Final Report Florida DEP PO# S3700 303975 Tetra Tech, Inc subcontract agreement # 11718-02 Trends of Anthropogenic Mercury Mass Flows and Emissions in Florida Submitted by: Janja D. Husar and Rudolf B. Husar Lantern Corporation 63 Ridgemoor Dr. Clayton, MO 63105 Project Officers: Thomas Atkeson, PhD Florida Department of Environmental Protection Mercury Program 2600 Blair Stone Rd, MS 6540 Tallahassee, FL32399 and Curtis Pollman, PhD TetraTech, Inc 408 W. University Ave. Suite 308 Gainesville, FL 32608 June 25, 2002 Table of Contents Summary......................................................................................................................................... 3 Introduction.................................................................................................................................... 6 National Anthropogenic Mercury Budgets and Mass Flows ................................................ 6 Mobilization of Mercury in Fuels and Goods: U.S. National Trends .................................. 9 Approach and Results............................................................................................................... 9 Summary: US Mercury Flow in Fuels and Goods ............................................................... 26 Trend of anthropogenic mercury in Florida ............................................................................... 29 Florida Mercury Flow in Fuels .............................................................................................. 29 Florida Mercury Flow in Products ........................................................................................ 33 Summary: Florida Mercury Flow ......................................................................................... 36 Summary: Florida Mercury Emissions ................................................................................ 37 Trend of anthropogenic mercury in Southern Florida .............................................................. 41 Mercury Flow Methodology................................................................................................... 41 County by County Mercury Flow ......................................................................................... 43 Mercury Emissions for the Broward, Dade and Palm Beach Counties Methodology ..... 45 County Mercury Emissions.................................................................................................... 47 Preliminary comparison of mercury emission estimates by RMB Consulting and this mercury flow study ................................................................................................................. 48 References .................................................................................................................................... 49 Appendix ....................................................................................................................................... 52 2 Summary The amount of mercury mobilized in fuels and goods was estimated for 1930-2000 for US and Florida. The emissions of mercury to the atmosphere for 1930-2000 were also estimated. The distribution and fate of mercury as it cycles through the biosphere and lithosphere was not discussed in this report, neither was the chemical speciation of mercury emissions. Mercury Mobilization The approach used in this report was based on fuel consumption and mercury use in production of mercury containing products. The US coal production compiled by coal mining region and the mean mercury content for each producing region was used to calculate the yearly Hg mobilization rate. For Florida, the weighted average Florida coal mercury content was calculated for 1998 based on coal shipments and associated Hg content. The rather broad logarithmic standard deviations σg of coal mercury content was noted. For both US and Florida, the mercury mobilization in petroleum was estimated from distributed petroleum products. This reconstruction is presently feasible, since there are more reliable available data on mercury concentration in refined products. The releases of mercury at refineries to air, water, and solid waste were not addressed, lacking reliable data on oil content in crude oil. The mobilization of mercury through mercury containing products was assessed using two approaches. The first approach utilized U.S. Bureau of Mines (BOM) mineral commodity summaries on mercury (U.S. Bureau of Mines, yearly). The categories that BOM reports as end users of mercury are: electrical (batteries, lighting, wiring/switches); paint; agricultural chemicals; measuring and control instruments, laboratory use; pharmaceutical; dental; chlorine and caustic soda manufacturing; and other uses. The above approach provides the upper limit of mercury input in the environment. The second approach was to use the consumption of goods and mercury content in the goods to estimate yearly mobilization of mercury. The two approaches were then compared and analyzed. The mercury mobilization in products in Florida for the electric, laboratory use, control and dental sectors was apportioned by Florida population. Agriculture sector was apportioned by acreage used in vegetable production and golf course statistics. Chlorine and acoustic soda manufacturing use of mercury was omitted from Florida trends, since the manufacturing was done outside Florida and the products do not contain mercury. The “Other” category was also omitted. The amount of mercury mobilized by human activity from 1930-2000 was estimated for US and Florida. Table S1. Cumulative mercury mobilization in (Mg). 1930-2000. US Florida Coal 7,000 62* Petroleum 365 7 Product Usage 106,800 1,986 Total 114,125 2,055 3 Mercury Emissions US emission trends were estimated based on the following assumptions: for coal an average of 50% emissions factor was used and for crude oil mercury concentration was assumed to be 10 ppb. For paint emission at 75% in the first year after application was assumed, with the remainder released to water and soil. For electrical, laboratory use, and control category it was assumed that 30% was incinerated for 1930-1960. For the period 1960-2000, lower combustion factors based on literature were used. A tentative atmospheric emission trend is presented in Figure S1. A notable feature of the emissions trend is the sharp drop since 1990. The largest mercury emissions in the 1970-1990 period were associated with water-based paint applications and electrical (battery) devices. Coal contribution in the 1990s has increased compared to other categories. Figure S1. Trend of estimated US mercury emissions to the atmosphere. The mercury emissions in Florida were estimated by assigning an air emissions fraction to each category. Coal emissions were taken as described below by using median mercury content in coal (Figure S3). For the paints it was assumed that 75% of mercury is emitted to the atmosphere in the first year after application. Laboratory, electrical, and control products were assumed to be disposed to the municipal solid waste (MSW) with a portion of the MSW incinerated. The fate of mercury retained at mines and in fly ash was not discussed, neither was the fate of mercury that remained in landfills with products disposition. Figure S2. Trend of anthropogenic mercury atmospheric emissions in Florida 1930-2000. 4 The long term trend coal mercury emission data for Florida arise form the current “production driven” estimates. This method relies on the mercury concentration of coals as measured at various coal beds and subsequently cleaned and shipped to Florida. Florida coal consumption has tripled since the early 1980s. Electric utilities were the dominant coal consumers. In 1999, 97% of coal shipped to Florida was combusted in power plants. Eastern US coal is cleaned at mines (assumed 21% mercury removal). According to the literature in Florida, the efficiency for mercury removal in power plants was 57% in 1999. Based on the removal efficiency at power plants in 1999, the mercury emission trend from coal combustion was reconstructed for Florida (Figure S3). The estimated amount of mercury emitted in Florida by coal combustion in 1999, was 1.93, 1.18, 0.93, and 0.42 Mg/yr for the weighted average coal mercury content for 84th percentile, mean, medium, and 16th percentile, respectively. Figure S3 also shows the Information Collection Request (ICR) based mercury emissions at power plants in Florida. For 1999, the EPRI ICR mercury emission estimate was 0.86 Mg/yr and the EPA estimate was 0.87 Mg/yr. In 1999, the median and mean emission estimates from our materials flow method were 0.93 Mg/yr and 1.18 Mg/yr, respectively. Evidently, the ICR estimate are somewhat below the mean and median but are well within the range of the possible coal mercury emissions. In fact, the correspondence between the two independently measured estimates is considered to be excellent. Figure S3. Mercury emissions of coal used in Florida, based on coal origin and coal content in coal as-mined (Figure 30) and estimated 21% removal of mercury by coal washing and cleaning at mines, and estimated 57% removal efficiency at power plants in Florida (Chu, 2000). Estimated ICR power plant mercury emissions in Florida for 1999 were 0.86 Mg/yr (Chu, 2000) and 0.87 Mg/yr EPA, 2000. 5 Introduction The basic elements of life including carbon, nitrogen, phosphorus, calcium are in constant circulation between the earth’s major environmental compartments: atmosphere, hydrosphere, lithosphere, and biosphere, Figure 1 (Husar and Husar, 1991). These earth’s compartments remain in balance as long as the rate of flow of matter and energy in and out of the compartments is unchanged. Changes in the environmental compartments will occur if the circulation (in and out flow) of the substances is perturbed. Trace elements, unlike C, N, P and Ca, have a slow and sluggish cycle through the four environmental compartments. Lead, mercury and other metals tend to accumulate in the lithosphere or parts of the biosphere. Figure 1. The four environmental spheres (Husar and Husar, 1991). The importance of mercury (Hg) as an environmental contaminant stems from its ubiquitous nature due largely to the magnitude of sources, its volatility, mobility, and persistence in nature (Dvonch et al., 1995). Man made sources of mercury include mining, smelting, industrial manufacturing, consumer products containing mercury, fuel combustion. In this study the trend (1930-2000) of mercury mobilization in fuels and products and consequent emissions to the atmosphere was constructed for the US and then applied to regional level in Florida. National Anthropogenic Mercury Budgets and Mass Flows Recent work by Sznopek and Goonan, 2000 contains an updated trend of the national mercury flow that includes the primary production, consumption, recycling as well as mercury flow from stocks. The apparent mercury supply (Figure 2) includes primary and secondary production, net imports, and government stockpile releases. From 1970 to 1986, the main contributors to mercury flow were primary mine production and imports. From 1993 on, the primary mine production was negligible, the secondary production (recycling) increased and stock releases were terminated. During 1988-92, the consumption of mercury for industrial purposes declined to a record low (Engstrom and Swain, 1997). 6 Net Import Stock Stock Release Mining Mine Production Production Consumption Secondary Production Recycling Figure 2. Trend of the US ‘apparent’ mercury supply, 1970-1998. (Sznopek and Goonan, 2000). The EPA Mercury Report to Congress, 1997, addressed the atmospheric emissions of mercury. The report concluded that the mercury releases to the atmosphere in 1995 were dominated by coal and oil combustion (53%) (Figure 3). Figure 3. Mercury atmospheric emission inventory (EPA, 1997). Sznopek and Goonan, 2000 used the EPA Mercury Report to Congress, 1997 data for atmospheric emissions and added the flow of mercury in products (industrial goods). For 1996, they report that estimated 144 Mg of mercury was emitted to the atmosphere (Figure 4 and 5) 7 based on combustion of fuels and goods incineration. They also reported that in 1996, 295 Mg mercury in industrial goods was disposed into landfills (Figure 5). Sznopek and Goonan, 2000 reported that in 1996, stocks of mercury totaled 6,800 Mg (private) and 4,600 Mg (U.S. government, not shown in Figure 5), totaling 11,400 Mg of mercury. They also pointed out that given the 1996 mercury industrial demand of 372 Mg/yr (U.S Bureau of Mines, 1996) for creating goods, the US has a 27-year stockpile of mercury. Figure 4. Materials flow schematics for 1996. The blue lines are atmospheric emissions from the EPA (1997) report, adding to 144 Mg/yr atmospheric emissions. The right hand portion of the schematics depicts mercury flow in goods (Sznopek and Goonan, 2000). Figure 5. 1996 mercury flow and disposition (Mg/yr), in goods (Sznopek and Goonan, 2000). 