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Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol
Shrivastava, Manish ; Lou, Silja ; Zelenyuk, Alla ; Easter, Richard C. ; Corley, Richard A. ; Thrall, Brian D. ; Rasch, Philip J. ; Fast, Jerome D. ; Simonich, Staci L. Massey ; Shen, Huizhong ; Tao, Shu
刊名PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
2017
关键词polycyclic aromatic hydrocarbons organic aerosols climate model viscous aerosol shield heterogeneous chemistry ATMOSPHERIC TRANSPORT HETEROGENEOUS REACTIONS OH RADICALS PARTICLES REACTIVITY PAHS MODEL OZONE KINETICS PHASE
DOI10.1073/pnas.1618475114
英文摘要Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on humans and ecosystems. One of the most carcinogenic PAHs, benzo(a) pyrene (BaP), is efficiently bound to and transported with atmospheric particles. Laboratory measurements show that particle-bound BaP degrades in a few hours by heterogeneous reaction with ozone, yet field observations indicate BaP persists much longer in the atmosphere, and some previous chemical transport modeling studies have ignored heterogeneous oxidation of BaP to bring model predictions into better agreement with field observations. We attribute this unexplained discrepancy to the shielding of BaP from oxidation by coatings of viscous organic aerosol (OA). Accounting for this OA viscosity-dependent shielding, which varies with temperature and humidity, in a global climate/chemistry model brings model predictions into much better agreement with BaP measurements, and demonstrates stronger long-range transport, greater deposition fluxes, and substantially elevated lung cancer risk from PAHs. Model results indicate that the OA coating is more effective in shielding BaP in the middle/high latitudes compared with the tropics because of differences in OA properties (semisolid when cool/dry vs. liquid-like when warm/humid). Faster chemical degradation of BaP in the tropics leads to higher concentrations of BaP oxidation products over the tropics compared with higher latitudes. This study has profound implications demonstrating that OA strongly modulates the atmospheric persistence of PAHs and their cancer risks.; Environmental Molecular Science Laboratory (EMSL); US DOE's Office of Biological and Environmental Research; National Science Foundation; Office of Science of the DOE; US DOE [DE-AC05-76RL01830]; National Institute of Environmental Health Sciences (NIEHS) [P30ES00210, P42ES016465]; National Science Foundation (NSF) [AGS-11411214]; US DOE Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences; US DOE, Office of Science, Biological and Environmental Research programas part of the Earth System Modeling Program; Ministry of Education, Youth and Sports of the Czech Republic [LM2015051]; National Sustainability Programme [LO1214]; SCI(E); ARTICLE; 6; 1246-1251; 114
语种英语
内容类型期刊论文
源URL[http://ir.pku.edu.cn/handle/20.500.11897/475203]  
专题城市与环境学院
推荐引用方式
GB/T 7714
Shrivastava, Manish,Lou, Silja,Zelenyuk, Alla,et al. Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2017.
APA Shrivastava, Manish.,Lou, Silja.,Zelenyuk, Alla.,Easter, Richard C..,Corley, Richard A..,...&Tao, Shu.(2017).Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA.
MLA Shrivastava, Manish,et al."Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2017).
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