Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.1073/pnas.1902517116 |
Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations | |
Zhou, Shouming1; Hwang, Brian C. H.2; Lakey, Pascale S. J.2; Zuend, Andreas3; Abbatt, Jonathan P. D.1; Shiraiwa, Manabu2 | |
2019 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2019 |
卷号 | 116期号:24页码:11658-11663 |
文章类型 | Article |
语种 | 英语 |
国家 | Canada; USA |
英文摘要 | Benzo[a]pyrene (BaP), a key polycyclic aromatic hydrocarbon (PAH) often associated with soot particles coated by organic compounds, is a known carcinogen and mutagen. When mixed with organics, the kinetics and mechanisms of chemical transformations of BaP by ozone in indoor and outdoor environments are still not fully elucidated. Using direct analysis in real-time mass spectrometry (DART-MS), kinetics studies of the ozonolysis of BaP in thin films exhibited fast initial loss of BaP followed by a slower decay at long exposure times. Kinetic multilayer modeling demonstrates that the slow decay of BaP over long times can be simulated if there is slow diffusion of BaP from the film interior to the surface, resolving longstanding unresolved observations of incomplete PAH decay upon prolonged ozone exposure. Phase separation drives the slow diffusion time scales in multicomponent systems. Specifically, thermodynamic modeling predicts that BaP phase separates from secondary organic aerosol material so that the BaP-rich layer at the surface shields the inner BaP from ozone. Also, BaP is miscible with organic oils such as squalane, linoleic acid, and cooking oil, but its oxidation products are virtually immiscible, resulting in the formation of a viscous surface crust that hinders diffusion of BaP from the film interior to the surface. These findings imply that phase separation and slow diffusion significantly prolong the chemical lifetime of PAH5, affecting long-range transport of PAH5 in the atmosphere and their fates in indoor environments. |
英文关键词 | phase state ozone indoor chemistry bulk diffusion kinetic modeling |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000471039700021 |
WOS关键词 | SECONDARY ORGANIC MATERIAL ; LONG-RANGE TRANSPORT ; OLEIC-ACID ; AEROSOL-PARTICLES ; ACTIVITY-COEFFICIENTS ; CHEMICAL-REACTIVITY ; THERMODYNAMIC MODEL ; CANCER-RISK ; OZONE ; SURFACE |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/205129 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada; 2.Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA; 3.McGill Univ, Dept Atmospher & Ocean Sci, Montreal, PQ H3A 0B9, Canada |
推荐引用方式 GB/T 7714 | Zhou, Shouming,Hwang, Brian C. H.,Lakey, Pascale S. J.,et al. Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2019,116(24):11658-11663. |
APA | Zhou, Shouming,Hwang, Brian C. H.,Lakey, Pascale S. J.,Zuend, Andreas,Abbatt, Jonathan P. D.,&Shiraiwa, Manabu.(2019).Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,116(24),11658-11663. |
MLA | Zhou, Shouming,et al."Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 116.24(2019):11658-11663. |
条目包含的文件 | 条目无相关文件。 |
除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。
修改评论