Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs

Science Advances
Qing MuYafang Cheng

Abstract

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 co...Continue Reading

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Citations

May 31, 2019·Proceedings of the National Academy of Sciences of the United States of America·Shouming ZhouManabu Shiraiwa
Jan 9, 2021·Environmental Science & Technology·Yicong HeShantanu H Jathar
Nov 20, 2020·Science Advances·David S RichardsRyan D Davis
May 12, 2021·Environmental Science & Technology·Jienan Li, Daniel A Knopf
Jun 27, 2019·Environmental Science & Technology·Marie D MulderGerhard Lammel
Sep 14, 2019·The Journal of Physical Chemistry Letters·Kristian J KilandAllan K Bertram
Feb 23, 2020·The Journal of Physical Chemistry. a·Erin EvoyAllan K Bertram
Dec 31, 2020·Environmental Science & Technology·Xiangxinyue MengMin Hu

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Software Mentioned

OFFLEM
JVAL
RAD
HTAP
MESSy ( Modular Earth Submodel System
MECCA
KM
ONLEM
CONVECT
MESSy

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