Chemical Interactions Between Ship-Originated Air Pollutants and Ocean-Emitted Halogens

17 pags., 9 figs., 1 tab.Ocean-going ships supply products from one region to another and contribute to the world’s economy. Ship exhaust contains many air pollutants and results in significant changes in marine atmospheric composition. The role of reactive halogen species (RHS) in the troposphere has received increasing recognition and oceans are the largest contributors to their atmospheric burden. However, the impact of shipping emissions on RHS and that of RHS on ship-originated air pollutants have not been studied in detail. Here, an updated Weather Research Forecasting coupled with Chemistry model is utilized to explore the chemical interactions between ship emissions and oceanic RHS over the East Asia seas in summer. The emissions and resulting chemical transformations from shipping activities increase the level of NO and NO at the surface, increase O in the South China Sea, but decrease O in the East China Sea. Such changes in pollutants result in remarkable changes in the levels of RHS (>200% increase of chlorine; ∼30% and ∼5% decrease of bromine and iodine, respectively) as well as in their partitioning. The abundant RHS, in turn, reshape the loadings of air pollutants (∼20% decrease of NO and NO; ∼15% decrease of O) and those of the oxidants (>10% reduction of OH and HO; ∼40% decrease of NO) with marked patterns along the ship tracks. We, therefore, suggest that these important chemical interactions of ship-originated emissions with RHS should be considered in the environmental policy assessments of the role of shipping emissions in air quality and climate.This study received funding from the European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation Program (Project ERC-2016- COG 726349 CLIMAHAL) and was supported by the Consejo Superior de Investigaciones Científicas (CSIC) of Spain and The Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning and Shanghai Thousand Talents Program. The development and maintenance of the WRF-Chem model are conducted by NOAA/ESRL/GSD in active collaboration with other institutes. Computing resources, support, and data storage were provided by the Climate Simulation Laboratory at NCAR’s Computational and Information Systems Laboratory (CISL), sponsored by the NSF. International cooperation between CSIC (Spain) and CONICET (Argentina) was supported by the i-COOP program (B20331). R.P.F. would like to thank ANPCyT (PICT 2015-0714), UNCuyo (SeCTyP M032/3853), and UTN (PID 4920-194/2018) for financial support. IITM is funded by the Ministry of Earth Sciences, Government of India