8 Mobilization of Mercury in Fuels and Goods: U.S. National Trends Approach and Results This section describes the mobilization of mercury in fuels and goods at the national level. The anthropogenic mercury flow through the environment was reconstructed from historical data on fuel consumption, and use of mercury in manufactured products. For some goods (electrical and paint) the product shipments/or retail sales, combined with mercury concentration in products was also used to estimate the mercury flow. U.S. Mercury in Fuels Coal The production of coal was compiled by coal mining region since 1800, (Milici, 1997). Coal production in U.S. reached 500 million Mg/yr in the early 1900s. The slowing demand for coal was evident in the late 1930s and the early 1950s. However, since the 1950s the coal production has doubled. The 1999 coal production reached 1,027 million Mg/yr (Figure 6, Appendix Table 1). Until the 1950s the Appalachian basin was the principal coal-producing region. The increased coal demand, since the 1970s, was met by the western coal (Milici, 1997). For the past twenty years the USGS compiled an extensive database (COALQUAL) for mercury content in coal by coal mining regions. The mean mercury content for each producing region was obtained from Finkelman and Tewalt, 1998 (Table 1). Mercury mobilization in coal was obtained by multiplying the coal production of every mining region with appropriate coal mercury content (Table 1). By 2000, the mercury mobilization through coal exceeded 140 Mg/yr (Figure 7, Appendix Table 3). Cumulative over 70 years (1930-2000), about 7,000 Mg mercury was taken from the geological deposits and distributed into the environment, mostly through combustion to the atmosphere (3,500-5,200 Mg) and directly to land and water (1,800-3,500 Mg). Table 1. Mercury content of coal (Finkelman and Tewalt, 1998; Toole-O’Neil et al., 1999). Hg conc., ppm Appallachian 0.20 Eastern Interior 0.10 Gulf Coast 0.22 Rocky Mnts 0.09 Great Plains 0.12 9 Figure 6. US coal production trend and production distribution by coal producing regions. Figure 7. Trend of mercury mobilized in coal. High (75%) and low (50%) estimates of mercury atmospheric emissions are also shown. 10 Petroleum Petroleum products also carry mercury from the geological reservoir and distribute mercury to the environment along their passage. To reconstruct mercury flow through petroleum, we begin by examining crude oil consumed along with the crude oil mercury concentration. At present, there are insufficient data on crude oil mercury content with high degree of confidence. (Wilhelm, 2001). The range of reported mercury content in crude oil spans from <10 ppb to 30,000 ppb. Wilhelm, 2001 analyzed the existing crude oil mercury concentration database and estimated that the mean crude oil concentration can be assumed at 10 ppb. The crude oil consumption in US refineries was obtained from the Department of Energy database (U.S. DOE, (a)). If we assume the mean mercury concentration of crude oil at 10 ppb, then the cumulative amount of mercury mobilized by crude oil consumed in the period 19302000 would be about 400 Mg, which is about an order of magnitude smaller than mercury mobilized by coal. However, if mercury concentration in crude oil is found by future research to be different, the consequences will vary. If concentrations of crude oil were found to be <10 ppb, then the petroleum impact on the environment will be even lower than the one presented in this report. The other extreme is, however, if the crude oil mercury concentrations were found to be >50 ppb, then crude oil contribution to the environment could reach levels similar to coal contributions. Wilhelm, 2001 examined the pathway of crude oil processed in the United States. In 1999, input of crude oil into US refineries was about 0.82 billion Mg/yr. Taking the mean concentration of mercury in crude oil to be 10 ppb then about 8.1 Mg of mercury was mobilized with crude oil in 1999. Out of 8.1 Mg mercury mobilized, 4.8 Mg mercury was distributed through the refined products to be burned later, while 1.5 Mg was released in the air at the refineries. Additional 1.8 Mg was disposed to wastewater and solid waste at the refineries (Figure 8). Figure 8. Mass balance of mercury flow at refineries in 1999 based on average 10 ppb mercury content in crude oil (Wilhelm, 2001). Lacking data on mercury content of crude oil at refineries or refinery mercury releases (air, water, and soil) we have omitted the contributions from the refineries in our report. Mercury flow at refineries is an important pathway and it should be resolved with future monitoring of crude oil mercury concentration at refineries as well as monitoring of refinery releases to air, wastewater and solid waste. (Minnesota Pollution Control Agency, 1999). The approach we have used is the estimation of mercury flow in distributed petroleum products. This flow is presently easier to reconstruct, since there are more reliable data available on mercury concentration in refined products, Wilhelm, 2001 (Table 2). 11 Table 2. Mercury content of petroleum products (Wilhelm, 2001). Hg conc, ppb LPG Asphalt & road oil Aviation gasoline Distillate fuel Jet fuel Kerosene Lubri cants Motor gasoline Residual fuel Other 10 0.27 2.0 5.0 2.0 0.04 10 2.0 10 50 The consumption of petroleum products was obtained from U.S. DOE EIA State Energy Data Report for 1960-2000 (US DOE, 1999), and from U.S. Bureau of Mines for 1936-1960, Figure 9, Appendix Table 2. The mercury content of petroleum products was obtained from Wilhelm, 2001, Table 2. Mercury US flow was then calculated (Figure 10). Residual, distillate and jet fuels, as well as motor gasoline are distributed and consumed throughout U.S., while the “other” (petroleum feedstocks, petroleum coke, still gas, naphtas, pentanes, plant condensate, wax and various blending components) category and LPG are consumed at both refineries and distributed to utilities. Mercury mobilization for petroleum products in U.S. increased from about 1.5 Mg/yr in 1930 to about 6 Mg/yr in 1999. As shown in Figure 10 and Appendix Table 4, the flow of mercury in petroleum products was about two orders of magnitude lower than the coal mercury flow. In the period 1930-2000 about 260 Mg Hg was distributed over US in products. Figure 9. U.S. consumption of petroleum products. Figure 10. US mercury flow trend in petroleum products. 12 U.S. Mercury in Products The flow of mercury from products into the environment for 1930-2000 was assessed using two approaches. The first approach was to utilize U.S. Bureau of Mines (BOM) mineral commodity summaries on mercury (U.S. Bureau of Mines, yearly). The categories that BOM reports as end users of mercury are: Electrical (batteries, lighting, wiring/switches) Paint Agricultural chemicals Measuring and control instruments Laboratory use Pharmaceutical Dental Chlorine and caustic soda manufacturing Other uses The above approach provides the upper limit of mercury input in the environment. The second approach was to use the consumption of goods and mercury content in the goods to estimate yearly flow of mercury. The two approaches were then compared and analyzed. Electrical Sector The electrical sector as reported in BOM, encompasses the use of mercury in production of batteries, switches and wiring, and fluorescent and high intensity lighting products. The electrical sector represented the largest mercury consumption category between 1976-1986, reaching levels of 1,000 Mg/yr (63% of total mercury use in products), and declining to approximate <80 Mg/yr in 1999 (25% of total mercury use in products), Figure 11. Thus, the mercury in electrical sector is of the greatest importance in assessing the mercury flow and pathways of mercury through the environment. Figure 11. The electrical sector percentage of total mercury consumption in goods (U.S. Bureau of Mines). In 1941, BOM quotes that the electrical sector amounted to 8% of total mercury uses. The fluorescent lighting and batteries were the only electrical uses reported and that the above two categories used about equal amount of mercury. In subsequent years, however, BOM reported only a single mercury consumption number for electrical uses. In 1978, BOM started reporting electrical mercury uses in three categories, battery, switches/wiring, and lighting with their cumulative value representing the electrical consumption (Jasinski, 1994). In 1998, BOM stopped reporting mercury consumption in products altogether. In subsequent years, only 13 narrative statements on consumption were reported. For example in 1999 BOM reports, "approximately 25% of mercury consumed domestically was for electrical and electronic applications”. Electrical uses of mercury have increased since 1941. There was a sharp peak in electrical sector consumption in 1944 and 1945, followed by a sharp drop to pre 1941 levels. After 1947 the use of mercury in electrical sector has leveled off at around 250 Mg/yr until the early 1960s. In the late 1960s and early 1970s mercury consumption in electrical sector increased slightly. In the late 1970s the electrical use of mercury increased exponentially, reaching levels of 1,000 Mg/year from 1976 to 1986. In the late 1980s and early 1990s mercury use in the electrical sector dropped dramatically, falling to 86 Mg/yr in 1997 (Figure 12). The electrical categories, (batteries, switches, and lighting) were reconstructed using literature information. Sznopek and Goonan, 2000 reconstructed the use of mercury in wiring and switching sector for the period 1963-1978. We have reconstructed the lighting sector by assuming monotonical increase of mercury use and anchored our starting and ending points at 1941 and 1978. From the difference the mercury use in battery sector, 1941-1978 was reconstructed (Figure 12, Appendix Table 5). It is interesting to note that in the 1980s, according to BOM data, batteries dominated the use of mercury in electrical category, while in the 1990s, switches and lighting were more important (Figure 13). Figure 12. U.S. Bureau of Mines data for electrical sector. In 1978 BOM started reporting electrical data in three categories, batteries, switches/wiring and lighting. Switches/wiring were extended to 1963 by estimates of Sznopak and Goonan, 2000, lighting sub-category was extrapolated to 1941. Figure 13. Comparison of 1986 and 1996 electrical mix obtained from BOM data. In 1986, use of mercury in electrical sector (901 Mg/yr) was dominated by battery industry demand. In 1996, in the electrical sector (78 Mg/yr) the battery industry eliminated the use of mercury in its products, and only switches and lighting industries were reporting mercury use (US Bureau of Mines). 14 Batteries In the early 20th century, consumer batteries were made from carbon-zinc. Shortly before WWII Samuel Ruben invented the mercury primary cell. Mercury-zinc batteries were originally used in hearing aids, and their use has been expanded to transistorized equipment, watches, calculators, etc. Alkaline batteries were invented in 1959 by Lew Urry for Eveready and battery consumption increased exponentially since 1967. Beginning in the late 1980s, state legislatures began enacting laws to phase out mercury use in batteries. Mercury use in alkaline batteries was eliminated in the early 1990s. In 1996, mercury use in all household batteries was banned, except for limited non-household uses (NEMA, 1996). Estimates based on mercury consumption (BOM). Mercury use in the battery industry was documented by BOM since 1978 (Jasinski, 1994). In 1941, BOM reported that 162 Mg was used by the electrical sector with equal amounts used for lighting and batteries (81 Mg). Based on information that lighting and switching industry mercury use was relatively constant over this period (Sznopek and Goonan, 2000), battery industry consumption 1941-1978 was reconstructed and shown in Figure 14 (dashed line). Estimates based on battery discards (EPA, 1992). In another approach by EPA, 1992, the amount of mercury discarded in the environment was estimated based on the battery retail sales. The retail sales were provided by the National Electrical Manufacturers Association (NEMA) for 1963-1988, including projections for 1993, and 1998. The amount of mercury battery import was assumed at 15 %. It was also assumed that all batteries sold were discarded within two years. The mercury content of different types of batteries was established. Based on the above information mercury discard into the environment was then calculated (EPA, 1992) and shown in Figure 14. Figure 14. Mercury flow through batteries. The top line represents mercury use in battery production (BOM). The reconstructed trend is from EPA, 1992 based on sold and discarded batteries. As shown in Figure 14, mercury consumption in battery industry (BOM) in the period 19851995 is twice the amount of mercury discarded to the environment from the battery retail sales and their respective mercury content (EPA, 1992). Since the EPA, 1992 method assumes a battery life of two years after purchase, the 1990-2000 period shows higher amounts of mercury still entering the environment. The cumulative amount of mercury estimated to flow to the environment in the period 1967-2000 using BOM data amounts to 15,300 Mg Hg, while the EPA, 1992 method to 10,800 Mg Hg. For the 1991-2000 period only 100 Mg mercury has 15 entered the environment (BOM), while based on the EPA, 1992 method 2,000 Mg Hg was discarded to the environment. The question of mercury flow to the environment from the battery sector could not be fully resolved at this time. The amount of mercury consumed by the U.S. battery industry (BOM) was, therefore, used in this study as an upper limit of mercury flow to the environment. Fluorescent and High Intensity Discharge lights Fluorescent and high intensity discharge (HID) lights were invented in the 1930s. Since the 1960s the shipments of fluorescent and HID