Spatial and temporal variations of atmospheric chemical condition in the Southeastern U.S.

Abstract

Animal feeding operations (AFOs) are the largest ammonia (NH3) emission sources in the United States (U.S.). However, the impact of NH3 emissions from AFOs on the formation of secondary inorganic PM2.5 (iPM2.5) has not been well understood and systematically assessed. Under the Southeastern Aerosol Research and Characterization (SEARCH) Network, the hourly concentrations of iPM2.5 chemical compositions and its precursor gases as well as meteorological data were measured at eight urban/nonurban sites labeled as JST/YRK, BHM/CTR, GFP/OAK, and PNS/OLF during 1998–2016. Using the SEARCH data, this research investigated the spatiotemporal variations of atmospheric chemical conditions in those rural and urban areas. The spatiotemporal variations of atmospheric chemical conditions at the eight sites are characterized by four parameters, including (1) gas ratio (GR), (2) gas-phase NH3 molar fraction (NH3/NHx), (3) total available NH3 (gaseous ammonia + aerosol ammonium) to sulfate (SO42−) molar ratio (TA/TS), and (4) PM2.5 ammonium + nitrate to total PM2.5 mass ratio (AN/PM2.5). Results indicate that the NH3 emissions from AFOs may explain the greater values of GR, NH3/NHx, and TA/TS in the wind directions coming from AFOs at YRK and OAK rural sites than the other wind directions. In the wind directions coming from AFOs at YRK and OAK, NH3 was in excess of fully neutralizing acidic gases, more NH3 stayed in gas phase than those in other wind directions, and both ammonium sulfate and ammonium nitrate existed in iPM2.5. The upward trend in NH3/NHx indicates that gas-particle partitioning ofNH3–NH4+shifted toward gas phase, while the downward trend in AN/PM2.5 may implicate that smaller fraction of PM2.5 was directly NH3 sensitive. Understanding of the spatiotemporal variations of atmospheric chemical condition provides insights to improve our understanding of iPM2.5 formation under rural and urban conditions, the reduction in sulfur dioxide (SO2) and nitrogen oxides (NOx) emissions resulted in the reduction of iPM2.5 formation despite the increase in NH3 emissions in the Southeastern U.S.