Ubiquity of Anthropogenic Terpenoids in Cities Worldwide: Emission Ratios, Emission Quantification and Implications for Urban Atmospheric Chemistry
Ubiquity of Anthropogenic Terpenoids in Cities Worldwide: Emission Ratios, Emission Quantification and Implications for Urban Atmospheric Chemistry
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DOI：
10.1029/2022jd037566
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发表时间：
2023-02
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通讯作者：
A. Borbon;P. Dominutti;A. Panopoulou;V. Gros;S. Sauvage;M. Farhat;C. Afif;N. Elguindi;A. Fornaro;C. Granier;J. Hopkins;E. Liakakou;Thiago Nogueira;Tailine Corrêa dos Santos;T. Salameh;Alexandre Armangaud;D. Piga;O. Perrussel
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作者：
A. Borbon;P. Dominutti;A. Panopoulou;V. Gros;S. Sauvage;M. Farhat;C. Afif;N. Elguindi;A. Fornaro;C. Granier;J. Hopkins;E. Liakakou;Thiago Nogueira;Tailine Corrêa dos Santos;T. Salameh;Alexandre Armangaud;D. Piga;O. Perrussel
萜类化合物(异戊二烯和单萜)是一种高活性的挥发性有机化合物(VOCs)，几十年来因其生物来源而闻名。在这里，我们讨论它们的人为排放的性质和大小。我们汇编并重新分析了过去十年在从中纬度到亚热带地区的城市地区收集的14个现场VOC观测数据集。我们显示，即使在中纬度冬季，城市环境空气中也存在人为萜类化合物，与人为化合物(R2>；0.50)存在明显的协变。尽管消费产品排放的单萜烯在北美城市日益重要，但有一些证据表明，发展中国家的城市从尾气排气中排放单萜烯。据估计，与交通相关的单萜烯比例可高达其环境水平的40%。对一些萜类化合物(异戊二烯、α-蒎烯和柠檬烯)的人为排放比(ER)进行了估算和空间比较。以法国、黎巴嫩和越南为重点，从区域和全球城市和国家尺度的排放清单(CAMS-GLOB-ANT_V4.2)中间接估计了萜类化合物的人为排放量。这些人为排放不超过其他人为VOC排放的3%。然而，它们在NO3氧化和臭氧分解方面比其他人为VOCs的反应活性高出一到三个数量级。这项研究提出了两个今后需要进一步研究的问题：(A)交通排放的萜类化合物的重要性，特别是在发展中世界的城市地区；(B)人为萜类化合物在中纬度地区夜间和冬季大气化学中的作用。
Terpenoids (isoprene and monoterpenes) are highly reactive Volatile Organic Compounds (VOCs) known for decades for their biogenic origin. Here, we discuss the nature and magnitude of their anthropogenic emissions. We compiled and re‐analyzed 14 data sets of in situ VOC observations collected over the last decade in contrasting urban areas from mid‐latitudes to subtropical regions. We show the systematic presence of anthropogenic terpenoids in urban ambient air with clear covariations with anthropogenic compounds (R2 > 0.50) even during mid‐latitude winters. Despite the emerging importance of monoterpene emissions from consumer products in North American cities, there is some evidence of monoterpene emissions from tailpipe exhaust in cities of the developing world. The traffic‐related fraction of monoterpenes is estimated and can account for up to 40% of their ambient levels. The anthropogenic emission ratios (ER) of some terpenoids (isoprene, α‐pinene and limonene) are estimated and spatially compared. The anthropogenic emissions of terpenoids are indirectly estimated from those ER combined to regional and global emission inventories (CAMS‐GLOB‐ANT_v4.2) at urban and country scale focusing on France, Lebanon, and Vietnam. Those anthropogenic emissions do not represent more than 3% of other anthropogenic VOC emissions. However, they dominate by one to three orders of magnitude the reactivity of other anthropogenic VOCs regarding NO3 oxidation and ozonolysis. This study raises two questions which need further investigations in the future: (a) the significance of terpenoid emissions from traffic, especially in urban areas of the developing world and (b) the role of anthropogenic terpenoids in nighttime and wintertime atmospheric chemistry at mid‐latitudes.