lamps increased monotonically as shown in Figure 15 (U.S. Bureau of Census, yearly, (a)). Estimates based on mercury consumption (BOM). In 1941, BOM reported that 162 Mg mercury was used by the electrical sector with equal amounts used for lighting and batteries, 81 Mg each. In the subsequent years BOM reported lighting as part of the electrical industry consumption. From 1978 to 1997, the lighting category was again reported separately. Lacking any other information we have linearly decreased the amount of mercury used in lighting industry from 1941 to 1978 (Figure 16). Estimates based on fluorescent and HID discards. The alternate mercury flow in lighting was reconstructed using U.S. Bureau of Census (BOC) fluorescent and HID lamps domestic shipments (Figure 15, Appendix Table 7). The fluorescent and HID industry provided mercury content of lamps (75 mg/lamp, 55 mg/lamp, 30 mg/lamp) for different time periods, and HID mercury content (33 mg/lamp and 25 mg/lamp) (EPA, 1992; Benazon Environmental, 1998) (Figure 15). The shipments and the appropriate industry provided Hg content was the basis of the reconstructed flow of mercury in the lighting sector (Figure 16, Appendix Table). It is apparent from these two mercury flow estimates (Figure 16) that the BOM estimate of the lighting industry mercury consumption is twice the estimate of mercury discarded with lamps in the 1980s. In the 1990s the difference is about 25%. The historical information prior to 1978 should be used with caution, but it could be estimated as about 20-80 Mg/yr, and an order of magnitude smaller than the battery flow. It is to be noted that the lighting sector contribution to mercury flow in electrical sector in 1980s was small, between 4-5% (Figure 13 and Figure 19). However, once the use of mercury in batteries was eliminated in 1996, the lighting contribution rose to 16-37% of mercury used/discarded in the electrical sector (Figure 15 and 19). Figure 15. Fluorescent and HID lamp shipments and Hg content in fluorescent lamps. The declining dashed/solid line is the approximate mercury content of mercury-based lamps, obtained by dividing mercury use (BOM) in lighting industry by fluorescent and HID lamp shipments. 16 Figure 16. Reconstruction of mercury use in lighting using U.S. Bureau of Census fluorescent and HID lamps shipments, and mercury content in lamps (Benazon, 1998) The life time of lamps was assumed as four years.. Wiring Devices and Switches This category covers mercury in wiring devices and electric light switches. The EPA's Mercury Study Report to Congress, (EPA, 1997) noted that the electrical switches containing mercury were not manufactured prior to the 1960s. The switching/wiring industry according to Sznopek and Goonan, 2000 has not changed much since the 1960s, contributing around 100 Mg/yr in 1960-1980. The 1982 US economic recession was evident in reduced usage of mercury for switches (Figure 17). The late 1980s showed an increased demand for mercury followed by the 1990s when alternative non-mercury switches were introduced. According to BOM, 1997 “in many applications, mercury switches are replaced with either electronic or other special switches”. The U.S. EPA, 1997 reported that 10% of the switches were discarded after 10 years, 40% after 30 years, and 50% after 50 years. Taking all these factors into consideration the 1996 mercury flow to the environment was 64 Mg/yr. Sznopek and Goonan, 2000 also estimated that 50% of the switches will be recycled, thus 32 Mg/yr was recycled in 1996 and that therefore only 32 Mg/yr entered the environment. Based on the above assumptions the flow of mercury from switches to the environment will continue for decades, even though the switch industry has eliminated mercury from its products. Figure 17. Mercury use in wiring devices and switches. Reconstructed mercury in switches using the Sznopek and Goonan, 2000 method. 17 Electrical Sector Summary Historically, the electrical sector has contributed the largest amount of mercury to the environment. Fortunately, two rather independent methods were available to estimate this mercury flow: BOM mercury use by electrical sector and mercury estimates obtained using retail sales/shipments were thus compared. The BOM data are continuos from 1930-1997 but do not take into account exports and imports, and the life cycle of the products. The BOM method gives almost a factor of two higher mercury flow estimate in 1980-1990 period. However, in the 1990s the retail method based on retail and life cycle of products gives a somewhat higher estimate than BOM method (Figure 18, Appendix Table 6). In 1986 in the retail method, batteries contributed 92% of the total electrical uses, while in 1996 batteries contribution decreased to 57% (Figure 19). Switches accounted for 4% of electrical uses in 1986 and 17% in 1996, and lighting share increased from 4% to 16% (Figure 19). Batteries’ contribution to the reconstructed (retail) flow of mercury in 1995-2000 may be overestimated, since the retail estimates were based on EPA, 1992. Unfortunately, more recent data on battery retail, exports and imports were not available. Another aspect of this comparison is that it is estimated that about 15,000 Mg of mercury was used in U.S. to produce batteries since 1969. Electrical discard estimate for the same period was about 12,000 Mg. The 3,000 Mg Hg unaccounted for were either exported from U.S. or the retail approach underestimated the sales/discard of batteries and/or the mercury content of batteries. Lighting sector has used about 1,100 Mg Hg since 1967. It was estimated that about 800 Mg was discarded to the environment and about 300 Mg is the difference in these two estimates. However, this industry has not found a replacement for mercury. It is still using mercury for its products (<20 Mg/yr) and will continue to contribute mercury to the environment. The recycling is often mentioned as a future venue of keeping mercury out of the environment. Switches, have a life expectancy of up to 50 years. Thus, in years to come, switches will contribute to the flow of mercury into the environment. Up to year 2000, more than 3,000 Mg Hg was used in switches. It is estimated that about 700 Mg were discarded into the environment and more than 2,300 Mg Hg are probably still in the switches in use. The switches will be either recycled or discarded in the environment and their effect might linger for decades. Figure 18. Electrical sector, comparison of BOM mercury flow and reconstructed based on shipments and mercury content of electrical products, including life span of products. 18 Figure 19. Comparison of 1986 and 1996 reconstructed electrical mix obtained from retail sales/ shipment data and mercury concentration in products, including life expectancy of products. 19 Paint Sector The next largest category of mercury use in products in the 1980s was the water soluble (latex) paint category (Barr Engineering, 2001). In the late 1950s organomercury compounds, and phenylmercuric acetate in particular, were added to the water type paints to prolong the paint's shelf life as fungicides. EPA provided certain guidelines for the paint industry, restricting interior water type paints to 300 ppm Hg, and exterior water type paints to 2000 ppm Hg. The paint industry was not required to report on mercury concentration of its products. Apparently it varied, reaching sometimes >900 ppm for interior latex paint (CDC, 1990). The Benazon Engineering Company, 1998 reports interior latex paint mercury concentration of 45 ppm, and exterior 1050 ppm (estimate that only 20% of exterior latex contained mercury), based on interviews of paint companies in 1990s (Figure 20, Appendix Table 8). Figure 20. Mercury content, EPA guidelines and Benazon, 1998 estimates for interior water type paints. The declining solid line is the approximate mercury content of water type paints, obtained by dividing mercury use (BOM) in paint industry by water type paint shipments. Estimates based on mercury consumption (BOM). Historical use of mercury in paint industry can be reconstructed using BOM data. Mercury in paint was completely eliminated in 1990 (Benazon, 1998). Estimates based on paint shipments. The information on US paint shipments is available from the U.S. Bureau of Census, (annual) Current Industrial Reports. The historical total paint shipments were obtained from U.S. Bureau of Census, 1975. The total paint shipments increased since the 1950s. In 1955 the Bureau of Census started reporting as a separate category gallons of paints shipped as architectural paint. The percentage of architectural paints of total paints used in US remained relatively constant at about 42% since 1955. In 1965, the architectural paint was further subdivided and reported as solvent and water type, interior and exterior type, respectively. In the early 1960s solvent based paints were dominant. However, water type paints took over the market and by 1990 and contributed to more than 60% of architectural paints. (Figure 21). To reconstruct mercury in paints using paint shipment, EPA guideline of 300 ppm was assumed. Figure 22 shows that trend of Hg use in the industry can be reconstructed for 1960 to 1980 using EPA guidelines. In the 1980s, the paint industry reduced the amount of mercury in water type 20 paints. According to paint industry information (Benazon, 1998) Hg average concentration of indoor water type paints in the 1980s, was 45ppm, and up to 1050 ppm in exterior type paints (20% exterior type paints contained Hg). In 1990, the use of mercury fungicides in paints was banned. Using the above information the mercury flow in paint was reconstructed. Figure 21. U.S. trend of shipment of all paints, architectural paints, including water-type, and solvent type paints (in 1000 of gallons). Figure 22. Reconstruction of US mercury in paint (Appendix Table 9). The cumulative use of mercury by paint industry for 1930-2000 was about 8,400 Mg. According to (Taylor and Tickle, 1969, Taylor et al., 1969, Taylor and Hunter, 1972) as quoted in Benazon Environmental, 1998, 50% of the mercury of indoor paint and 75% of the outdoor paint is volatilized into the atmosphere in the first year after application. The Minnesota mercury emission inventory (Barr, 2001) uses 75% mercury volatilization per year. The remaining 25% of the mercury in paint is released subsequently to the atmosphere or is washed off (exterior paint) by rain. Since the paint industry has discontinued use of mercury in paint in 1990, mercury flow by this sector should be negligible in 2000. 21 Agriculture In agriculture mercury was primarily used as fungicide. The fungicidal properties of mercurial compounds have been recognized since the latter part of the 19th century. Originally the major usage of inorganic mercury compounds was for seed protection. Mercury fungicides, containing 2 to 4% of metallic mercury were used for application to seeds, cotton, rice, wheat, rye, barley, oats, flax, peanuts, safflower. Also mercury fungicides were used as seed protectants for potato seed pieces, for cabbage seedlings, for gladiolas, and other bulbs. Mercurous chloride was continued to be recommended for turf and golf course treatment (Sharvelle, 1961) throughout the 1970s (Murphy and Aucott, 1999). In the 1960s, with introduction of organic mercurials the range of their application has been expanded from seeds to foliage protection (Sharvelle, 1961). Mercurial fungicides were used as foliar fungicides for scab of apples, pears, strawberries and other fruits. Based on US Bureau of Mines statistics (Jasinski, 1994; Murphy and Aucott, 1999) mercury consumed in agriculture in 1930-1940 ranged between 50 Mg/yr, representing 13% of total US mercury consumption (Murphy and Aucott, 1999). Between 1940-1960 mercury consumption in agriculture steadily increased reaching its peak in 1956. In 1970, the use of mercury fungicides in agriculture was banned. However, the use of mercury fungicides remained legal for specific diseases and for turf management. By 1980 only 1 Mg/year was reported as used in agriculture (Figure 23). The uses of mercury as fungicides was documented by Sharvelle, 1961 and Murphy and Aucott, 1999. Table 3 was assembled to account for mercury use in agriculture. Wheat, barley, oats, rye Apples Turf Potatoes Cabbage Vegetables and Fruits Bulbs and corms Hg estimate 0.3-0.6 g/bushel (seeds) 4.5-9 g/acre 43 gr/acre Seed soaking Soil treatment Seed soaking, foilage treatment Bulbs and corms soaking Reference Sharvelle, 1961 Murphy and Aucott, 1999 Sharvelle, 1961 Sharvelle, 1961 Sharvelle, 1961 Sharvelle, 1961 Sharvelle, 1961 Table 3. Mercury use in agriculture. US Department of Agriculture (USDA) annual Agricultural Statistics was used to obtain drivers for small seed (wheat, barley, oats, rye) consumption in USA (Appendix Table 10). Using Sharvelle, 1961, 0.3g of mercury application per bushel, the consumption trend of mercury for USA was reconstructed in Figure 23, Appendix Table 11. For 1930-1946 the use of mercury fungicide was overestimated compared to Bureau of Mines estimate of mercury use in agriculture. For 1947-1970, the mercury use for seeds slowly declined, due to decline in tonnage of seeds used in agriculture. The use of fungicides for golf courses was estimated using the number of golf courses in USA (Scharff, 1970, Ross, 1979, NGF web site). The size of the golf course was assumed as 80 acres. 