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中国东南部11个城市站点气态羰基化合物的时空模式及臭氧敏感性

Spatiotemporal patterns and ozone sensitivity of gaseous carbonyls at eleven urban sites in southeastern China.

作者信息

Zhang Xin, Wu Zhenhai, He Zhen, Zhong Xuefen, Bi Fang, Li Yunfeng, Gao Rui, Li Hong, Wang Wenxing

机构信息

State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China; Environment Research Institute, Shandong University, Qingdao 266237, China.

State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China.

出版信息

Sci Total Environ. 2022 Jun 10;824:153719. doi: 10.1016/j.scitotenv.2022.153719. Epub 2022 Feb 8.

DOI:10.1016/j.scitotenv.2022.153719
PMID:35149078
Abstract

Gaseous carbonyls are essential trace gases for tropospheric chemistry and contribute significantly to the formation of ambient air ozone (O) in densely populated regions, especially in China. Pollution characterization and the analysis of O, nitrogen oxides, and volatile organic compounds (O-NO-VOCs) sensitivities of carbonyls were investigated from October 22 to 28, 2018 at eleven urban sites in nine cities in Fujian Province, southeastern China. The total mixing ratios of 15 kinds of gaseous carbonyls (Σ15OVOCs) was 12.15 ± 2.53 ppbv in Fujian Province. The concentrations in the eastern coastal regions were higher than those in the western mountainous regions. Formaldehyde, acetone, and acetaldehyde were the top three species of Σ15OVOCs concentration. Photochemical formation during the daytime and vehicle emission during the rush hours significantly contributed to formaldehyde and acetaldehyde. The shoe-making industry is well developed in Putian, where the acetone mixing ratio was significantly higher than in other cities. The O-NO-VOCs sensitivities at all urban sites were in VOC-limited or transitional regimes based on the ratios of formaldehyde to NO; from morning to afternoon, the VOC-limited sensitivity decreased, and the NO-limited sensitivity increased gradually. Formaldehyde contributed the most significant O formation potential (OFP) proportion of the Σ15OVOCs. The OFP of carbonyl species accounted for half of the total VOCs in Fuzhou and Putian, suggesting that more attention needs to be given to gaseous carbonyls control. Overall, the links inferred by this study provide evidence and clues to mitigate the increasing ambient O concentration on the west coast of the Taiwan Strait.

摘要

气态羰基化合物是对流层化学中的重要痕量气体,对人口密集地区(尤其是中国)的环境空气中臭氧(O₃)的形成有重大贡献。2018年10月22日至28日,在中国东南部福建省九个城市的11个城市站点,对羰基化合物的污染特征以及O₃、氮氧化物和挥发性有机化合物(O₃-NOₓ-VOCs)敏感性进行了调查。福建省15种气态羰基化合物(Σ₁₅OVOCs)的总混合比为12.15±2.53 ppbv。东部沿海地区的浓度高于西部山区。甲醛、丙酮和乙醛是Σ₁₅OVOCs浓度最高的前三种物质。白天的光化学形成和高峰时段的车辆排放对甲醛和乙醛有显著贡献。莆田的制鞋业发达,其丙酮混合比明显高于其他城市。根据甲醛与NO的比值,所有城市站点的O₃-NOₓ-VOCs敏感性均处于VOC限制或过渡状态;从上午到下午,VOC限制敏感性降低,NO限制敏感性逐渐增加。甲醛对Σ₁₅OVOCs的O₃形成潜力(OFP)贡献比例最大。羰基化合物的OFP在福州和莆田占总VOCs的一半,这表明需要更加关注气态羰基化合物的控制。总体而言,本研究推断的联系为缓解台湾海峡西海岸环境O₃浓度上升提供了证据和线索。

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