TY - JOUR
T1 - Atmospheric chemistry, sources and sinks of carbon suboxide, C3O2
AU - Keßel, Stephan
AU - Cabrera-Perez, David
AU - Horowitz, Abraham
AU - Veres, Patrick
AU - Sander, Rolf
AU - Taraborrelli, Domenico
AU - Tucceri, Maria
AU - Crowley, John N.
AU - Pozzer, Andrea
AU - Stönner, Christof
AU - Vereecken, Luc
AU - Lelieveld, Jos
AU - Williams, Jonathan
PY - 2017/7/20
Y1 - 2017/7/20
N2 - Carbon suboxide, O+C+C+C+O, has been detected in ambient air samples and has the potential to be a noxious pollutant and oxidant precursor; however, its lifetime and fate in the atmosphere are largely unknown. In this work, we collect an extensive set of studies on the atmospheric chemistry of C3O2. Rate coefficients for the reactions of C3O2 with OH radicals and ozone were determined as kOH D(2.6±0.5)X10-12 cm3 molecule-1 s-1 at 295K (independent of pressure between ∼25 and 1000 mbar) and kO3 1.5 10-21cm3 molecule-1-1 at 295 K. A theoretical study on the mechanisms of these reactions indicates that the sole products are CO and CO2, as observed experimentally. The UV absorption spectrum and the interaction of C3O2 with water (Henry's law solubility and hydrolysis rate constant) were also investigated, enabling its photodissociation lifetime and hydrolysis rates, respectively, to be assessed. The role of C3O2 in the atmosphere was examined using in situ measurements, an analysis of the atmospheric sources and sinks and simulation with the EMAC atmospheric chemistry-general circulation model. The results indicate sub-pptv levels at the Earth's surface, up to about 10 pptv in regions with relatively strong sources, e.g. influenced by biomass burning, and a mean lifetime of ∼3.2 days. These predictions carry considerable uncertainty, as more measurement data are needed to determine ambient concentrations and constrain the source strengths.
AB - Carbon suboxide, O+C+C+C+O, has been detected in ambient air samples and has the potential to be a noxious pollutant and oxidant precursor; however, its lifetime and fate in the atmosphere are largely unknown. In this work, we collect an extensive set of studies on the atmospheric chemistry of C3O2. Rate coefficients for the reactions of C3O2 with OH radicals and ozone were determined as kOH D(2.6±0.5)X10-12 cm3 molecule-1 s-1 at 295K (independent of pressure between ∼25 and 1000 mbar) and kO3 1.5 10-21cm3 molecule-1-1 at 295 K. A theoretical study on the mechanisms of these reactions indicates that the sole products are CO and CO2, as observed experimentally. The UV absorption spectrum and the interaction of C3O2 with water (Henry's law solubility and hydrolysis rate constant) were also investigated, enabling its photodissociation lifetime and hydrolysis rates, respectively, to be assessed. The role of C3O2 in the atmosphere was examined using in situ measurements, an analysis of the atmospheric sources and sinks and simulation with the EMAC atmospheric chemistry-general circulation model. The results indicate sub-pptv levels at the Earth's surface, up to about 10 pptv in regions with relatively strong sources, e.g. influenced by biomass burning, and a mean lifetime of ∼3.2 days. These predictions carry considerable uncertainty, as more measurement data are needed to determine ambient concentrations and constrain the source strengths.
UR - https://www.scopus.com/pages/publications/85025074843
U2 - 10.5194/acp-17-8789-2017
DO - 10.5194/acp-17-8789-2017
M3 - Article
AN - SCOPUS:85025074843
SN - 1680-7316
VL - 17
SP - 8789
EP - 8804
JO - Atmospheric Chemistry and Physics
JF - Atmospheric Chemistry and Physics
IS - 14
ER -