22 The treatment recommended required 43 g/acre of mercury (Sharvelle, 1961). This estimate is an upper limit. The routine treatment of golf courses with fungicides was prevalent in the late 1950s and the 1960s. In previous years, all the literature suggests that only affected areas were treated with much higher concentrations of fungicides. In 1970s mercury fungicides were gradually substituted with non-mercury fungicides. The use of mercury for foliage treatment started in 1942. Apples and pears were mainly treated with organomercury compounds. Annual acreage of apples was obtained from USDA Agricultural Statistics and 4.5 g/acre (Murphy and Aucott, 1999) was applied since middle 1940s. The use of mercury for potato seeds, vegetable seeds (tomatoes, watermelon, beets), for soil treatment for cabbage and cauliflower, for flower bulbs and corms is not well documented to apportion the mercury use. Therefore, the remaining mercury (after subtracting small grain, apple, and turf use) in the 1950 and 1960 was apportioned to vegetables and others. Figure 23. Apportionment of mercury use in U. S. agriculture In U.S. in the period 1930-2000 approximately 3,717 Mg of mercury was used for agriculture and golf courses. A certain amount of mercury may have volatilized, while the rest remained in soil and or leached to subsoil and ground water (Murphy and Aucott, 1999). 23 Measurement and Control Devices Sector This category primarily includes manometers, barometers, thermostats, and thermometers. For this category we have used data as supplied by BOM. The cumulative use of mercury by the control sector for 1930-2000 was about 10,000 Mg, and it was generally in a range of 100-200 Mg/yr per year. In the1990s the use of mercury in control devices has declined from 100 Mg/yr to around 24 Mg/yr. The fate of these devices was described by Barr, 2001. Barr, 2001 estimates that in 1990 about 1,000 Mg mercury is still in measurement and control instruments. He also estimates that for 1990, 60 Mg was recycled, and 47 Mg mercury was incinerated or disposed in a landfill. However, there is no historical information on disposition procedures. It can be thus inferred that from 1930-1990, about 9,000 Mg mercury was disposed cumulatively and most likely into the municipal solid waste (MSW). Laboratory Sector According to Sznopek and Goonan, 2000 this category included mercury use in laboratory instruments, and as reagents and catalysts. For this sector we have used data as supplied by BOM. The cumulative use of mercury by laboratory sector for 1930-2000 was about 1,800 Mg, and it was generally about 20-30 Mg/yr per year. In the 1990s Sznopek and Goonan, 2000 estimate that most of the mercury in the laboratory sector is recycled, while a small fraction is incinerated or disposed in landfills. There is no information on historical disposition procedures. Pharmaceutical Sector This category includes mercury used in pharmaceuticals. Historically, it was extensively used in the production of skin and hair bleach (ammoniated mercury), cathartics, antiseptics, and diuretics. However, the use of mercury in cosmetics was banned in 1970 and the importance of mercury in medicine has steadily diminished due to the advent of safer non-mercurial medicinal products in the market. A mercury preservative, thimerosal, is still used in cosmetics and pharmaceuticals (vaccines). In 1999, the Food and Drug Administration reported an estimated use of mercury in human and veterinary drug products was 75-80 kg for the entire U.S. The data source is BOM. The peak use of mercury in pharmaceuticals was in the mid-1940s, ranging about 300-500 Mg/yr. After the 1940s the use of mercury declined, and mercury was last reported used in 1976 as 2 Mg/yr. The cumulative use of mercury by pharmaceutical sector for 1930-2000 was estimated to be about 3,400 Mg, and it was generally in a range of 100-200 Mg/yr per year. Mercury in pharmaceuticals followed the general pathways for consumer products to municipal solid waste and wastewater (Barr, 2001) Dental Sector This category includes mercury used in dental preparations and the historical data are available from BOM. The use of mercury in the dental sector increased steadily since 1930 from about 20 Mg/yr to its peak of 103 Mg/yr in1974. Since 1974 the use of mercury in dental preparations has declined. The cumulative use of mercury in dental sector for 1930-2000 was estimated to be about 3,200 Mg. Mercury in dental sector is disposed to air (dentist office, crematoriums), water (discharge from dental offices) and solid waste (amalgam waste) (Barr, 2001). The distribution to the environmental compartments (air, water, soil) and “storage”/delay times were not estimated. 24 Chlorine and Caustic Soda Manufacturing According to the BOM data chlorine and caustic soda manufacturing was a significant consumer of mercury. Mercury is used in the industrial process of chlorine and caustic soda manufacturing. However, the products do not contain mercury. Hence, the flow of mercury to the environment is restricted to the vicinity of the chlorine and caustic soda plants. Since our focus was Florida, and there are no chlorine and caustic soda manufacturing plants, the impact of this category was not investigated. In the time period 1930-2000 14,000 Mg was used by the industry. Other Category The “Other” category was used by BOM to allocate mercury uses that did not belong to the above eight categories. Bureau of Mines Yearbook Mercury Chapter (consumption and uses), reports that in 1939 about 45 Mg mercury will be used for a single G. E. boiler. Mercury used for boilers in the 1930s was recycled, BOM reported. In subsequent BOM Yearbooks, other uses were mentioned, vermilion pigment, felt manufacturing, military uses, fulminate, etc. In 1978, mercury used for installation and expansion of chlorine and caustic soda plants was included in the “Other” category. Military uses were not disclosed, but it is implied that mercury was used in detonators. To re-construct the “Other” category was beyond the scope of this project. For this category we have used data as supplied by BOM. The cumulative use of mercury in other sector for 1930-2000 was estimated to be about 30,500 Mg. Out of 30,550 for the19302000 period only about 1,800 Mg/yr was reported for the 1980-2000 period. 25 Summary: US Mercury Flow in Fuels and Goods The mercury mobilization through human activities shows a dynamic history during the 19302000 period. Figure 24 shows the overall mercury mobilization in the US during the 1930-2000 period. It includes the flow through goods as well as fuels. The large scale industrial consumption began at the turn of the century. In the 1930-1970 the consumption of mercury in consumer goods was increasing. However, the industry uses were not well documented or disclosed. In 1940, 74% of mercury consumption was categorized as "Other" category. Since 1970, the use of mercury in consumer goods was disclosed and accounted more precisely, and the "Other” category represented <10%. In the period of 1970-1990 electrical sector (batteries, switches, and lighting) was the dominant mercury industrial consumer. The drastic reduction in mercury demand for consumer goods occurred since 1989. Mercury consumption in consumer/industrial goods was reduced from around 1,500 Mg/yr in 1989 to about 346 Mg/yr in 1997. Mercury mobilization in coal has increased since the turn of the century. However, the coal contribution in the 1940s to the overall mercury input into the system was <6% (Figure 24). By 1995, mercury mobilization by coal contributed about 20% (Figure 24, Appendix Table 12). Mercury mobilization by crude oil increased since 1940. Crude oil contribution is still uncertain, lacking reliable data on the mercury content in crude oil, and information on fate of mercury in extraction process, shipping, refining, and ultimately concentration of mercury in petroleum products consumed. Nevertheless, the available scant data indicate that oil products contribute <1 % to mercury flow. Figure 24. Trend of US mercury mobilization in industrial/consumer goods and fuels. The long term trend data arise form the current “production driven” estimates. This method relies on the mercury concentration of coals as measured at various coal beds and subsequently shipped to the coal consumers. The mercury content of coal as-mined (Table 1) has a large variability within a given region (see Figure 28). As depicted in Figure 28, the median mercury concentration for different states in the Appalachian region can vary between about 0.1 ppm and 26 0.2 ppm. A detailed analysis of coal production within a region was not attempted, and neither the COALQUAL database was analyzed for every state. The next process that reduces mercury in coal is coal cleaning at mines. Eastern coals are generally washed and cleaned before shipment. EPA, 1997 estimated an average of 21% removal of mercury for eastern (Appalachian coal). Historical reconstruction of level of coal cleaning was not attempted. In 1999, the estimate for mercury delivered in coal to electric utilities using our materials flow method was 102 Mg/yr (21% cleaning, 90% power plant consumption). According to Chu, 2000 an average of 40% of mercury is removed at power plants by various pollution control devices. If we apply the above emission factor to cleaned coal than the emissions estimate from the mass flow method is 61 Mg/yr. In the reports by EPA, 2000 and Chu, 2000 the coal mercury emissions of point sources (electric utilities) were estimated from mercury content of coal as-received or as-fired based on the Information Collection Request (ICR) database. EPA, 2000 estimated that for 1999, 75 Mg/yr mercury was delivered in coal to the power plants. Out of that, 45 Mg/yr mercury was emitted to the atmosphere by the power plants. Based on the EPRI model, 68 Mg/yr was delivered in coal and 41 Mg/yr emitted to the atmosphere. These ICR arrived US coal emission estimates of point sources (41-45Mg/yr) are below the mass flow emissions estimates of 61 Mg/yr, but are still within the range. To assemble the US emission trends, assumption were used are as follows: for coal an average of 50% emissions factor was used and for crude oil concentration of 10 ppb. For paint emission at 66% in the first year after application was assumed. For electrical, laboratory use, and control category it was assumed that 30% was incinerated for 1930-1960. For the period 1960-2000, Franklin and Associates, 1998 combustion factors were used (Figure 25). Based on the above assumption a tentative atmospheric emission trend is presented in Figure 26. The largest contribution in the 1970-1990 period was mercury emissions associated with waterbased paint applications and electrical (battery) devices. Coal contribution in the 1990s has increased compared to other categories. In fact, by the 1990s, coal combustion became the dominant mercury emission category. Figure 25. US muncipal solid waste combustion ratio (Franklin and Associates, 1998). 27 Figure 26. Trend of estimated US mercury emissions to the atmosphere. 28 Trend of anthropogenic mercury in Florida This section describes the reconstruction of mercury trends in Florida for the period 1930-2000. The reconstruction was conducted on two scales, first at the state level followed by a more detailed reconstruction for southern Florida. The methodology included Florida specific accounting for mercury in fuels and in agriculture. For the remaining categories of mercury flow the state of Florida and county specific flows were estimated by prorating national averages by population. This section contains both estimates of overall anthropogenically induced mercury flow, as well as estimates of mercury emissions to the atmosphere. The trend of anthropogenic mercury flow in fuels was assembled using coal and petroleum consumption data for Florida. The mercury flow through the electric, laboratory use, control and dental sectors was apportioned by Florida population. Agriculture sector was apportioned by acreage used in vegetable production and golf course statistics. Chlorine and acoustic soda manufacturing use of mercury was omitted from Florida trends, since the manufacturing was done outside Florida and the products do not contain mercury. The “Other” category was also omitted in Florida trend reconstruction (see description of “Other” category in the US section). Florida Mercury Flow in Fuels Coal The mercury flow through coal was reconstructed from data on coal consumption, coal mercury content and Hg retention factors. Since 1960, the coal consumption data for each state are available (U.S. DOE, 1999) in the electronic form. Prior to 1957, state-by-state coal consumption data were available only for 1889, 1917, 1927 and 1945. These years were used as anchor years and Florida data were interpolated using national coal consumption data (Husar, 1986). The yearly coal consumption data in Florida are given in Appendix, Table 13. Coal shipments for Florida and their origin were available for 1985 (DOE/EIA, 1985) and 1998 (DOE/EIA, 1998). In 1985, the coal consumed in Florida was mainly from Eastern Kentucky (~50%), Western Kentucky and Illinois (~25%, each). In 1998, the coal consumed in Florida was more diverse. Still, about 50% coal originated from Eastern Kentucky and about 25% originated from Illinois. The remaining coal originated from West Virginia, Western Kentucky, Wyoming, Virginia, Tennessee, Indiana, Pennsylvania, and Alabama in decreasing order of shipments (Figure 27). Figure 27. Coal distribution by origin in 1985 and 1998 in Florida. 