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@article{1494016,
author = {Mu, Qing and Shiraiwa, Manabu and Octaviani, Mega and Ma, Nan and Ding, Aijun and Su, Hang and Lammel, Gerhard and Poschl, Ulrich and Cheng, Yafang},
article_location = {New York},
article_number = {3},
doi = {http://dx.doi.org/10.1126/sciadv.aap7314},
keywords = {POLYCYCLIC AROMATIC-HYDROCARBONS; SECONDARY ORGANIC AEROSOLS; GAS-PARTICLE INTERACTIONS; KINETIC MULTILAYER MODEL; LONG-RANGE TRANSPORT; GLOBAL DISTRIBUTION; BULK DIFFUSION; CANCER-RISK; OZONE; SURFACE},
language = {eng},
issn = {2375-2548},
journal = {Science advances},
title = {Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs},
url = {https://www.ncbi.nlm.nih.gov/pubmed/29750188},
volume = {4},
year = {2018}
}
TY - JOUR
ID - 1494016
AU - Mu, Qing - Shiraiwa, Manabu - Octaviani, Mega - Ma, Nan - Ding, Aijun - Su, Hang - Lammel, Gerhard - Poschl, Ulrich - Cheng, Yafang
PY - 2018
TI - Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs
JF - Science advances
VL - 4
IS - 3
SP - 1-8
EP - 1-8
PB - American Association for the Advancement of Science
SN - 23752548
KW - POLYCYCLIC AROMATIC-HYDROCARBONS
KW - SECONDARY ORGANIC AEROSOLS
KW - GAS-PARTICLE INTERACTIONS
KW - KINETIC MULTILAYER MODEL
KW - LONG-RANGE TRANSPORT
KW - GLOBAL DISTRIBUTION
KW - BULK DIFFUSION
KW - CANCER-RISK
KW - OZONE
KW - SURFACE
UR - https://www.ncbi.nlm.nih.gov/pubmed/29750188
L2 - https://www.ncbi.nlm.nih.gov/pubmed/29750188
N2 - 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 multi-phase 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.
ER -
MU, Qing, Manabu SHIRAIWA, Mega OCTAVIANI, Nan MA, Aijun DING, Hang SU, Gerhard LAMMEL, Ulrich POSCHL a Yafang CHENG. Temperature effect on phase state and reactivity controls atmospheric multiphase chemistry and transport of PAHs. \textit{Science advances}. New York: American Association for the Advancement of Science, roč.~4, č.~3, s.~1-8. ISSN~2375-2548. doi:10.1126/sciadv.aap7314. 2018.
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