Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States.
Sara L Farrell, Havala O T Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, Kathleen Fahey
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引用次数: 0
Abstract
A portion of Alaska's Fairbanks North Star Borough was designated as nonattainment for the 2006 24 h fine particulate matter 2.5 μm or less in diameter (PM2.5) National Ambient Air Quality Standards (NAAQS) in 2009. PM2.5 NAAQS exceedances in Fairbanks mainly occur during dark and cold winters, when temperature inversions form and trap high emissions at the surface. Sulfate ( ), often the second-largest contributor to PM2.5 mass during these wintertime PM episodes, is underpredicted by atmospheric chemical transport models (CTMs). Most CTMs account for primary and secondary formed via gas-phase oxidation of sulfur dioxide ( ) and in-cloud aqueous oxidation of dissolved S(IV). Dissolution and reaction of in aqueous aerosols are generally not included in CTMs but can be represented as heterogeneous reactive uptake and may help better represent the high concentrations observed during Fairbanks winters. In addition, hydroxymethanesulfonate (HMS), a particulate sulfur species sometimes misidentified as , is known to form during Fairbanks winters. Heterogeneous formation of and HMS in aerosol liquid water (ALW) was implemented in the Community Multiscale Air Quality (CMAQ) modeling system. CMAQ simulations were performed for wintertime PM episodes in Fairbanks (2008) as well as over the Northern Hemisphere and Contiguous United States (CONUS) for 2015-2016. The added heterogeneous sulfur chemistry reduced model mean sulfate bias by ~0.6 μg m-3 during a cold winter PM episode in Fairbanks, AK. Improvements in model performance are also seen in Beijing during wintertime haze events (reducing model mean sulfate bias by ~2.9 μgS m-3). This additional sulfur chemistry also improves modeled summertime bias in the southeastern US, with implications for future modeling of biogenic organosulfates.
期刊介绍:
Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere.
The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.