29 Mercury content of coal as-mined for states supplying coal for Florida was estimated from the USGS COALQUAL database (Finkelman et al., 1994). Each coal-mining region is characterized by a well-defined distribution of coal mercury content, as depicted in Figures 28 and 29. The normalized cumulative frequency distributions show that the mercury concentrations are roughly lognormal with a rather broad logarithmic standard deviations σg in the range 2-3. Furthermore, the median values are clustered by region. The highest median of 0.20-0.25 ppm was observed for Pennsylvania, Ohio and Alabama, while the other regions were in the 0.05-0.15 ppm median range. Figures 28 and 29 also delineated the 16th and 84th percentile values, corresponding to median±σg. The range between the two sigma values represent the possible values for the coal mercury content of coal mined in each region. Figure 28. Mercury distribution in Appalachian coal, COALQUAL database (Finkelman et al., 1994). Figure 29. Mercury distribution in Interior and Western coal, COALQUAL database (Finkelman et al., 1994) The weighted average Florida coal mercury content was calculated for 1998, as 0.05 ppm for the 16th percentile, 0.23 ppm for the 84th percentile, 0.11 ppm for the median and 0.14 ppm for the mean (Figure 30). Based on Florida coal consumption, coal origin, and associated coal content (16th, 84th, median and mean) the range of mercury mobilized was calculated (Figure 31). The amount of mercury in coal mobilized for use in Florida in 1999, was 5.7, 3.5, 2.7, and 1.2 Mg/yr for the 84th percentile, mean, medium, and 16th percentile, respectively. 30 Figure 30. Mercury in coal as-mined by origin. USGS COALQUAL data base (Finkelman et al., 1994) for coals consumed in Florida. Figure 31. Mercury mobilized in coal used in Florida, based on coal origin and coal content in coal as-mined (Appendix Table 14). Eastern coals are generally washed and cleaned before shipment, EPA, 1997. An average of 21% removal of mercury from coal was assumed for the coals shipped to Florida. Thus, a fraction of as-mined mercury is retained in the vicinity of the mines due to coal washing. Figure 32 depicts the estimated mercury in coal-as shipped (as-fired) in Florida. The mercury content of coals consumed in Florida, as depicted in Figure 32 shows the result of two independent estimates. The long term trend data arise form the current “production driven” estimates. This method relies on the mercury concentration of coals as measured at various coal beds and subsequently cleaned and shipped to Florida. The second coal mercury estimate is the Information Collection Request (ICR) that is based on mercury measurements in coal that is received at the electric utilities in Florida (accounting to 97% of total coal consumed in Florida in 1999). In 1999, the median and mean estimates from the materials flow method were 2.3 31 Mg/yr and 2.9 Mg/yr, respectively. For the same year, the ICR estimate was 2.0 Mg/yr (Chu, 2000). Evidently, the ICR estimate is somewhat below the mean and median but it is well within the range of the possible coal mercury in coal as-fired. In fact, the correspondence between the two independently measured estimates is considered to be excellent. Figure 32. Mercury in coal used in Florida, based on coal origin and coal content in coal as-mined (Figure 30) and estimated 21% removal of mercury by coal washing and cleaning at mines (Appendix Table 15). Based on Figure 31, and on median and mean mercury content, cumulatively from 1930-2000, about 62-79 Mg mercury was mined in coal that was used in Florida. Based on Figure 32, and on median (0.11 ppm) and mean (0.14 ppm) mercury content, and 21% mercury removal at mines, about 49-63 Mg mercury was delivered with cleaned coal to Florida and combusted. 32 Petroleum Mercury in petroleum was reconstructed using Florida consumption data (U.S. DOE, 1999; Appendix Table 13) for petroleum products and mercury content of each product (Wilhelm, 2001), (Table 2). The resulting mercury flow trend is shown in Figure 33, Appendix Table 16. Residual fuel and motor gasoline are the key mercury containing petroleum products throughout the 1930-2000 period. Note, that the overall contribution of petroleum mercury is very low, more than 200 kg/yr for Florida, factor of ten lower than coal. Over the 70 years (1930-2000) only about 7 Mg of mercury was distributed over Florida with the petroleum products. Figure 33. Florida mercury flow trend in petroleum products (appendix Table 16). Florida Mercury Flow in Products Electrical Sector The electrical sector is one of the most important consumer of mercury in products. In this report we have used the U.S. Bureau of Mines (BOM) data for the electrical sector. There is a consistent BOM record on mercury use in goods available since the 1930s, with the caveat, that the results are the upper limit of mercury flow. Mercury consumption in electrical sector is prorated from the national to Florida values by the population ratio. Batteries were the dominant mercury carrying products. The maximum contribution of mercury in the 1980s was in the range of 50 Mg/yr (Figure 34, Appendix Table 19). For the 1930-2000 time period 1,050 Mg mercury was mobilized in Florida with electrical products. 33 Figure 34. Florida mercury flow in electrical devices. Paint Sector The paint mercury estimate for Florida is based on U.S. Bureau of Mines mercury use data in paint industry and Florida population data (Figure 35, Appendix Table 19). In the 1940s mercuric oxide was added to ship paints as antifouling additive. In the 1950s the main mercury use in paints was as fungicide and bactericide. By the 1990s, mercury was eliminated from newly manufactured water-based paints. For the 1930-2000 time period about 300 Mg mercury was mobilized with paint products in Florida. Figure 35. Florida mercury flow in paints. Agriculture Sector The production of wheat, barley, oats, rye and apples is not significant in Florida. Thus, only the vegetable mercury use was prorated to Florida, using vegetable acreage of Florida compared to USA vegetable acreage. About 56 Mg mercury was used for agricultural applications in Florida for the period 1930-2000. The golf course mercury fungicide was estimated using Florida golf course statistics (Bureau of Census, annual 1959-2000). In 70 years it was estimated that 31 Mg was applied to golf courses. The increase in mercury use for golf courses in the 1970s is driven by increase of number of golf courses in Florida. Newer information on the use of mercury products in turf management was 34 not available. The overall trend of agricultural mercury use (Figure 36, Appendix Table 17) shows rather low (~2 Mg/yr) but fluctuating between 1 and 8 Mg/yr. Figure 36. It is estimated that the mercury use for golf turf maintenance was increasing. For other agricultural uses of mercury, it could be assumed that about 2 Mg/yr was used in the 1950s and about 1 Mg/yr in the 1960s. Data are subject to change as better information is obtained. Measurement and Control Device, Laboratory, Pharmaceutical and Dental Sector The mercury use in pharmaceutical, control (manometers, barometers, thermostats, and thermometers) and dental categories were prorated from the national estimates to Florida by population. Chlorine and Caustic Soda Manufacturing and Other Sector Chlorine and caustic sod manufacturing sector was not included in Florida. The manufacturing was done outside Florida and products do not contain mercury. The Other sector was not included in Florida. (See US Other section). 35 Summary: Florida Mercury Flow The overall mercury mobilization in Florida during the 1930-2000 period is shown in Figure 37. It includes the flow through goods as well as fuels. Since the 1940s, there was a steady increase of mercury flow reaching about 70 Mg/yr in the 1980s. The electrical and paint sectors were the most dominant contributors, reaching about 60 Mg and about 10 Mg/yr, respectively. Figure 37. Trend of anthropogenic mercury flow in Florida (Appendix Table 18). The cumulative flow (1930-2000) of mercury in Florida is shown in Table 4 and Figure 38. Of the total of 2,073 Mg mobilized, two thirds is attributed to electrical and control devices. Table 4. Cumulative mercury mobilization, Mg, 1930-2000. US Florida Coal Petroleum Pharmac Agriculture Paint Lab use Electrical Control Dental Chlor-alkali 7,000 325 3,400 5,400 9,000 1,800 29,000 10,000 3,200 62* 7 72 87 306 56 1,051 298 116 14,000 Other Total 31,000 114,125 2,055 *Florida coal Hg concentration of 0.11ppm (median) from USGS, COALQUAL. Figure 38. Cumulative mercury mobilization in Florida, 1930-2000. 36 Summary: Florida Mercury Emissions Florida coal consumption has tripled since the early 1980s. Electric utilities were the dominant coal consumers. In 1999, 97% of coal shipped to Florida was combusted in power plants (Figure 39). Only a fraction of the mobilized coal mercury is emitted to the atmosphere (Chu and Porcella, 1995; Pirrone et al., 1998). The average (0.21%) of the eastern US coal is cleaned (Figure 32) at mines (EPA, 1997). According to Chu, 2000 in Florida, efficiency for mercury removal in power plants was 57% in 1999. Based on the removal efficiency at power plants in 1999, the mercury emission trend from coal combustion was reconstructed for Florida (Figure 40). The amount of mercury emitted in Florida by coal combustion in 1999, was 1.93, 1.18, 0.93, and 0.42 Mg/yr for the coal mercury content of 84th percentile, mean, medium, and 16th percentile, respectively. The mercury coal emissions in Florida, as depicted in Figure 40 show the result of two independent estimates. The long term trend data arise form the current “production driven” estimates. This method relies on the mercury concentration of coals as measured at various coal beds and subsequently cleaned and shipped to Florida. The second coal mercury flow Information Collection Request (ICR) is based on mercury measurements emissions at power plants in Florida. In 1999, the median and mean emission estimates from the materials flow method were 0.93 Mg/yr and 1.18 Mg/yr, respectively. For the same year, the ICR estimate was 0.86 Mg/yr and the EPA estimate was 0.87 Mg/yr. Evidently, the ICR estimate are somewhat below the mean and median but it is well within the range of the possible coal mercury emissions. In fact, the correspondence between the two independently measured estimates is considered to be excellent. Figure 39. More than 97% (1999) of coal consumed in Florida is by electric utilities (EIA and FERC) 37 Figure 40. Mercury emissions of coal used in Florida, based on coal origin and coal content in coal as-mined (Figure 30) and estimated 21% removal of mercury by coal washing and cleaning at mines, and estimated 57% removal efficiency at power plants in Florida (Chu, 2000). Estimated ICR power plant mercury emissions in Florida for 1999 were 0.86 Mg/yr (Chu, 2000) and 0.87 Mg/yr EPA, 2000. The trend for estimated Florida coal mercury emissions is depicted in Figure 40 and Appendix Table 19. Mercury emissions exhibit a slow increase between 1960 and 1980, followed by a sharp increase between 1980 and 1990, and leveling off in the early 1990s. Based on Figure 40, and on median (0.11 ppm) and mean (0.14 ppm) mercury content, 21% mercury removal by coal cleaning at mines (EPA, 1997) and 57% mercury removal by controls at power plants in Florida, about 49-63 Mg mercury was emitted in Florida in the past 70 years. The mercury emission in Florida was calculated by assigning an air emissions fraction to each category. Coal emissions were taken as described above using median mercury content in coal (Figure 40). Petroleum emissions were taken as in Figure 33. For the paints it was assumed that 75% of mercury is emitted to the atmosphere in the first year after application (Barr Engineering, 2001). Laboratory, electrical, and control products were assumed to be disposed to the municipal solid waste (MSW) with a portion of the MSW incinerated. Prior to 1980, there were several options to control MSW. Open burning of waste was a common method to save landfill space (FL DEP, 1996). Also there were municipal incinerators. For southern Florida counties Broward and Dade, municipal incineration capacity (KBN,1992; RMB, 1998) is given in Figure 47 and 48. Prior to 1995, most of the hospitals and research facilities incinerated their own waste as well. In 1992, for instance in Dade and Broward counties there were 33 hospital incinerators (KBN, 1992; RMB, 1998), with more than 50,000 t/yr waste incinerated. In 1999, there were only two commercial incineration facilities in southern Florida. Mercury emissions from medical incineration were not explicitly considered in this report. For 1990-1998 the percentage of municipal waste burned in Waste to Energy (WTE) plants was available from Florida DEP, yearly (Figure 41). In 1990, the Florida waste combustion ratio and US combustion ratio were both 0.16 (Franklin and Associates, 1998). In absence of historical data on incineration in Florida, we have assumed the US combustion ratios prior to 1990. 