Investigating sources of gaseous oxidized mercury in dry deposition at three sites across Florida, USA

Abstract. During 2009–2010, the State of Florida established a series of air quality monitoring stations to collect data for development of a statewide total maximum daily load (TMDL) for mercury (Hg). At three of these sites, located near Ft. Lauderdale (DVE), Pensacola (OLF), and Tampa Bay (TPA), passive samplers for the measurement of air Hg concentrations and surrogate surfaces for measurement of Hg dry deposition were deployed. While it is known that Hg in wet deposition in Florida is high compared to the rest of the United States, there is little information on Hg dry deposition. The objectives of the work were to: (1) investigate the utility of passive sampling systems for Hg in an area with low and consistent air concentrations as measured by the Tekran^® mercury measurement system, (2) estimate dry deposition of gaseous oxidized Hg, and (3) investigate potential sources. This paper focuses on Objective 3. All sites were situated within 15 km of 1000 MW electricity generating plants (EGPs) and major highways. Bi-weekly dry deposition and passive sampler Hg uptake were not directly correlated with the automated Tekran^® system measurements, and there was limited agreement between these systems for periods of high deposition. Using diel, biweekly, and seasonal Hg observations, and ancillary data collected at each site, the potential sources of Hg deposited to surrogate surfaces were investigated. With this information, we conclude that there are three major processes/sources contributing to Hg dry deposition in Florida, with these varying as a function of location and time of year. These include: (1) in situ oxidation of locally and regionally derived Hg facilitated by mobile source emissions, (2) indirect and direct inputs of Hg from local EGPs, and (3) direct input of Hg associated with long range transport of air from the northeastern United States. Based on data collected with the surrogate surface sampling system, natural background dry deposition for Florida is estimated to be 0.03 ng m⁻² h⁻¹. Deposition associated with mobile sources is 0.10 ng m⁻² h⁻¹ at TPA and DVE, and 0.03 ng m⁻² h⁻¹ at OLF. Long range transport contributes 0.8 ng m⁻² h⁻¹ in the spring. At DVE ~0.10 ng m⁻² h⁻¹ is contributed directly or indirectly from local point sources. We also suggest based on the data collected with the Tekran^® and passive sampling systems that different chemical forms of GOM are associated with each of these sources.