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Title: Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol

Abstract

Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on ecosystems and human health. Laboratory measurements show that one of the most carcinogenic PAHs, benzo(a)pyrene, which is adsorbed on surfaces of soot particles, reacts very quickly with atmospheric oxidants like ozone within ~2 hours. Yet, field observations indicate that it actually persists for much longer periods in the atmosphere, and this large discrepancy is not well understood. Driven by novel experimental understanding, we develop a new modelling approach, whereby particle-bound BaP is shielded from oxidation by a coating of viscous organic aerosol (OA). We show that application of this new approach in a global climate model leads to higher atmospheric BaP concentrations that agree much better with measurements, compared to the default model, as well as stronger long-range transport and greater deposition fluxes. Here, this new approach also predicts elevated lung-cancer risk from PAHs. Predicted oxidation of BaP is highest over a tropical belt where OA is liquid-like.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [3];  [4]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Oregon State Univ., Corvallis, OR (United States)
  3. Georgia Inst. of Technology, Atlanta, GA (United States)
  4. Peking Univ., Beijing (China)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1344043
Report Number(s):
PNNL-SA-121554
Journal ID: ISSN 0027-8424; 48913
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 6; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Environmental Molecular Sciences Laboratory; polycyclic aromatic hydrocarbons; organic aerosols; climate model; viscous aerosol shield; heterogeneous chemistry

Citation Formats

Shrivastava, Manish, Lou, Silja, Zelenyuk, Alla, Easter, Richard C., Corley, Richard A., Thrall, Brian D., Rasch, Philip J., Fast, Jerome D., Massey Simonich, Staci L., Shen, Huizhong, and Tao, Shu. Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol. United States: N. p., 2017. Web. doi:10.1073/pnas.1618475114.
Shrivastava, Manish, Lou, Silja, Zelenyuk, Alla, Easter, Richard C., Corley, Richard A., Thrall, Brian D., Rasch, Philip J., Fast, Jerome D., Massey Simonich, Staci L., Shen, Huizhong, & Tao, Shu. Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol. United States. doi:10.1073/pnas.1618475114.
Shrivastava, Manish, Lou, Silja, Zelenyuk, Alla, Easter, Richard C., Corley, Richard A., Thrall, Brian D., Rasch, Philip J., Fast, Jerome D., Massey Simonich, Staci L., Shen, Huizhong, and Tao, Shu. Mon . "Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol". United States. doi:10.1073/pnas.1618475114. https://www.osti.gov/servlets/purl/1344043.
@article{osti_1344043,
title = {Global long-range transport and lung cancer risk from polycyclic aromatic hydrocarbons shielded by coatings of organic aerosol},
author = {Shrivastava, Manish and Lou, Silja and Zelenyuk, Alla and Easter, Richard C. and Corley, Richard A. and Thrall, Brian D. and Rasch, Philip J. and Fast, Jerome D. and Massey Simonich, Staci L. and Shen, Huizhong and Tao, Shu},
abstractNote = {Polycyclic aromatic hydrocarbons (PAHs) have toxic impacts on ecosystems and human health. Laboratory measurements show that one of the most carcinogenic PAHs, benzo(a)pyrene, which is adsorbed on surfaces of soot particles, reacts very quickly with atmospheric oxidants like ozone within ~2 hours. Yet, field observations indicate that it actually persists for much longer periods in the atmosphere, and this large discrepancy is not well understood. Driven by novel experimental understanding, we develop a new modelling approach, whereby particle-bound BaP is shielded from oxidation by a coating of viscous organic aerosol (OA). We show that application of this new approach in a global climate model leads to higher atmospheric BaP concentrations that agree much better with measurements, compared to the default model, as well as stronger long-range transport and greater deposition fluxes. Here, this new approach also predicts elevated lung-cancer risk from PAHs. Predicted oxidation of BaP is highest over a tropical belt where OA is liquid-like.},
doi = {10.1073/pnas.1618475114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 6,
volume = 114,
place = {United States},
year = {Mon Jan 23 00:00:00 EST 2017},
month = {Mon Jan 23 00:00:00 EST 2017}
}

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