38 Figure 41. Ratio of US (Franklin and Assoc., 1998) and Florida combustion ratios for solid waste (Florida DEP, yealy) The overall emission trend in Florida is shown in Figure 41 and Figure 42. Based on these estimates from 1960-1990, the paint sector was the main contributor to atmospheric emissions. Electrical contributions were dominant in the 1980s. Coal emission contribution became dominant fraction in the late 1990s (Figure 42) due to the rapid decline in paint and electrical emissions. Figure 42. Trend of anthropogenic mercury atmospheric emissions in Florida 1930-2000. 39 Figure 43. Estimated trend of anthropogenic mercury air emissions in Florida 1990-2000. Comparison of municipal waste incineration emissions. The above estimated electrical, control, and laboratory use emissions as shown in Figure 43, were compared to the Florida DEP, 2000 estimated mercury emissions from WTE facilities. Figure 44, showing a satisfactory match for 1994-1997, and almost a factor of two difference in 1991 and 1993. Figure 44. Comparison of Florida mercury emissions trend from municipal waste combustion (FL DEP, 1999) and from this study. 40 Trend of anthropogenic mercury in Southern Florida Mercury Flow Methodology Southern Florida is defined here as 24 counties as given in Figure 45. For the presentation of some of the results, the southern Florida domain was further aggregated as West Coast, East Coast, and Interior. Figure 45. Delineation of southern Florida and population. The southern Florida coal mercury flow estimates were obtained county by county using the Florida coal utility plant by plant consumption for the period 1972-1999 (FERC, yearly) and population adjusted Florida coal consumption for the period 1930-1972. The mercury flow from coal was calculated directly from coal consumption data from individual electric utility plants and subsequently aggregated for specific counties. The Florida coal consumption by utilities increased from around 1 million short tons/yr in 1960 to about 29 million short tons/yr in 1998. As depicted in Figure 39, coal consumption by utilities dominated Florida coal consumption (>97%) (U.S. DOE Energy Information Administration, 1999). In the 24 counties of southern Florida only three utility plants consume coal and all three are located in the Tampa Bay area (Big Bend, Gannon and Polk). The coal consumption trend of these three utilities is also given in Figure 39. Petroleum consumption was population adjusted for each county based on Florida consumption. The petroleum mercury flow factor (kg Hg/person,year) was calculated by dividing the Florida mercury petroleum flow (Figure 33) by Florida population. The calculated petroleum factor ranged between 0.4*10-5 kgHg/person,yr for the 1930s, peaking at 2.2*10-5 kgHg/person,yr in 1979 and declining to 1.5*10-5 kgHg/person,yr, in 1999. Clearly, the petroleum flow factor is two orders of magnitude lower than the per capita flow factor in goods. The per capita mercury flow factors (kgHg/person,year) for goods consumed in Florida were calculated based on Florida mercury flow data and Florida population. The mercury flow factor 41 was calculated by dividing the Florida mercury flow in the different categories, electrical, control laboratory use and dental, paints pharmaceutical, and agriculture by the Florida population. The resulting per capita flow factors are shown in Figure 46. These factors were used in calculating mercury flows in specific counties. Figure 46. Florida mercury flow factors per person per year. The largest mercury flow factor was for the electrical category up to 5*10-3 kgHg/person,yr, driven primarily by battery consumption. Following an early peak in the 1940s there was a continuous rise to the 1980s, followed by a dramatic decline. By the late 1990s the mercury factors for electrical products were minimal. Evidently, the trend of mercury in electrical devices was the main contributor to the overall trend of mercury flow in Florida. The agricultural mercury flow factor was calculated by dividing the Florida agricultural mercury flow by population (Figure 46). The uncertainties of mercury use on farmland and on the golf courses is not well documented and greatly variable from year to year, crop to crop, from farm to farm, and golf course to golf course. Therefore, the estimation of the spatially resolved agricultural mercury flow is rather uncertain. Lacking a more suitable approach, the agricultural mercury flow was also allocated according to the population. 42 County by County Mercury Flow The mercury flow for each county in southern Florida was reconstructed using the mercury flow factors as given in Figure 46 and the county population data. The resulting flow estimates for the Broward and Hillsborough counties the data are also presented in Figures 47 and 48. In Broward County (Figure 47), the mercury highest flow was the about 7 Mg Hg/yr in the1980s with the electrical and paint sector contributing the most. For the Hillsborough County, (Figure 48) the levels in the 1980s were <5 Mg Hg/yr. The relative contribution of coal to the overall flow of mercury in the Hillsborough County has increased in the 1990’s. Figure 47. Broward County mercury flow. Figure 48. Hillsborough county mercury flow. The county-by-county mercury flow data for southern Florida were further aggregated into three regions, West Coast, East Coast and Interior. The mercury flow for each region is shown in Figure 49 for years 1980, 1990, and 1999. The mercury flow trend in each region is shown in Figure 50. Evidently, the East and West Coast of southern Florida dominate the mercury flow. The mercury flow for the Interior counties is an order of magnitude lower than the East or West Coast. 43 Figure 49. Mercury flow for the West Coast, East Coast and Interior for 1980, 1990 and 1997. Figure 50. Trend of mercury flow for the southern Florida West and East Coast, and Interior. 44 Mercury Emissions for the Broward, Dade and Palm Beach Counties Methodology In this section we describe our estimates of atmospheric mercury emissions for Dade, Broward and Palm Beach Counties in southern Florida The mercury flow-based emission estimates are also compared to preliminary results of RMB Consulting, 2002. The estimates for coal contribution for the above three counties were assumed to be negligent, and were not included. Petroleum county emissions were assumed the same as in flow estimates. For mercury in products categories (electrical, controls, laboratory), it was assumed that they are disposed as the solid municipal waste. The amount of solid waste per county was available from 1990 to 1998 (Florida DEP, yearly). However, historical MSW amounts were not available. Based on the US (tons per person per year) levels, the Dade, Broward and Palm Beach counties MSW was estimated for 1930-1990. (Figure 51, 52, 53). The next key parameter in estimating emissions was the fraction of waste burned in each county and year. For 1990 –1998, these values were obtained from the Florida DEP reports for Dade, Broward and Palm Beach counties. The historical values of combusted fraction were assumed in the range of 10-30 % (Figure 41). Figure 51. Estimated MSW, tons/person/year Figure 52. Combustion fraction in Dade county. 45 Figure 53. Combustion fraction in Broward county. Figure 54. Combustion fraction in Dade county. For paint it was assumed that 75% of the mercury in the consumed paint was released to the atmosphere in the first year. Pharmaceutical and dental categories were assumed incinerated at national level 1930-1990, and for the 1990s the specific county level of incineration was applied. Agricultural sector was not considered in estimating the atmospheric emissions of mercury. 46 County Mercury Emissions The resulting mercury emission trends for the Broward County is given in Figure 55. The most notable features are the dominance of paint and electrical mercury sources as well as the sharp drop in emissions in the late 1980s. This last step in our analysis, i.e. estimating the county atmospheric emissions from the mercury flow data is judged to be the most uncertain part of the entire analysis. Figure 55. Estimated atmospheric emission trend for the Broward County. 47 Preliminary comparison of mercury emission estimates by RMB Consulting and this mercury flow study Using our assumption that electrical, control and laboratory use category will end up in the MSW we have applied the methodology as described in the previous section for the Broward, Dade and Palm Beach counties. The sum of emissions in those counties is depicted in Figure 56. Figure 56. Comparison of waste incineration emissions for Broward, Dade, and Palm Beach counties. The total mercury flow from electrical, laboratory use, control categories is depicted as a solid line ranging from about 18,000 kg/yr in the 1980s and decreasing to <2000 kg/yr in 1997 (Figure 56). A somewhat uncertain fraction of this flow is emitted to the atmosphere. For comparison the atmospheric emission estimates by RMB Consulting, 2002 are also presented in Figure 56. MSW_R represents the municipal solid waste incineration while MSW_R + MWI_R is the sum including medical waste incineration. According to the RMB estimates the emissions have steadily increased in the 1980s driven by both MSW and MWI. Around 1992 the RMB estimates show a sharp drop which continued until 2000. A comparison of mercury flow trends (electrical, lab, control) with the RMB estimate shows that the RMB emission estimates are well below the overall mercury flow, ranging between 10-50%. This is expected, since only a fraction of the mercury in goods is emitted in major point sources. The shaded area in Figure 56 represents a crude emission estimate based on the mercury flow data assuming that 10%-30% of mercury in goods (electrical+control+lab use) is incinerated. 48 References Barr Engineering Co, Substance Flow Analysis of Mercury in Products, Report to Minnesota Pollution Control Agency, 8/15/2001. Benazon Environmental, Inc Historical Mercury Consumption and Release Estimates for the Province of Ontario, April, 1998. CDC, 1990. (http://www.cdc.gov/mmwr/preview/mmwrhtml/0001566htm) Chu, P. and Porcella, D. B. (1995) Mercury stack emissions from US electric power plants, in Porcella, D.B. Huckabee, J.W. and Wheatley, B. (eds.) Mercury as a Global Pollutant, Water, Air and Soil Pollution, 80, 134-144. FL DEP (yearly) Florida Department of Environmental Protection, Division of Waste and Management, Solid Waste Management in Florida, yearly, 1990-2000, FL DEP (1996) Florida Department of Environmental Protection, Division of Waste and Management, Solid Waste Management in Florida, p 63. FL DEP (1999), worksheet, personal communication. FERC (yearly) Federal Energy Regulatory Commission, Form 423: Monthly Report of Cost and Quality of Fuels for Electric Plants. Annual historical data since 1972, http://www.ferc.gov/electric/f423/F423annual.htm. Engstrom, D. and Swain, .E., (1997) Recent declines in atmospheric mercury deposition in the upper Midwest, Environ. Sci and Techn., 31, 960-967. Franklin Associates Ltd. (1998) Characterization of Municipal Solid Waste in the United States: 1997 update, U.S. EPA, Municipal and Industrial Solid Waste Division, Office of Solid Waste, Report # EPA530-R-98-007, (http://www.epa.gov/epaoswer/nonhw/muncpl/mswrpt97/msw97re.pdf) Jasinski, S. M. The Materials Flow of Mercury in the United States, Bureau of Mines Information Circular , IC 9412, 1994. Federal Energy Regulatory Commission, www.ferc.gov/electric/f423/F423annual.htm. Finkelman, R. B., Oman, C. L. Bragg, L. J. and Tewalt, S. J. (1994) The U.S. Geological Survey Coal Quality Data Base. Open-File Report 94-177,) (http://energy.er.usgs.gov/products/databases/CoalQual/Docs/Of94-177.pdf). Finkelman, R.B. And Tewalt, S. J. (1998) Mercury in U.S. coal, U.S.G.S. Open-File Report 980772 (http://energy.er.usgs.gov/products/openfile/OFR98-0772/index.htm)). Husar, R. B. (1986) Manmade SOx Emission Trends for the United States, Report to E. Pechan & Associates. Husar, R.B. and Husar, J.D. (1990) Sulfur. In The Earth as Transformed by Human Action (edited by Turner B.L., et al.) Cambridge University Press with Clark University, Cambridge. Jasinski, S. M. (1994) The materials flow of mercury in the United States, Bureau of Mines Information Circular 9412, http://geology.cr.usgs.gov/pub/circulars/c9412/index.html. Kelly, W. R. and Long, S. E. (2001) An estimate fo mercury emissions to the atmopshere from petroleum refining, submitted to Environ, Sci. & Tech., 2001. 