| Title | Development and evaluation of a new compact mechanism for aromatic oxidation in atmospheric models |
| Authors | Bates, Kelvin H. Jacob, Daniel J. Li, Ke Ivatt, Peter D. Evans, Mat J. Yan, Yingying Lin, Jintai |
| Affiliation | Harvard Univ, Harvard John A Paulson Sch Engn & Appl Sci, Cambridge, MA 02138 USA Univ Calif Davis, Dept Environm Toxicol, Davis, CA 95616 USA Nanjing Univ Informat Sci & Technol, Sch Environm Sci & Engn, Nanjing, Peoples R China Univ York, Dept Chem, Wolfson Atmospher Chem Labs, York, N Yorkshire, England Univ York, Natl Ctr Atmospher Sci, Dept Chem, York, N Yorkshire, England China Univ Geosci Wuhan, Sch Environm Studies, Dept Atmospher Sci, Wuhan, Peoples R China Peking Univ, Sch Phys, Dept Atmospher & Ocean Sci, Lab Climate & Ocean Atmosphere Studies, Beijing, Peoples R China |
| Keywords | SECONDARY ORGANIC AEROSOL RING-RETAINING PRODUCTS GAS-PHASE REACTION ADJOINT SENSITIVITY-ANALYSIS INTERMEDIATES CRI MECHANISM RADICAL-INITIATED REACTIONS CHEMICAL KINETIC SYSTEMS NOX-AIR PHOTOOXIDATIONS ANTHROPOGENIC EMISSIONS SOA FORMATION |
| Issue Date | 17-Dec-2021 |
| Publisher | ATMOSPHERIC CHEMISTRY AND PHYSICS |
| Abstract | Aromatic hydrocarbons, including benzene, toluene, and xylenes, play an important role in atmospheric chemistry, but the associated chemical mechanisms are complex and uncertain. Sparing representation of this chemistry in models is needed for computational tractability. Here, we develop a new compact mechanism for aromatic chemistry (GC13) that captures current knowledge from laboratory and computational studies with only 17 unique species and 44 reactions. We compare GC13 to six other currently used mechanisms of varying complexity in box model simulations of environmental chamber data and diurnal boundary layer chemistry, and show that GC13 provides results consistent with or better than more complex mechanisms for oxygenated products (alcohols, carbonyls, dicarbonyls), ozone, and hydrogen oxide (HOx OH + HO2) radicals. Specifically, GC13 features increased radical recycling and increased ozone destruction from phenoxy-phenylperoxy radical cycling relative to other mechanisms. We implement GC13 into the GEOS-Chem global chemical transport model and find higher glyoxal yields and net ozone loss from aromatic chemistry compared with other mechanisms. Aromatic oxidation in the model contributes 23 %, 5 %, and 8 % of global glyoxal, methylglyoxal, and formic acid production, respectively, and has mixed effects on formaldehyde. It drives small decreases in global tropospheric OH (-2.2 %), NOx ( NO + NO2; -3.7 %), and ozone (-0.8 %), but a large increase in NO3 (+22 %) from phenoxy-phenylperoxy radical cycling. Regional effects in polluted environments can be substantially larger, especially from the photolysis of carbonyls produced by aromatic oxidation, which drives large wintertime increases in OH and ozone concentrations. |
| URI | http://hdl.handle.net/20.500.11897/632804 |
| ISSN | 1680-7316 |
| DOI | 10.5194/acp-21-18351-2021 |
| Indexed | SCI(E) |
| Appears in Collections: | 物理学院 |
