captured in the PRD region, with a peak PM concentration of around 400μgm, the highest value ever reported at this site. During the haze episode, elevated concentrations of oxygenated volatile organic compounds (OVOCs, 33±16 ppbv) and organic matter (41±15μg m) were observed, indicating the enhanced roles of secondary organic aerosols (SOAs) in the formation of haze pollution. Water-soluble organic carbon (WSOC, 12.8±5.5μg C m) dominated the organic aerosols, with a WSOC/OC ratio of 0.63±0.12 and high correlation (R=0.85) with estimated secondary organic carbon (SOC), suggesting the predominance of a secondary origin of the measured organic aerosols during the haze episode. Four carboxylic acids (oxalic, acetic, formic, and pyruvic acids) were characterized in the aerosols (1.30±0.38μgm) and accounted for 3.6±1.2% of WSOC in carbon mass, with oxalic acid as the most abundant species. The simultaneous measurements of volatile organic compounds (VOCs), OVOCs, and organic acids in aerosols at this site provided an opportunity to investigate the relationship between the precursors and the products, as well as the potential formation pathways. Water-soluble aldehydes and ketones, predominantly produced via the oxidation of anthropogenic VOCs (mainly propane, toluene, n-butane, and m, p-xylene), were the main contributors of the organic acids. The formation of OVOCs is largely attributed to gas-phase photochemical oxidation, whereas the WSOC and dicarboxylic acids were produced from both photochemistry and nocturnal heterogeneous reactions. These findings provided further insights into the oxidation and evolution of organic compounds during the haze pollution episode.

摘要

中国南方珠江三角洲(PRD)地区的快速工业化和经济发展导致过去二十年来人为排放量大幅增加,从而频繁出现雾霾污染。2017年1月初,珠江三角洲地区遭遇了一次严重的区域性雾霾污染事件,颗粒物浓度峰值约为400μg/m³,是该监测点有记录以来的最高值。在雾霾期间,观测到氧化挥发性有机化合物(OVOCs,33±16 ppbv)和有机物(41±15μg/m³)浓度升高,表明二次有机气溶胶(SOAs)在雾霾污染形成中发挥了更大作用。水溶性有机碳(WSOC,12.8±5.5μg C/m³)在有机气溶胶中占主导地位,WSOC/OC比值为0.63±0.12,与估算的二次有机碳(SOC)具有高度相关性(R=0.85),这表明在雾霾期间所测有机气溶胶主要来源于二次生成。在气溶胶中鉴定出四种羧酸(草酸、乙酸、甲酸和丙酮酸)(1.30±0.38μg/m³),占WSOC碳质量的3.6±1.2%,其中草酸含量最高。该监测点对气溶胶中挥发性有机化合物(VOCs)、OVOCs和有机酸的同步测量为研究前体物与产物之间的关系以及潜在的形成途径提供了契机。水溶性醛类和酮类主要通过人为VOCs(主要是丙烷、甲苯、正丁烷和间、对二甲苯)的氧化产生,是有机酸的主要来源。OVOCs的形成主要归因于气相光化学氧化,而WSOC和二元羧酸则由光化学和夜间非均相反应共同产生。这些发现为雾霾污染事件期间有机化合物的氧化和演变提供了进一步的见解。

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