Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects

<p>We used the CAM5 model to examine how different particle-bound polycyclic aromatic hydrocarbon (PAH) degradation approaches affect the spatial distribution of benzo(a)pyrene (BaP). Three approaches were evaluated: NOA (no effect of OA coatings state on BaP), shielded (viscous OA coatings sh...

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Main Authors: S. Lou, M. Shrivastava, A. Albinet, S. Tomaz, D. Srivastava, O. Favez, H. Shen, A. Ding
Format: Article
Language:English
Published: Copernicus Publications 2025-07-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/25/8163/2025/acp-25-8163-2025.pdf
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author S. Lou
S. Lou
S. Lou
M. Shrivastava
A. Albinet
S. Tomaz
S. Tomaz
D. Srivastava
D. Srivastava
O. Favez
H. Shen
A. Ding
A. Ding
A. Ding
author_facet S. Lou
S. Lou
S. Lou
M. Shrivastava
A. Albinet
S. Tomaz
S. Tomaz
D. Srivastava
D. Srivastava
O. Favez
H. Shen
A. Ding
A. Ding
A. Ding
author_sort S. Lou
collection DOAJ
description <p>We used the CAM5 model to examine how different particle-bound polycyclic aromatic hydrocarbon (PAH) degradation approaches affect the spatial distribution of benzo(a)pyrene (BaP). Three approaches were evaluated: NOA (no effect of OA coatings state on BaP), shielded (viscous OA coatings shield BaP from oxidation under cool and dry conditions) and ROI-T (viscous OA coatings slow BaP oxidation in response to temperature and humidity). Results show that BaP concentrations vary seasonally, influenced by emissions, deposition, transport and degradation approach, all of which are influenced by meteorological conditions. All simulations predict higher population-weighted global average (PWGA) fresh BaP concentrations during December–January–February (DJF) compared to June–July–August (JJA), due to increased emissions from household activities and reduced removal processes during colder months. The shielded and ROI-T approaches, which account for OA coatings, result in 2–6 times higher BaP concentrations in DJF compared to NOA. The shielded simulation predicts the highest PWGA fresh BaP concentration (1.3 <span class="inline-formula">ng m<sup>−3</sup></span>), with 90 % of BaP protected from oxidation. In contrast, the ROI-T approach forecasts lower concentrations in middle to low latitudes, as it assumes less effective OA coatings under warmer, more humid conditions. Evaluations against observed BaP concentrations show the shielded approach performs best, with a normalized mean bias (NMB) within <span class="inline-formula">±</span> 20 %. The combined incremental lifetime cancer risk (ILCR) for both fresh and oxidized PAHs is similar across simulations, emphasizing the importance of considering both forms in health risk assessments. This study highlights the critical role of accurate degradation approaches in PAH modeling.</p>
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spelling doaj-art-0001fb2d1bbe4fa78a118de2fe02b99a2025-08-20T03:31:54ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242025-07-01258163818310.5194/acp-25-8163-2025Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effectsS. Lou0S. Lou1S. Lou2M. Shrivastava3A. Albinet4S. Tomaz5S. Tomaz6D. Srivastava7D. Srivastava8O. Favez9H. Shen10A. Ding11A. Ding12A. Ding13Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Jiangsu Provincial Collaborative Innovation Center of Climate Change, Nanjing University, Nanjing, 210023, ChinaFrontiers Science Center for Critical Earth Material Cycling, Nanjing University, Nanjing 210023, ChinaState Key Laboratory of Severe Weather Meteorological Science and Technology, Nanjing University, Nanjing 210023, ChinaPacific Northwest National Laboratory, Richland, WA 99354, USAInstitut National de l'Environnement industriel et des RISques (INERIS), 60550, Verneuil-en-Halatte, FranceInstitut National de l'Environnement industriel et des RISques (INERIS), 60550, Verneuil-en-Halatte, Francenow at: INRS, 1 rue du Morvan CS 60027, 54519, Vandœuvre-lès-Nancy, FranceInstitut National de l'Environnement industriel et des RISques (INERIS), 60550, Verneuil-en-Halatte, Francenow at: School of Geography Earth and Environmental Science, University of Birmingham, Edgbaston, Birmingham, B15 2TT, UKInstitut National de l'Environnement industriel et des RISques (INERIS), 60550, Verneuil-en-Halatte, FranceShenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, ChinaJoint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Jiangsu Provincial Collaborative Innovation Center of Climate Change, Nanjing University, Nanjing, 210023, ChinaFrontiers Science Center for Critical Earth Material Cycling, Nanjing University, Nanjing 210023, ChinaState Key Laboratory of Severe Weather Meteorological Science and Technology, Nanjing University, Nanjing 210023, China<p>We used the CAM5 model to examine how different particle-bound polycyclic aromatic hydrocarbon (PAH) degradation approaches affect the spatial distribution of benzo(a)pyrene (BaP). Three approaches were evaluated: NOA (no effect of OA coatings state on BaP), shielded (viscous OA coatings shield BaP from oxidation under cool and dry conditions) and ROI-T (viscous OA coatings slow BaP oxidation in response to temperature and humidity). Results show that BaP concentrations vary seasonally, influenced by emissions, deposition, transport and degradation approach, all of which are influenced by meteorological conditions. All simulations predict higher population-weighted global average (PWGA) fresh BaP concentrations during December–January–February (DJF) compared to June–July–August (JJA), due to increased emissions from household activities and reduced removal processes during colder months. The shielded and ROI-T approaches, which account for OA coatings, result in 2–6 times higher BaP concentrations in DJF compared to NOA. The shielded simulation predicts the highest PWGA fresh BaP concentration (1.3 <span class="inline-formula">ng m<sup>−3</sup></span>), with 90 % of BaP protected from oxidation. In contrast, the ROI-T approach forecasts lower concentrations in middle to low latitudes, as it assumes less effective OA coatings under warmer, more humid conditions. Evaluations against observed BaP concentrations show the shielded approach performs best, with a normalized mean bias (NMB) within <span class="inline-formula">±</span> 20 %. The combined incremental lifetime cancer risk (ILCR) for both fresh and oxidized PAHs is similar across simulations, emphasizing the importance of considering both forms in health risk assessments. This study highlights the critical role of accurate degradation approaches in PAH modeling.</p>https://acp.copernicus.org/articles/25/8163/2025/acp-25-8163-2025.pdf
spellingShingle S. Lou
S. Lou
S. Lou
M. Shrivastava
A. Albinet
S. Tomaz
S. Tomaz
D. Srivastava
D. Srivastava
O. Favez
H. Shen
A. Ding
A. Ding
A. Ding
Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
Atmospheric Chemistry and Physics
title Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
title_full Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
title_fullStr Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
title_full_unstemmed Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
title_short Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
title_sort uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
url https://acp.copernicus.org/articles/25/8163/2025/acp-25-8163-2025.pdf
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