Graduation Year

2013

Document Type

Dissertation

Degree

Ph.D.

Degree Granting Department

Public Health

Major Professor

Amy L. Stuart

Keywords

emissions inventory, fish consumption, mercury, modeling, source apportionment, wet deposition

Abstract

I investigate the links between mercury use, release, deposition, and population exposure in Tampa Bay, with the focus of identifying levers for reducing population mercury exposures. To achieve this, I investigated the trends in mercury use and release by products and processes in the Tampa Bay area using a Material Flow Analysis. Analysis of USEPA National Emissions Inventory data over time (1999 - 2008) identified relevant air source emission categories, and explored and compared state and regional trends in mercury emissions. To understand source contributions to wet deposited mercury in the Tampa Bay area, I analyzed trends in mercury deposition data from the National Atmospheric Deposition Program, Mercury Deposition Network, and the 2001 Bay Regional Atmospheric Chemistry Experiment. I also collected wet deposition samples for mercury and trace metals in the Tampa Bay area during a 6-month campaign at a site at the University of South Florida (USF) campus. Samples were analyzed using Cold Vapor Atomic Fluorescence Spectrometry (CVAFS) for mercury, and Inductively Coupled Plasma Mass Spectrometry (ICP-MS) for trace metals analysis. Concentration data were analyzed for source contributions using HYSPLIT back-trajectory meteorology-based modeling to assess source locations, and the Positive Matrix Factorization (PMF) statistical receptor model to apportion the deposition data by source type. To explore the factors influencing fish consumption behaviors of the local angler population, I analyzed population surveys collected previously from fisher-folks along the Hillsborough River, in Hillsborough County, Florida. Results from the mercury inventory indicate that mercury releases from industrial sources and dental facilities were the most important sources of mercury to the Tampa Bay area. Furthermore, the solid-waste pool was the most important direct sink in the domain, with air emissions an important indirect sink. Emissions inventory data indicated that coal-fired power plants were the largest contributors of mercury emissions in the Tampa Bay area. Medical and municipal waste incineration also accounted for significant fractions of total mercury releases to the domain. Emissions from sources in Hillsborough County accounted for a significant portion of mercury emissions in the region and state. Measurement data indicated that event mercury concentration was only very weakly correlated with event precipitation depth, with both studies showing agreement with this phenomenon. Back-trajectory simulations reveal that high mercury concentration events were often from air masses with recent trajectories over Florida land (6 and 24 hr), and with previous high precipitation depth events over the trajectory in the long term (72 hr). The statistical PMF results indicate the importance of coal burning power plant emissions, medical and municipal waste incineration, and agrochemicals on mercury in wet deposition in the Tampa Bay area. Changes were observed between the 2001 and 2012 data, including greater mercury concentrations in 2012, and the removal of medical waste incineration as a mercury source in the 2012 model results. Together with local emissions inventory data, these results suggest that sources local to the Tampa Bay area and in Florida likely contribute substantially to mercury deposition in the region. Finally, population survey data suggests that mercury exposure risks are poorly understood by the fishing population in Hillsborough County. Taken together, these results suggest that policies targeting mercury emissions control, particurlarly for coal-fired power plants and municipal waste processing, and fish consumption education may be instrumental to the protection of susceptible populations.

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