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@ARTICLE{Rosanka:877782,
author = {Rosanka, Simon and Vu, Giang H. T. and Nguyen, Hue M. T.
and Pham, Tien V. and Javed, Umar and Taraborrelli, Domenico
and Vereecken, Luc},
title = {{A}tmospheric chemical loss processes of isocyanic acid
({HNCO}): a combined theoretical kinetic and global
modelling study},
journal = {Atmospheric chemistry and physics},
volume = {20},
number = {11},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2020-02449},
pages = {6671 - 6686},
year = {2020},
abstract = {Isocyanic acid (HNCO) is a chemical constituent suspected
to be harmful to humans if ambient concentrations exceed
∼1 ppbv. HNCO is mainly emitted by combustion processes
but is also inadvertently released by NOx mitigation
measures in flue gas treatments. With increasing biomass
burning and more widespread usage of catalytic converters in
car engines, good prediction of HNCO atmospheric levels with
global models is desirable. Little is known directly about
the chemical loss processes of HNCO, which limits the
implementation in global Earth system models. This study
aims to close this knowledge gap by combining a theoretical
kinetic study on the major oxidants reacting with HNCO with
a global modelling study. The potential energy surfaces of
the reactions of HNCO with OH and NO3 radicals, Cl atoms,
and ozone were studied using high-level
CCSD(T)/CBS(DTQ)//M06-2X/aug-cc-pVTZ quantum chemical
methodologies, followed by transition state theory (TST)
theoretical kinetic predictions of the rate coefficients at
temperatures of 200–3000 K. It was found that the
reactions are all slow in atmospheric conditions, with
k(300K)≤7×10−16 cm3molecule−1s−1, and that
product formation occurs predominantly by H abstraction; the
predictions are in good agreement with earlier experimental
work, where available. The reverse reactions of NCO radicals
with H2O, HNO3, and HCl, of importance mostly in combustion,
were also examined briefly.The findings are implemented into
the atmospheric model EMAC (ECHAM/MESSy Atmospheric
Chemistry) to estimate the importance of each chemical loss
process on a global scale. The EMAC predictions confirm that
the gas-phase chemical loss of HNCO is a negligible process,
contributing less than $1 \%$ and leaving heterogeneous
losses as the major sinks. The removal of HNCO by clouds and
precipitation contributes about $10 \%$ of the total loss,
while globally dry deposition is the main sink, accounting
for $∼90 \%.$ The global simulation also shows that due
to its long chemical lifetime in the free troposphere, HNCO
can be efficiently transported into the UTLS by deep
convection events. Daily-average mixing ratios of
ground-level HNCO are found to regularly exceed 1 ppbv in
regions dominated by biomass burning events, but rarely
exceed levels above 10 ppt in other areas of the
troposphere, though locally instantaneous toxic levels are
expected.},
cin = {IEK-8 / JARA-HPC},
ddc = {550},
cid = {I:(DE-Juel1)IEK-8-20101013 / $I:(DE-82)080012_20140620$},
pnm = {243 - Tropospheric trace substances and their
transformation processes (POF3-243) / FRONTier simulations
of AIR composition evolution (FRONTAIR) $(jiek81_20190501)$},
pid = {G:(DE-HGF)POF3-243 / $G:(DE-Juel1)jiek81_20190501$},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000538775000001},
doi = {10.5194/acp-20-6671-2020},
url = {https://juser.fz-juelich.de/record/877782},
}