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中国西部兰州市石化工业区挥发性有机化合物的化学反应活性及其对臭氧形成的影响。

Chemical reactivity of volatile organic compounds and their effects on ozone formation in a petrochemical industrial area of Lanzhou, Western China.

作者信息

Guo Wenkai, Yang Yanping, Chen Qiang, Zhu Yuhuan, Zhang Yaru, Zhang Yingnan, Liu Yongle, Li Guangyao, Sun Wei, She Jing

机构信息

Key Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, China.

Key Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, China; Northwest Institute of Eco-environmental Resources, Chinese Academy of Sciences, Lanzhou 730000, China; Gansu Environmental Monitoring Center, Lanzhou 730000, China.

出版信息

Sci Total Environ. 2022 Sep 15;839:155901. doi: 10.1016/j.scitotenv.2022.155901. Epub 2022 May 12.

Abstract

Measurements of ozone (O) and its precursors were performed in the summer of 2019 in Lanzhou, a petrochemical industrial city, to better understand the reactivity of volatile organic compounds (VOCs) and their effects on O production. During the campaign, the daily maximum 8-hour average (MDA8) O, NO, and total VOC (TVOC) concentrations reached 72.2 ± 19.9 ppb, 24.9 ± 10.8 ppb, and 50.8 ± 46.1 ppb, respectively. Alkanes, alkenes, halocarbons, aromatics, and alkynes contributed 45.3%, 24.0%, 16.5%, 10.0%, and 4.2% to TVOCs, respectively. The OH reactivity and relative incremental reactivity (RIR) of VOCs at different times were calculated. The results indicated that alkenes played a predominant role, accounting for an average of 68.5% of the initial VOC reactivity. Compared to other regions, alkenes are relatively more important for O formation in the petrochemical industry area of Lanzhou, while aromatics are relatively less important. Generally, O formation occurred in a VOC-limited regime in the morning and in a transitional regime in the afternoon. The response surface methodology (RSM) combined with a chemical box model was applied to obtain relationships between O and its precursors and determine the most effective way to reduce the O concentration. Reduction in the non-alkene concentration slightly affected the O concentration. In contrast, the effect of nitrogen oxides (NO) was closely related to the alkene concentration, and NO concentration reduction could lead to an increase in the O concentration when alkenes were abated to less than 80% of the present concentration. To mitigate O pollution near the petrochemical industrial area of Lanzhou, reducing the alkene concentration, especially the C4 alkene concentration (1,3-butadiene, cis-2-butene, and trans-2-butene), was the fastest and most effective control strategy. The results of this study serve as a reference for O pollution control in petrochemical industrial areas.

摘要

在 2019 年夏季,我们在石化工业城市兰州进行了臭氧(O)及其前体物的测量,以更好地了解挥发性有机化合物(VOCs)的反应性及其对 O 生成的影响。在研究期间,每日最大 8 小时平均值(MDA8)臭氧、NO 和总挥发性有机化合物(TVOC)浓度分别达到 72.2±19.9 ppb、24.9±10.8 ppb 和 50.8±46.1 ppb。烷烃、烯烃、卤代烃、芳烃和炔烃分别占 TVOCs 的 45.3%、24.0%、16.5%、10.0%和 4.2%。在不同时间计算了 OH 反应性和相对增量反应性(RIR)。结果表明,烯烃起着主要作用,占初始 VOC 反应性的平均 68.5%。与其他地区相比,烯烃对兰州石化工业区 O 形成更为重要,而芳烃则相对不重要。一般来说,上午 O 形成处于 VOC 限制阶段,下午处于过渡阶段。响应面法(RSM)结合化学箱模型,获得了 O 及其前体物之间的关系,并确定了降低 O 浓度的最有效方法。非烯烃浓度的降低对 O 浓度的影响较小。相比之下,氮氧化物(NO)的影响与烯烃浓度密切相关,当烯烃浓度降低到当前浓度的 80%以下时,NO 浓度的降低会导致 O 浓度的增加。为了减轻兰州石化工业区附近的 O 污染,降低烯烃浓度,特别是 C4 烯烃浓度(1,3-丁二烯、顺式-2-丁烯和反式-2-丁烯),是最快和最有效的控制策略。本研究结果为石化工业区 O 污染控制提供了参考。

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