Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs
Polycyclic aromatic hydrocarbons like benzo(a)pyrene (BaP) in atmospheric particulate matter pose a threat to human health because of their high carcinogenicity. In the atmosphere, BaP is mainly degraded through a multiphase reaction with ozone, but the fate and atmospheric transport of BaP are poor...
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ftcdlib:oai:escholarship.org:ark:/13030/qt8fp9j5fz 2023-11-05T03:39:51+01:00 Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs Mu, Qing Shiraiwa, Manabu Octaviani, Mega Ma, Nan Ding, Aijun Su, Hang Lammel, Gerhard Pöschl, Ulrich Cheng, Yafang eaap7314 2018-03-02 application/pdf https://escholarship.org/uc/item/8fp9j5fz unknown eScholarship, University of California qt8fp9j5fz https://escholarship.org/uc/item/8fp9j5fz public Science Advances, vol 4, iss 3 Earth Sciences Atmospheric Sciences article 2018 ftcdlib 2023-10-09T18:08:15Z Polycyclic aromatic hydrocarbons like benzo(a)pyrene (BaP) in atmospheric particulate matter pose a threat to human health because of their high carcinogenicity. In the atmosphere, BaP is mainly degraded through a multiphase reaction with ozone, but the fate and atmospheric transport of BaP are poorly characterized. Earlier modeling studies used reaction rate coefficients determined in laboratory experiments at room temperature, which may overestimate/underestimate degradation rates when applied under atmospheric conditions. Moreover, the effects of diffusion on the particle bulk are not well constrained, leading to large discrepancies between model results and observations. We show how regional and global distributions and transport of BaP can be explained by a new kinetic scheme that provides a realistic description of the temperature and humidity dependence of phase state, diffusivity, and reactivity of BaP-containing particles. Low temperature and humidity can substantially increase the lifetime of BaP and enhance its atmospheric dispersion through both the planetary boundary layer and the free troposphere. The new scheme greatly improves the performance of multiscale models, leading to better agreement with observed BaP concentrations in both source regions and remote regions (Arctic), which cannot be achieved by less-elaborate degradation schemes (deviations by multiple orders of magnitude). Our results highlight the importance of considering temperature and humidity effects on both the phase state of aerosol particles and the chemical reactivity of particulate air pollutants. Article in Journal/Newspaper Arctic Human health University of California: eScholarship |
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University of California: eScholarship |
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Earth Sciences Atmospheric Sciences |
spellingShingle |
Earth Sciences Atmospheric Sciences Mu, Qing Shiraiwa, Manabu Octaviani, Mega Ma, Nan Ding, Aijun Su, Hang Lammel, Gerhard Pöschl, Ulrich Cheng, Yafang Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs |
topic_facet |
Earth Sciences Atmospheric Sciences |
description |
Polycyclic aromatic hydrocarbons like benzo(a)pyrene (BaP) in atmospheric particulate matter pose a threat to human health because of their high carcinogenicity. In the atmosphere, BaP is mainly degraded through a multiphase reaction with ozone, but the fate and atmospheric transport of BaP are poorly characterized. Earlier modeling studies used reaction rate coefficients determined in laboratory experiments at room temperature, which may overestimate/underestimate degradation rates when applied under atmospheric conditions. Moreover, the effects of diffusion on the particle bulk are not well constrained, leading to large discrepancies between model results and observations. We show how regional and global distributions and transport of BaP can be explained by a new kinetic scheme that provides a realistic description of the temperature and humidity dependence of phase state, diffusivity, and reactivity of BaP-containing particles. Low temperature and humidity can substantially increase the lifetime of BaP and enhance its atmospheric dispersion through both the planetary boundary layer and the free troposphere. The new scheme greatly improves the performance of multiscale models, leading to better agreement with observed BaP concentrations in both source regions and remote regions (Arctic), which cannot be achieved by less-elaborate degradation schemes (deviations by multiple orders of magnitude). Our results highlight the importance of considering temperature and humidity effects on both the phase state of aerosol particles and the chemical reactivity of particulate air pollutants. |
format |
Article in Journal/Newspaper |
author |
Mu, Qing Shiraiwa, Manabu Octaviani, Mega Ma, Nan Ding, Aijun Su, Hang Lammel, Gerhard Pöschl, Ulrich Cheng, Yafang |
author_facet |
Mu, Qing Shiraiwa, Manabu Octaviani, Mega Ma, Nan Ding, Aijun Su, Hang Lammel, Gerhard Pöschl, Ulrich Cheng, Yafang |
author_sort |
Mu, Qing |
title |
Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs |
title_short |
Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs |
title_full |
Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs |
title_fullStr |
Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs |
title_full_unstemmed |
Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs |
title_sort |
temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of pahs |
publisher |
eScholarship, University of California |
publishDate |
2018 |
url |
https://escholarship.org/uc/item/8fp9j5fz |
op_coverage |
eaap7314 |
genre |
Arctic Human health |
genre_facet |
Arctic Human health |
op_source |
Science Advances, vol 4, iss 3 |
op_relation |
qt8fp9j5fz https://escholarship.org/uc/item/8fp9j5fz |
op_rights |
public |
_version_ |
1781695783190396928 |