Informace o publikaci

Fast Formation of Nitro-PAHs in the Marine Atmosphere Constrained in a Regional-Scale Lagrangian Field Experiment

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MULDER Marie Daniëlle DUMANOGLU Y. EFSTATHIOU Christos KUKUČKA Petr MATEJOVIČOVÁ Jana MAURER Christian PŘIBYLOVÁ Petra PROKEŠ Roman SOFUOGLU A. SOFUOGLU S.C. WILSON J. ZETZSCH C. WOTAWA G. LAMMEL Gerhard

Rok publikování 2019
Druh Článek v odborném periodiku
Časopis / Zdroj ENVIRONMENTAL SCIENCE & TECHNOLOGY
Fakulta / Pracoviště MU

Přírodovědecká fakulta

Citace
www https://pubs.acs.org/doi/10.1021/acs.est.9b03090
Doi http://dx.doi.org/10.1021/acs.est.9b03090
Klíčová slova POLYCYCLIC AROMATIC-HYDROCARBONS; GAS-PHASE REACTIONS; RADICAL-INITIATED REACTIONS; CHEMICAL-TRANSPORT MODEL; LIQUID-VAPOR PRESSURES; PARTICULATE MATTER; ORGANIC-COMPOUNDS; CONSECUTIVE REACTIONS; DRY DEPOSITION; AMBIENT AIR
Popis Polycyclic aromatic hydrocarbons (PAHs) and some of their nitrated derivatives, NPAHs, are seemingly ubiquitous in the atmospheric environment. Atmospheric lifetimes may nevertheless vary within a wide range, and be as short as a few hours. The sources and sinks of NPAH in the atmosphere are not well understood. With a Lagrangian field experiment and modeling, we studied the conversion of the semivolatile PAHs fluoranthene and pyrene into the 2-nitro derivatives 2-nitrofluoranthene and 2-nitropyrene in a cloud-free marine atmosphere on the time scale of hours to 1 day between a coastal and an island site. Chemistry and transport during several episodes was simulated by a Lagrangian box model i.e., a box model coupled to a Lagrangian particle dispersion model, FLEXPART-WRF. It is found that the chemical kinetic data do capture photochemical degradation of the 4-ring PAHs under ambient conditions on the time scale of hours to 1 day, while the production of the corresponding NPAH, which sustained 2-nitrofluoranthene/fluoranthene and 2-nitropyrene/pyrene yields of (3.7 +/- 0.2) and (1.5 +/- 0.1)%, respectively, is by far underestimated. Predicted levels of NPAH come close to observed ones, when kinetic data describing the reactivity of the OH-adduct were explored by means of theoretically based estimates. Predictions are also underestimated by 1-2 orders of magnitude, when NPAH/PAH yields reported from laboratory experiments conducted under high NOx conditions are adopted for the simulations. It is concluded that NPAH sources effective under low NOx conditions, are largely underestimated.
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