TY - JOUR
T1 - Investigating the impact of aqueous-phase chemistry and wet deposition on organic aerosol formation using a molecular surrogate modeling approach
AU - Couvidat, Florian
AU - Sartelet, Karine
AU - Seigneur, Christian
PY - 2013/1/15
Y1 - 2013/1/15
N2 - A molecular surrogate representation of secondary organic aerosol (SOA) formation is used to investigate the effect of aqueous-phase (in clouds and particles) chemical processing and wet deposition on SOA atmospheric concentrations. To that end, the hydrophilic/hydrophobic organic (H 2O) model was augmented to account for several gas/aqueous-phase equilibria and aqueous-phase processes, including the formation of oxalic, glyoxilic and pyruvic acids, the oxidation of methyl vinyl ketone (MVK) and methacrolein (MACR), the formation of tetrols and organosulfates from epoxydiols (IEPOX), and further oxidation of water-soluble SOA (aging). Among those processes, SOA chemical aging and IEPOX reactions led to the most significant increases (up to 1 μg m-3 in some areas) in SOA concentrations in a one-month summer simulation over Europe. However, large uncertainties remain in the gas/aqueous-phase partitioning of oxalic acid, MVK, and MACR. Below-cloud scavenging of SOA precursor gases and of gas-phase SVOC was found to affect SOA concentrations by up to 20%, which suggests that it should be taken into account in air quality models.
AB - A molecular surrogate representation of secondary organic aerosol (SOA) formation is used to investigate the effect of aqueous-phase (in clouds and particles) chemical processing and wet deposition on SOA atmospheric concentrations. To that end, the hydrophilic/hydrophobic organic (H 2O) model was augmented to account for several gas/aqueous-phase equilibria and aqueous-phase processes, including the formation of oxalic, glyoxilic and pyruvic acids, the oxidation of methyl vinyl ketone (MVK) and methacrolein (MACR), the formation of tetrols and organosulfates from epoxydiols (IEPOX), and further oxidation of water-soluble SOA (aging). Among those processes, SOA chemical aging and IEPOX reactions led to the most significant increases (up to 1 μg m-3 in some areas) in SOA concentrations in a one-month summer simulation over Europe. However, large uncertainties remain in the gas/aqueous-phase partitioning of oxalic acid, MVK, and MACR. Below-cloud scavenging of SOA precursor gases and of gas-phase SVOC was found to affect SOA concentrations by up to 20%, which suggests that it should be taken into account in air quality models.
UR - https://www.scopus.com/pages/publications/84872553992
U2 - 10.1021/es3034318
DO - 10.1021/es3034318
M3 - Article
C2 - 23190252
AN - SCOPUS:84872553992
SN - 0013-936X
VL - 47
SP - 914
EP - 922
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 2
ER -