Modeling global persistent organic chemicals in clouds

•Atmospheric partition of persistent organic chemicals was affected by cloud liquid water content and air temperature.•Hydrophilic chemicals could be strongly partitioned onto cloud water droplets.•Hydrophobic chemicals tended to partition onto particles.•Clouds played an important role in global distribution of persistent organic chemicals in the atmosphere.

A cloud model was implemented in a global atmospheric transport model to simulate cloud liquid water content and quantify the influence of clouds on gas/aqueous phase partitioning of persistent organic chemicals (POCs). Partitioning fractions of gas/aqueous and particle phases in clouds for three POCs α-hexachlorocyclohexane (α-HCH), polychlorinated biphenyl-28 (PCB-28), and PCB-138 in a cloudy atmosphere were estimated. Results show that the partition fraction of these selected chemicals depend on cloud liquid water content (LWC) and air temperature. We calculated global distribution of water droplet/ice particle-air partitioning coefficients of the three chemicals in clouds. The partition fractions at selected model grids in the Northern Hemisphere show that α-HCH, a hydrophilic chemical, is sorbed strongly onto cloud water droplets. The computed partition fractions at four selected model grids show that α-HCH tends to be sorbed onto clouds over land (source region) from summer to early fall, and over ocean from late spring to early fall. 20-60% of α-HCH is able to be sorbed to cloud waters over mid-latitude oceans during summer days. PCB-138, one of hydrophobic POCs, on the other hand, tends to be sorbed to particles in the atmosphere subject to air temperature. We also show that, on seasonal or annual average, 10-20% of averaged PCB-28 over the Northern Hemisphere could be sorbed onto clouds, leading to reduction of its gas-phase concentration in the atmosphere.