49 Liang, L., Horvat, M., and Danilchik (1996) A novel analytical method for determination of picogram levels of total mercury in gasoline and other petroleum related products, Sci. Tot. Environ., 187, 57- 64. Liang, L., Lazoff, S,. Gilkeson J., Swain E., Horvat M. (1999) A simple combustion method for determination of total mercury (THg) in crude oil and related products, In Mercury as Global Pollutant-5th International Conference , May 23-28, Rio de Janeiro, Brazil. Metcalf, R. L. (1955) Organic Insecticides: their Chemistry and Mode of Action, Interscience Publishers, New York. Murphy, E. and Aucott, M. (1999) A Methodology to Assess the Amounts of Pesticidal Mercury Used Historically in New Jersey, Journal of Soil Contamination, 8, 131-14. Milici, R. C. (1997) Coal-producing regions of the conterminous United States, compiled by Robert C. Milici, U.S.G.S. Open-File Report 97-447 (http://energy.er.usgs.gov/products/openfile/OFR97-447/index.htm). Minnesota Pollution Control Agency (1999), Options and Strategies for Reducing Mercury Releases, Source Reduction Feasibility and Reduction Strategies Committee Report, http://www.pca.state.mn.us/hot/legislature/reports/1999/mercury.pdf NEMA, National Electrical Manufacturers Association (1996) The declining presence of mercury in batteries and municipal solid waste, NEMA 1300 North 17th Ave., Rosslyn, VA 22209. Pirrrone, N., Allegrini, I., Keeler, G. J. Nriagu, J. O., Rossman, R., and Robbins, J. A. (1998) Historical atmospheric mercury emissions and depositions in North America compared to mercury accumulations in sedimentary records, Atmos. Environ., 32, 929-940. RMB Consulting & Research Inc. (2002) Atmospheric mercury emissions from major point sources Brtoward, Dade, and Palm Counties, Report prepared by RMB Consulting &Reaserch, Inc, 5104 Bur Oak Circle, Raleigh, NC 27612. Ross John M. (ed) Encyclopedia of Golf, Harper &Row, New York, 1979. http://www.ngf.org/faq/growthofgolf.html Scharff, R. (ed) Encyclopedia of Golf, Harper &Row, New York, 1970. Sharvelle, E. The Nature and Uses of Modern Fungicides, Burgess Publishing Company, Minneapolis, 1961. Sznopek, J.L. and Goonan, T. G. (2000) The materials flow of mercury in the economies of the United States and world, USGS Survey Circular 1197 http://geology.cr.usgs.gov/pub/circulars/c1197/index.html. Taylor, C. G. and Tickle, W (1969) Radiometric studies of mercury loss from fungicidal paints I, J. Appl. Chem. (London), 19, 1-7 Taylor, C. G., Tickle, W. and Dwyer, A. (1969) Radiometric studies of mercury loss from fungicidal paints II, J. Appl. Chem. (London), 19, 8-11. Taylor, C. G. and Hunter, G. H. (1972) Radiometric studies of mercury loss from fungicidal paints III, J. Appl. Chem. Biotechnol. (London), 22, 711-718. Toole-O’Neil, B., Tewalt, S. J., Finkelman, R. B. and Akers, D. J. (1999) Mercury concentration in coal-unraveling the puzzle, Fuel, 78, 47-54. 50 U.S. Bureau of Mines (a), US Department of Interior, Minerals Yearbooks 1937-1997, Mineral commodity summaries, Mercury, pages vary. U.S. Bureau of Mines (b), US Department of Interior, Minerals Yearbooks 1937-1997, Fuels. U.S. Bureau of Census (a) Current Industrial Reports, Manufacturing Profiles (MA36L), electric lighting fixtures. U.S. Bureau of Census (b) http://www.census.gov/prod/2manmin/mp94.pdf U.S. Bureau of Census (b), Current Industrial Reports, Manufacturing Profiles (MA28F), paint, varnishes and lacquer;http://www.census.gov/prod/2001pubs/mp98.pdf or http://www.census.gov/ftp/pub/industry/1/ma28f99.pdf U.S. Bureau of Census Historical Statistics of the United States, Colonial Times to 1970, Bicentennial Edition, Washington, DC 1975. U. S. Bureau of the Census County Business Patterns, Florida, GPO annual, 1959-2000 U. S. Bureau of the Census (http://www.census.gov/prod/ec97/97numlist/325.pdf) U.S. DOE (a) Energy Information Administration, Annual Energy Review, http://www.eia.doe.gov/emeu/aer/petro.html. U.S. DOE Energy Information Administration (2000) Petroleum Supply Annual 2000, Volume 1. U.S. DOE Energy Information Administration (1985). Coal Distribution, January-December, 1985. U.S. Department of Energy, Washington D.C. DOE/EIA-0125 (85/4Q). U.S. DOE Energy Information Administration (1999) State Energy Data Report, http://www.eia.doe.gov/emeu/sedr/contents.html#PDF Files, (ftp://ftp.eia.doe.gov/pub/state.data/data/). U.S. DOE Energy Information Administration (1998) (http://www.eia.doe.gov/cneaf/coal/cia/html/t64p01p5.htm) U.S. EPA (1997), Mercury Study Report to Congress, Volume II An inventory of anthropogenic mercury emissions in the United States, EPA-452/R-97-004. OAQPS and ORD. Wilhelm, S. M. (2001) Estimate of mercury emissions to the atmosphere from petroleum, Environ, Sci. & Tech., 35, 4704-4710. 51 Appendix Table 1. USA coal production by region 1930-2000 in million Mg/yr (http://energy.er.usgs.gov/products/openfile/OFR97-447/index.htm). YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Appalachian 373 308 246 267 291 291 341 343 269 307 359 400 446 442 459 421 409 482 457 332 387 403 352 338 288 339 370 362 294 293 291 279 293 319 337 351 359 368 363 367 388 345 357 346 348 366 374 361 338 386 404 392 396 348 403 389 388 401 406 420 442 414 413 371 404 395 430 440 444 446 461 Eastern Interior 73 61 51 54 58 63 70 71 58 65 71 80 94 103 114 108 94 105 102 81 92 86 75 75 71 80 86 85 79 82 83 83 87 93 98 103 112 118 115 120 127 116 130 127 121 127 124 121 102 118 122 110 119 113 130 119 123 126 118 122 128 121 120 97 110 99 117 120 121 122 126 Gulf Coast 1 1 1 1 1 1 1 1 1 1 1 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 4 6 7 10 13 14 18 25 27 30 32 35 37 41 46 48 50 52 53 52 53 52 51 51 59 60 60 61 63 Rocky Mountain 21 17 15 14 14 16 19 20 16 17 18 20 25 28 29 27 22 24 21 19 19 18 17 16 11 13 12 12 9 9 10 11 10 12 14 15 15 15 16 18 26 31 37 45 58 70 86 105 118 147 169 182 185 183 206 214 212 220 246 256 271 278 278 300 335 357 352 360 363 365 378 Great Plains 2 1 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 3 3 3 3 3 3 3 3 3 3 2 2 2 2 2 2 2 2 2 3 4 4 4 5 6 6 6 7 8 10 11 13 14 15 16 16 17 20 24 23 23 27 27 27 27 29 29 29 27 31 32 32 32 34 US 470 388 313 337 366 372 432 436 346 392 451 503 567 575 603 559 528 614 582 435 500 510 447 432 372 435 471 461 385 386 387 375 392 427 451 472 489 505 498 510 546 497 534 531 541 581 606 613 588 688 736 730 748 696 797 788 792 818 847 877 921 892 893 848 929 929 989 1,012 1,020 1,027 1,061 53 Table 2. USA petroleum consumption 1930-2000 in million Mg/yr (ftp://ftp.eia.doe.gov/pub/state.data/data/ from 1960-1999; Jet fuel reporting started in 1952.Aviation gasoline, fuel used in transportation sector, reporting started in 1960 YEAR Asphalt Aviat Kerosen Lubrict LPG Jet fuel Motor gas. Other Distillate f Residual f. 1930 4 0 8 2 0 0 39 2 4 36 1931 4 0 8 2 0 0 43 3 5 36 1932 4 0 8 2 0 0 47 4 7 37 1933 4 0 8 2 0 0 51 5 9 38 1934 4 0 8 3 0 0 55 6 10 39 1935 4 0 8 3 0 0 59 7 12 40 1936 4 0 8 3 0 0 64 8 14 41 1937 4 0 8 3 0 0 68 9 15 42 1938 5 0 8 3 0 0 72 10 17 43 1939 5 0 8 3 0 0 76 11 18 44 1940 5 0 9 3 0 0 80 12 22 46 1941 6 0 9 4 0 0 91 13 24 52 1942 6 0 10 4 0 0 80 12 25 55 1943 5 0 9 4 0 0 78 13 28 64 1944 5 0 10 4 0 0 86 15 29 70 1945 5 0 10 5 0 0 95 16 31 71 1946 7 0 12 5 5 0 100 14 33 65 1947 7 0 14 5 7 0 108 14 41 71 1948 8 0 15 5 9 0 119 14 46 68 1949 8 0 14 5 9 0 125 14 45 68 1950 9 0 16 5 12 0 136 15 54 75 1951 10 0 17 6 14 0 149 16 61 77 1952 11 0 17 5 15 0 156 16 65 76 1953 11 0 16 6 16 0 164 18 67 76 1954 11 0 16 5 18 0 168 19 72 71 1955 13 0 16 6 20 0 182 22 79 76 1956 14 0 16 6 22 0 187 23 84 77 1957 13 0 15 6 23 0 190 24 84 75 1958 14 0 15 5 24 0 196 25 89 72 1959 15 0 15 6 29 0 203 26 90 77 1960 15 8 14 6 31 19 198 29 93 76 1961 15 8 13 6 32 21 201 31 95 75 1962 17 7 13 6 35 24 209 32 100 74 1963 17 7 13 6 38 26 216 37 102 74 1964 17 6 13 6 40 28 220 42 102 76 1965 18 6 13 6 42 30 229 43 106 80 1966 19 5 14 7 44 33 239 46 109 85 1967 19 4 14 6 47 41 247 47 112 89 1968 20 4 14 7 53 48 263 50 119 91 1969 21 3 14 7 61 49 275 53 123 98 1970 22 3 13 7 61 48 288 54 126 110 1971 23 2 12 7 62 50 299 54 133 114 1972 23 2 12 7 71 52 318 59 145 126 1973 26 2 11 8 72 53 332 63 154 141 1974 24 2 9 8 70 49 326 63 147 131 1975 21 2 8 7 66 50 332 62 142 123 1976 21 2 8 8 70 49 348 69 156 140 1977 22 2 9 8 71 52 357 78 167 153 1978 24 2 9 9 70 53 369 82 171 151 1979 24 2 9 9 79 54 350 89 165 141 1980 20 2 8 8 73 53 328 91 143 125 1981 17 2 6 8 73 50 328 71 141 104 1982 17 1 6 7 75 50 326 61 133 85 1983 19 1 6 7 75 52 330 63 134 71 1984 20 1 6 8 79 59 334 68 142 68 1985 21 1 6 7 80 61 340 65 143 60 1986 22 2 5 7 75 65 350 68 145 71 1987 23 1 5 8 80 69 359 73 148 63 1988 23 1 5 8 83 72 366 80 156 69 1989 23 1 4 8 83 74 365 79 157 68 1990 24 1 2 8 77 76 360 85 150 61 1991 22 1 2 7 84 73 358 81 145 58 1992 23 1 2 7 88 73 363 91 149 55 1993 24 1 2 8 86 73 372 87 151 54 1994 24 1 2 8 94 76 379 90 157 51 1995 24 1 3 8 95 75 388 87 160 42 1996 24 1 3 8 100 79 394 95 168 42 1997 25 1 3 8 101 80 399 99 171 40 1998 26 1 4 8 97 81 411 97 172 44 1999 27 1 4 8 109 83 420 100 178 41 2000 54 Table 3. US mercury mobilized in coal produced YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Appalachian 75 62 49 53 58 58 68 69 54 61 72 80 89 88 92 84 82 96 91 66 77 81 70 68 58 68 74 72 59 59 58 56 59 64 67 70 72 74 73 73 78 69 71 69 70 73 75 72 68 77 81 78 79 70 81 78 78 80 81 84 88 83 83 74 81 79 79 83 87 81 76 Eastern Interior 7 6 5 5 6 6 7 7 6 7 7 8 9 10 11 11 9 11 10 8 9 9 8 8 7 8 9 8 8 8 8 8 9 9 10 10 11 12 12 12 13 12 13 13 12 13 12 12 10 12 12 11 12 11 13 12 12 13 12 12 13 12 12 10 11 10 12 12 12 12 12 Gulf Coast 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 1 1 2 2 3 3 4 5 6 7 7 8 8 9 10 11 11 11 12 11 12 12 11 11 13 13 14 13 14 Rocky Mountain 2 2 1 1 1 1 2 2 1 2 2 2 2 3 3 2 2 2 2 2 2 2 2 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 2 2 3 3 4 5 6 8 9 11 13 15 16 17 16 19 19 19 20 22 23 24 25 25 27 30 32 32 32 33 34 34 Great Plains 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 1 1 1 1 1 1 1 1 1 1 2 2 2 2 2 2 2 3 3 3 3 3 3 3 3 3 4 3 4 4 4 4 4 US 84 70 56 60 66 66 77 78 61 70 81 90 101 101 106 98 93 109 104 77 89 91 80 77 66 77 84 82 68 68 68 65 68 75 79 82 85 87 86 88 93 84 89 88 89 95 99 98 94 109 116 114 117 107 123 121 122 126 129 134 140 135 135 126 137 135 140 145 149 144 140 55 Table 4. US mercury mobilized in petroleum products. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Asphalt 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 Aviation Kerosen. Lubricts. 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 LPG 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.2 0.2 0.2 0.2 0.2 0.2 0.3 0.3 0.3 0.3 0.4 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.6 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.8 0.7 0.7 0.7 0.8 0.8 0.8 0.8 0.8 0.8 0.8 0.8 0.8 0.9 0.9 0.9 0.9 1.0 1.0 1.0 1.1 Jet fuel 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.2 0.1 0.1 0.1 0.2 0.2 0.2 0.2 0.2 0.2 Motor gas. 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.2 0.2 0.2 0.2 0.2 0.2 0.2 0.2 0.2 0.2 0.2 0.3 0.3 0.3 0.3 0.3 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.5 0.5 0.5 0.5 0.6 0.6 0.6 0.6 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.7 0.8 0.8 0.8 0.8 0.8 0.8 Other Distillate f. 1.0 0.0 1.0 0.0 1.0 0.0 1.0 0.0 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.1 1.0 0.2 1.0 0.2 1.0 0.2 1.0 0.2 1.0 0.2 1.0 0.3 1.0 0.3 1.0 0.3 1.0 0.3 1.0 0.4 1.0 0.4 1.0 0.4 1.0 0.4 1.0 0.4 1.0 0.5 1.0 0.5 1.0 0.5 1.1 0.5 1.1 0.5 1.1 0.5 1.2 0.5 1.2 0.5 1.2 0.6 1.3 0.6 1.4 0.6 1.4 0.6 1.4 0.7 1.5 0.7 1.6 0.8 1.6 0.7 1.6 0.7 1.6 0.8 1.8 0.8 1.8 0.9 1.9 0.8 1.8 0.7 1.7 0.7 1.6 0.7 1.6 0.7 1.7 0.7 1.7 0.7 1.8 0.7 1.9 0.7 2.1 0.8 2.1 0.8 2.2 0.8 2.1 0.7 2.3 0.7 2.2 0.8 2.3 0.8 2.2 0.8 2.3 0.8 2.4 0.9 2.5 0.9 2.6 0.9 Residual f. 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.4 0.5 0.5 0.6 0.6 0.7 0.7 0.7 0.7 0.7 0.7 0.8 0.8 0.8 0.8 0.7 0.8 0.8 0.7 0.7 0.8 0.8 0.7 0.7 0.7 0.8 0.8 0.9 0.9 0.9 1.0 1.1 1.1 1.3 1.4 1.3 1.2 1.4 1.5 1.5 1.4 1.3 1.0 0.9 0.7 0.7 0.6 0.7 0.6 0.7 0.7 0.6 0.6 0.5 0.5 0.5 0.4 0.4 0.4 0.4 0.4 Total 1.4 1.4 1.5 1.5 1.5 1.5 1.6 1.6 1.6 1.7 1.7 1.8 1.8 1.9 2.0 2.0 2.0 2.2 2.2 2.2 2.4 2.5 2.5 2.6 2.6 2.7 2.8 2.7 2.8 2.9 3.0 3.1 3.2 3.2 3.3 3.5 3.6 3.7 4.0 4.2 4.4 4.5 5.0 5.3 5.1 5.0 5.3 5.7 5.7 5.7 5.3 4.9 4.6 4.5 4.6 4.6 4.9 5.0 5.2 5.2 5.2 5.1 5.3 5.3 5.4 5.3 5.6 5.6 5.7 6.0 56 Table 5. US mercury mobilized in electrical category (BOM) YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Lighting 81 80 78 77 76 74 73 72 70 69 68 66 65 63 62 61 59 58 57 55 54 53 51 50 49 47 46 45 43 42 41 39 38 36 35 34 32 31 18 36 36 28 44 51 40 41 45 31 31 33 29 34 38 27 30 29 29 Switches Batteries Electrical, BOM 103 103 103 103 103 103 103 103 103 103 103 103 103 103 110 111 106 91 69 80 94 95 103 131 176 141 70 71 82 83 79 84 49 57 81 77 35 167 767 60 160 151 182 346 286 210 267 310 257 276 256 264 250 264 300 346 332 341 403 458 410 529 491 405 439 394 480 539 447 811 871 843 872 959 1015 858 805 1024 952 750 533 448 250 106 78 13 10 6 3 0 0 162 157 113 244 843 134 233 223 252 415 353 276 332 373 319 337 315 322 307 319 354 399 383 494 555 608 559 677 637 550 582 536 621 678 585 948 1006 984 1001 1101 1142 955 929 1169 1087 894 709 655 422 209 178 129 131 112 117 78 86 57 Table 6. Mercury mobilized in electrical sector (US EPA, 1997) YEAR Lighting Switches Batteries Electrical, reconstructed 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1 1964 2 1965 3 1966 4 1967 5 283 1968 6 282 1969 7 280 1970 17 8 282 307 1971 17 9 284 310 1972 19 10 290 319 1973 20 11 300 331 1974 20 12 315 346 1975 20 13 328 361 1976 22 14 346 381 1977 22 15 365 403 1978 20 16 390 426 1979 20 17 424 461 1980 22 18 455 495 1981 23 19 484 526 1982 23 20 511 554 1983 25 21 537 583 1984 25 22 568 614 1985 26 22 586 634 1986 26 23 535 584 1987 29 24 564 617 1988 32 25 573 631 1989 24 27 516 567 1990 25 29 455 481 1991 26 30 394 394 1992 27 31 333 307 1993 28 32 272 220 1994 29 32 211 209 1995 30 33 152 199 1996 32 34 136 188 1997 33 34 120 177 1998 1999 2000 58 Table 7. Shipments and mercury flow for HID and fluorescent lamps (Shipments US Bureau of Census, yealy (a) and US EPA, 1992, mercury concentration *US EPA, 1992, ** Benazon, 2000). YEAR HID, 1000 l HID Hg mg/lamp Fluor,1000 l Hg* mg/lamp Hg**, mg/lamp Light*, Mg/yr Light**, Mg/yr 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 229,000 0.075 0.075 1967 226,000 0.075 0.075 1968 245,000 0.075 0.075 1969 264,000 0.075 0.075 1970 6,841 0.033 260,000 0.075 0.075 17.4 17.4 1971 7,684 0.033 260,000 0.075 0.075 17.2 17.2 1972 8,420 0.033 283,000 0.075 0.075 18.7 18.7 1973 9,349 0.033 294,000 0.075 0.075 19.9 19.9 1974 9,158 0.033 265,000 0.075 0.075 19.8 19.8 1975 8,737 0.033 256,000 0.075 0.075 19.8 19.8 1976 10,383 0.033 280,233 0.075 0.075 21.6 21.6 1977 10,853 0.033 290,305 0.075 0.075 22.4 22.4 1978 12,175 0.033 297,263 0.075 0.075 20.3 20.3 1979 13,532 0.033 318,931 0.075 0.075 19.6 19.6 1980 30,187 0.033 324,213 0.075 0.075 22.0 22.0 1981 21,397 0.033 338,062 0.075 0.075 22.5 22.5 1982 20,891 0.033 336,531 0.075 0.075 23.0 23.0 1983 22,146 0.033 376,184 0.075 0.075 24.7 24.7 1984 25,636 0.033 420,668 0.075 0.075 25.2 25.2 1985 25,529 0.025 428,061 0.055 0.055 26.0 26.0 1986 22,206 0.025 446,147 0.055 0.055 25.8 25.8 1987 28,143 0.025 454,381 0.055 0.055 28.9 28.9 1988 24,479 0.025 485,802 0.055 0.055 32.2 32.2 1989 28,090 0.025 497,725 0.055 0.055 24.2 24.2 1990 24,479 0.025 497,725 0.055 0.055 25.2 25.2 1991 22,408 0.025 549,691 0.055 0.055 25.6 25.6 1992 19,497 0.025 560,044 0.055 0.030 27.2 27.2 1993 21,605 0.025 589,693 0.055 0.030 27.9 27.9 1994 21,074 0.025 619,432 0.055 0.030 27.9 27.9 1995 25,009 0.025 644,432 0.055 0.030 30.9 30.9 1996 25,009 0.025 669,432 0.055 0.030 31.4 17.4 1997 25,009 0.025 694,432 0.055 0.030 33.1 18.3 1998 25,009 0.025 719,432 0.055 0.030 34.7 19.2 1999 25,009 0.025 744,432 0.055 0.030 36.1 20.0 2000 25,009 0.025 769,432 0.055 0.030 37.4 20.7 59 Table 8. Paint shipments, Mg/yr. