化学
波动性(金融)
臭氧
环境化学
微粒
碳纤维
大气碳循环
总有机碳
气溶胶
有机质
固碳
有机化学
二氧化碳
金融经济学
复合材料
经济
复合数
材料科学
作者
Gabriel Isaacman‐VanWertz,P. Massoli,Rachel O’Brien,Christopher Y. Lim,J. P. Franklin,Joshua A. Moss,J. F. Hunter,John B. Nowak,Manjula R. Canagaratna,Pawel K. Misztal,Caleb Arata,Joseph R. Roscioli,Scott T. Herndon,T. B. Onasch,Andrew T. Lambe,John T. Jayne,L. Su,D. A. Knopf,Allen H. Goldstein,Douglas R. Worsnop,Jesse H. Kroll
出处
期刊:Nature Chemistry
[Springer Nature]
日期:2018-02-26
卷期号:10 (4): 462-468
被引量:79
标识
DOI:10.1038/s41557-018-0002-2
摘要
The evolution of atmospheric organic carbon as it undergoes oxidation has a controlling influence on concentrations of key atmospheric species, including particulate matter, ozone and oxidants. However, full characterization of organic carbon over hours to days of atmospheric processing has been stymied by its extreme chemical complexity. Here we study the multigenerational oxidation of α-pinene in the laboratory, characterizing products with several state-of-the-art analytical techniques. Although quantification of some early generation products remains elusive, full carbon closure is achieved (within measurement uncertainty) by the end of the experiments. These results provide new insights into the effects of oxidation on organic carbon properties (volatility, oxidation state and reactivity) and the atmospheric lifecycle of organic carbon. Following an initial period characterized by functionalization reactions and particle growth, fragmentation reactions dominate, forming smaller species. After approximately one day of atmospheric aging, most carbon is sequestered in two long-lived reservoirs—volatile oxidized gases and low-volatility particulate matter. Nearly all organic carbon has now been quantified and characterized in a highly complex evolving atmospheric system, specifically, the multigenerational oxidation of α-pinene. It has been observed that initial addition of functional groups quickly gives way to fragmentation reactions, with organic carbon ultimately becoming sequestered in chemically resistant reservoirs: organic aerosols and long-lived gas-phase species.
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