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Paint Architectural Exter., water type Inter. Water-type 1,801,767 164,462 475,633 199,964 505,393 320,569 693,871 508,003 693,871 534,108 545,109 582,235 609,306 560,271 625,022 648,761 673,253 711,283 746,791 714,175 746,942 822,715 837,699 792,851 867,621 981,485 946,854 919,136 876,434 842,549 845,531 971,581 1,044,764 1,069,042 1,114,318 1,216,039 1,292,918 1,300,269 1,372,094 1,351,780 1,483,276 1,554,104 1,690,842 1,618,312 1,717,307 1,749,218 1,647,936 1,771,094 1,813,154 892,791 1,143,399 1,461,880 1,383,565 2,714,920 2,198,041 2,171,936 2,688,815 2,626,163 2,704,478 3,106,495 3,393,650 3,461,523 3,252,683 3,357,103 3,539,838 3,785,225 4,046,275 4,369,977 4,082,822 4,401,303 4,599,701 4,317,767 4,344,047 4,149,129 4,027,912 4,184,880 3,992,593 4,325,122 4,214,834 4,903,041 4,644,080 4,869,141 4,814,843 4,973,634 5,427,162 5,704,083 5,807,271 5,945,492 6,173,216 6,229,843 6,364,926 6,165,870 6,453,156 6,977,867 7,471,773 7,352,734 7,665,472 7,689,489 7,537,558 7,655,030 7,703,063 1,827,939 1,657,145 1,857,757 1,768,843 1,768,843 1,890,263 1,879,560 1,859,410 2,081,534 1,978,608 2,071,847 1,909,320 2,503,086 2,322,810 2,093,412 2,048,005 2,238,504 2,377,763 2,485,206 2,589,992 2,751,310 2,797,929 2,806,533 2,911,820 2,814,688 3,005,208 3,174,890 3,366,501 3,242,763 3,343,006 3,422,888 3,297,584 3,446,904 3,370,678 60 Table 9. Mercury in paints. YEAR Reconstr., 300 ppm 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 249 1967 229 1968 277 1969 306 1970 275 1971 283 1972 263 1973 252 1974 275 1975 253 1976 298 1977 288 1978 330 1979 389 1980 363 1981 398 1982 409 1983 421 1984 467 1985 462 1986 477 1987 483 1988 528 1989 547 1990 564 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Ext. water-type 112 114 122 128 118 131 136 141 149 157 150 Int. water-type 38 38 44 47 48 50 55 58 59 62 61 Reconstr. water-type 150 153 166 175 166 181 191 200 208 219 211 Hg, BOM 23 42 93 84 57 34 26 34 58 108 86 41 23 18 25 18 20 20 121 146 209 161 229 225 292 306 247 364 335 357 297 283 262 235 239 270 288 309 344 297 243 234 208 160 169 179 198 197 192 22 61 Table 10. Seed used in million bushels; apples and golf turf in million acres. YEAR Wheat Oats Barley Rye Apples Golf turf 1930 81 102 21 9 2.1 0.4 1931 80 90 14 9 2.1 0.4 1932 84 100 21 9 2.1 0.4 1933 78 59 11 9 2.1 0.4 1934 83 44 8 9 2.0 0.4 1935 87 97 20 9 1.9 0.4 1936 96 63 10 10 1.9 0.4 1937 93 94 16 9 1.8 0.4 1938 74 87 18 10 1.7 0.4 1939 73 77 19 7 1.6 0.4 1940 74 100 22 8 1.6 0.4 1941 62 95 25 8 1.5 0.4 1942 65 107 30 7 1.5 0.4 1943 77 91 23 6 1.5 0.4 1944 80 92 19 5 1.4 0.4 1945 82 122 19 4 1.4 0.4 1946 87 118 19 5 1.4 0.4 1947 91 94 20 5 1.4 0.4 1948 95 116 22 4 1.4 0.4 1949 81 109 21 5 1.4 0.4 1950 87 100 18 5 1.4 0.4 1951 88 105 15 4 1.3 0.4 1952 91 108 16 5 1.3 0.4 1953 82 118 24 6 1.2 0.4 1954 69 119 26 7 1.0 0.4 1955 66 111 24 6 1.0 0.4 1956 70 105 26 6 1.0 0.4 1957 67 95 26 6 1.0 0.4 1958 102 88 26 5 1.0 0.5 1959 78 79 24 6 1.0 0.5 1960 95 82 25 6 1.0 0.5 1961 86 75 23 7 0.9 0.5 1962 76 71 21 6 1.0 0.6 1963 80 65 18 6 0.9 0.6 1964 90 61 16 6 0.9 0.6 1965 92 60 17 6 0.9 0.7 1966 92 53 16 5 0.9 0.7 1967 107 60 17 5 0.9 0.7 1968 110 60 16 6 0.9 0.8 1969 56 62 16 6 0.9 1.0 1970 62 57 18 7 0.9 1.1 1971 1.1 1972 1.2 1973 1.2 1974 1.3 1975 1.3 1976 1.3 1977 1.3 1978 1.3 1979 1.3 1980 1.3 1981 1.3 1982 1.3 1983 1.4 1984 1.4 1985 1.4 1986 1.4 1987 1.4 1988 1.4 1989 1.4 1990 1.4 1991 1.5 1992 1.5 1993 1.5 1994 1.5 1995 1.6 1996 1.6 1997 1.6 1998 1.7 1999 1.7 2000 1.8 62 Table 11. U.S. mercury use estimates for seed treatment, foliar treatment of apples and grass turf treatment. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Wheat 23.1 22.8 23.9 22.2 23.6 24.9 27.3 26.5 21.2 20.8 21.2 17.8 18.7 22.0 22.9 23.4 24.7 26.0 27.1 23.0 24.9 25.1 26.1 23.4 19.6 18.7 20.1 19.1 29.1 22.3 27.0 24.6 21.8 22.9 25.6 26.2 26.2 30.4 31.4 16.0 17.7 Oats 29.1 25.6 28.6 16.8 12.4 27.6 18.1 26.8 24.8 21.8 28.4 27.0 30.6 26.0 26.2 34.7 33.6 26.8 33.1 31.1 28.5 29.9 30.8 33.6 33.9 31.6 29.9 27.1 25.1 22.5 23.4 21.4 20.2 18.5 17.4 17.1 15.1 17.1 17.1 17.7 16.2 Barley 6.0 4.0 6.0 3.0 2.3 5.8 2.9 4.4 5.1 5.5 6.2 7.2 8.6 6.4 5.5 5.3 5.3 5.6 6.3 6.0 5.1 4.3 4.6 6.8 7.4 6.8 7.4 7.4 7.4 6.8 7.1 6.6 6.0 5.1 4.6 4.8 4.6 4.8 4.6 4.6 5.1 Rye 2.5 2.5 2.5 2.5 2.5 2.5 2.8 2.6 2.8 2.1 2.3 2.4 1.9 1.6 1.5 1.3 1.4 1.4 1.3 1.4 1.4 1.2 1.3 1.6 2.0 1.8 1.7 1.7 1.6 1.6 1.6 1.9 1.7 1.8 1.7 1.6 1.5 1.4 1.7 1.8 2.0 Apples 7 7 7 7 7 6 6 6 6 6 6 6 5 5 4 4 4 4 4 4 4 4 4 4 4 4 4 4 4 Golf turf 18 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 17 18 18 18 19 19 20 21 22 23 25 26 28 29 30 33 34 45 49 50 52 53 54 55 56 56 57 57 58 Agriculture* 57 57 57 57 57 57 57 57 57 57 57 34 34 34 68 61 54 97 122 81 78 133 102 120 132 128 171 109 108 110 103 88 147 88 108 108 82 129 118 93 62 51 63 63 34 21 21 20 16 11 7 3 1 2 2 2 0 0 0 0 0 63 Table 12. US mercury mobilized in fuels and goods. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Coal Petrol 84 1.1 70 1.2 56 1.2 60 1.3 66 1.4 66 1.4 77 1.5 78 1.5 61 1.6 70 1.7 81 1.8 90 1.9 101 1.8 101 2.0 106 2.3 98 2.3 93 2.5 109 2.5 104 2.5 77 2.6 89 2.9 91 3.2 80 3.3 77 3.5 66 3.5 77 3.7 84 3.9 82 3.9 68 3.8 68 4.0 68 4.0 65 4.1 68 4.2 75 4.3 79 4.4 82 4.5 85 4.7 87 4.9 86 5.1 88 5.3 93 5.4 84 5.6 89 5.8 88 6.2 89 6.0 95 6.2 99 6.7 98 7.3 94 7.3 109 7.3 116 6.7 114 6.2 117 5.8 107 5.8 123 6.0 121 6.0 122 6.3 126 6.4 129 6.6 134 6.7 140 6.7 135 6.6 135 6.8 126 7.0 137 7.2 135 7.4 140 7.6 145 7.8 149 8.0 144 8.2 140 8.2 Clor- Pharm. 5 5 5 5 5 5 5 5 5 5 5 5 92 19 279 24 502 23 288 21 384 19 141 24 105 28 117 26 119 45 207 53 95 86 48 82 64 74 64 107 54 116 55 139 60 157 49 201 59 214 60 209 87 252 116 276 141 330 12 302 14 398 8 493 10 602 15 714 25 517 24 419 24 397 20 451 21 582 21 525 15 553 2 370 385 420 326 252 215 278 253 235 259 311 354 379 247 184 209 180 135 154 136 160 Agric. 68 53 56 135 99 108 194 243 161 155 267 203 239 264 255 342 218 216 260 223 195 237 185 182 128 103 144 132 112 70 51 63 63 34 21 21 20 3 1 Paint 52 42 34 61 53 52 71 72 41 43 59 23 42 93 84 57 34 26 34 58 108 86 41 23 18 25 18 20 20 121 146 209 161 229 225 292 306 247 364 335 357 297 283 262 235 239 270 288 309 344 297 243 234 208 160 169 179 198 197 192 22 6 Lab Use 17 14 11 20 18 17 24 24 14 14 20 6 10 12 9 12 9 11 15 12 22 18 22 43 39 34 34 31 33 38 45 51 60 43 55 39 76 67 69 67 62 62 20 23 16 12 21 14 14 14 13 11 10 10 9 14 20 20 26 18 32 28 28 24 26 22 20 Electric 65 52 40 77 65 65 90 92 49 53 73 162 157 113 244 843 134 233 223 252 415 353 276 332 373 319 337 315 322 307 319 354 399 383 494 555 608 559 677 637 550 582 536 621 678 585 948 1,006 985 1,005 1,106 1,142 955 929 1,169 1,087 901 709 655 422 209 132 129 131 112 114 78 86 Control 113 92 73 133 114 113 154 157 88 94 127 125 122 127 112 130 159 186 195 173 186 212 221 191 179 194 211 208 209 212 225 194 179 170 171 160 251 257 275 229 167 168 225 247 214 159 175 180 120 124 105 195 106 85 98 79 63 59 77 87 108 90 80 65 53 43 41 24 Dental 22 18 14 26 22 22 30 30 17 18 24 21 41 19 15 19 39 27 34 33 50 28 35 39 49 41 46 47 60 63 61 74 70 81 90 56 74 82 106 99 79 81 103 92 104 81 69 42 18 49 61 56 35 55 49 50 52 56 53 39 44 41 42 35 24 32 31 40 Other 596 485 385 702 600 596 813 827 463 494 669 1,041 990 932 568 588 444 420 705 540 506 847 534 789 417 942 709 785 747 630 471 550 776 1,179 1,289 991 639 537 361 448 294 118 175 92 165 118 177 191 216 188 125 140 131 130 147 84 114 93 141 72 58 26 102 103 110 93 86 36 64 Table 13. Florida fuel consumption 1930-2000 in million Mg/yr (ftp://ftp.eia.doe.gov/pub/state.data/data/ from 1960-1999, and BOM for 1930-1960. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Coal. 1.7 1.4 1.2 1.3 1.4 1.5 1.7 1.8 1.5 1.6 1.9 2.2 2.5 2.9 3.0 2.9 2.6 2.8 2.6 2.2 2.1 2.1 1.9 1.8 1.5 1.7 1.8 1.7 1.6 1.6 1.0 1.4 1.5 1.6 1.8 2.1 2.7 3.8 4.1 4.1 4.7 4.7 5.0 6.0 5.8 5.2 5.5 6.3 6.8 7.7 8.7 9.0 9.1 11.9 14.0 17.5 17.0 21.5 22.3 23.1 22.9 23.6 23.9 24.0 23.7 24.1 25.8 26.1 26.2 24.8 26.2 Asphalt 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.45 0.41 0.43 0.48 0.50 0.48 0.55 0.57 0.55 0.56 0.56 0.67 0.70 0.80 0.80 0.50 0.47 0.60 0.68 0.66 0.61 0.68 0.68 0.78 0.95 0.91 1.12 1.03 1.08 0.88 0.93 1.00 0.95 1.14 1.00 0.90 0.81 0.48 0.52 0.50 Aviation gas 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.62 0.54 0.74 0.76 0.64 0.58 0.52 0.49 0.47 0.36 0.43 0.35 0.29 0.28 0.29 0.26 0.23 0.20 0.21 0.17 0.18 0.16 0.12 0.12 0.10 0.11 0.14 0.11 0.12 0.13 0.11 0.10 0.08 0.07 0.07 0.08 0.07 0.08 0.06 0.08 Distillate f 0.11 0.13 0.15 0.17 0.19 0.21 0.23 0.24 0.24 0.27 0.29 0.34 0.33 0.36 0.33 0.36 0.45 0.51 0.55 0.52 0.63 0.73 0.94 0.98 1.15 1.31 1.39 1.39 1.11 1.12 1.18 1.24 1.42 1.46 1.51 1.68 1.90 1.85 2.04 2.02 2.13 2.25 2.65 3.11 3.07 3.19 3.34 3.97 4.16 3.97 4.02 4.08 3.13 3.81 3.99 4.15 4.34 4.49 4.70 4.82 4.69 4.28 4.73 3.22 4.60 5.45 5.35 5.85 6.13 6.49 Jet fuel 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 1.29 1.45 1.77 1.96 2.14 2.39 2.41 2.87 3.31 3.48 3.25 3.59 3.91 3.81 3.23 3.30 3.42 3.72 3.82 4.26 4.90 4.86 4.60 4.11 3.31 3.15 3.41 3.62 4.36 4.58 4.36 3.42 3.33 3.63 3.91 3.83 4.00 4.16 3.89 3.95 Kerosene 0.02 0.03 0.04 0.05 0.07 0.08 0.09 0.11 0.12 0.13 0.15 0.17 0.19 0.20 0.21 0.21 0.26 0.28 0.29 0.31 0.33 0.36 0.36 0.37 0.37 0.36 0.37 0.37 0.70 0.62 0.54 0.51 0.56 0.65 0.60 0.61 0.66 0.45 0.47 0.48 0.50 0.48 0.36 0.29 0.15 0.12 0.22 0.17 0.16 0.16 0.13 0.10 0.14 0.14 0.07 0.35 0.20 0.16 0.16 0.12 0.04 0.03 0.04 0.04 0.03 0.04 0.05 0.04 0.05 0.05 Lubric 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.12 0.12 0.13 0.13 0.13 0.14 0.14 0.12 0.14 0.15 0.15 0.16 0.18 0.20 0.19 0.16 0.18 0.19 0.21 0.22 0.19 0.18 0.17 0.18 0.19 0.17 0.17 0.19 0.19 0.19 0.20 0.18 0.18 0.18 0.19 0.19 0.18 0.19 0.20 0.20 Motor gas 0.10 0.10 0.10 0.23 0.37 0.51 0.64 0.78 0.92 1.05 1.19 1.33 1.55 1.43 1.19 1.39 1.86 2.12 2.37 2.54 2.85 3.13 3.44 3.70 4.01 4.46 4.98 5.44 5.72 6.11 5.89 6.00 6.38 6.63 6.87 7.25 7.73 8.12 8.89 9.61 10.40 11.07 12.29 13.57 13.39 13.72 14.18 14.70 15.46 15.17 14.91 15.27 15.57 16.14 16.57 17.10 17.88 18.80 19.34 19.40 19.42 19.30 19.53 20.50 20.78 21.51 21.70 22.08 23.08 23.68 Residual f 0.42 0.50 0.58 0.66 0.74 0.82 0.90 0.96 0.97 1.07 1.15 1.36 1.33 1.47 1.94 2.04 1.92 2.12 2.20 2.14 2.32 2.77 3.38 3.73 3.94 4.40 4.76 4.94 5.11 4.54 4.12 4.43 5.15 4.99 5.37 5.91 5.69 5.30 5.53 6.04 7.32 8.53 10.41 11.14 10.21 10.82 12.24 11.34 12.10 13.14 13.20 12.33 8.80 8.01 5.79 5.15 7.86 6.23 7.36 7.30 7.44 8.15 8.16 9.56 9.15 6.47 6.50 6.81 9.73 9.01 Other 0.00 0.01 0.01 0.01 0.01 0.01 0.01 0.02 0.02 0.02 0.02 0.02 0.02 0.02 0.03 0.03 0.02 0.02 0.02 0.02 0.02 0.03 0.03 0.03 0.03 0.04 0.04 0.04 0.04 0.04 0.05 0.05 0.06 0.11 0.18 0.18 0.16 0.16 0.18 0.18 0.19 0.19 0.22 0.23 0.24 0.23 0.26 0.30 0.33 0.44 0.41 0.54 0.42 0.38 0.44 0.42 0.47 0.46 0.46 0.45 0.50 0.42 0.44 0.44 0.45 0.42 1.41 1.94 2.12 2.13 65 Table 14. Florida mercury in coal as mined, 1930-2000 in Mg/yr (16th (0.05 ppm) 84th (0.23 ppm ), median (0.11 ppm) and mean (0.14ppm). YEAR 16th perc. 84th perc Medain Mean 1930 0.08 0.38 0.18 0.23 1931 0.07 0.32 0.16 0.20 1932 0.06 0.28 0.13 0.17 1933 0.07 0.30 0.14 0.18 1934 0.07 0.33 0.16 0.20 1935 0.07 0.34 0.16 0.21 1936 0.08 0.39 0.19 0.24 1937 0.09 0.41 0.19 0.25 1938 0.08 0.35 0.17 0.21 1939 0.08 0.38 0.18 0.23 1940 0.09 0.43 0.20 0.26 1941 0.11 0.50 0.24 0.30 1942 0.13 0.58 0.28 0.35 1943 0.15 0.67 0.32 0.41 1944 0.15 0.69 0.33 0.42 1945 0.15 0.67 0.32 0.41 1946 0.13 0.60 0.29 0.37 1947 0.14 0.63 0.30 0.39 1948 0.13 0.60 0.29 0.36 1949 0.11 0.50 0.24 0.30 1950 0.11 0.49 0.24 0.30 1951 0.11 0.49 0.23 0.30 1952 0.09 0.43 0.20 0.26 1953 0.09 0.40 0.19 0.25 1954 0.08 0.35 0.17 0.22 1955 0.09 0.40 0.19 0.24 1956 0.09 0.42 0.20 0.25 1957 0.09 0.40 0.19 0.24 1958 0.08 0.36 0.17 0.22 1959 0.08 0.37 0.18 0.23 1960 0.05 0.23 0.11 0.14 1961 0.07 0.31 0.15 0.19 1962 0.07 0.34 0.16 0.21 1963 0.08 0.37 0.18 0.23 1964 0.09 0.41 0.19 0.25 1965 0.11 0.48 0.23 0.30 1966 0.14 0.63 0.30 0.38 1967 0.19 0.87 0.42 0.53 1968 0.20 0.94 0.45 0.57 1969 0.21 0.95 0.45 0.58 1970 0.23 1.07 0.51 0.65 1971 0.23 1.07 0.51 0.65 1972 0.25 1.14 0.55 0.69 1973 0.30 1.39 0.66 0.84 1974 0.29 1.34 0.64 0.81 1975 0.26 1.21 0.58 0.73 1976 0.28 1.27 0.61 0.77 1977 0.31 1.44 0.69 0.88 1978 0.34 1.55 0.74 0.95 1979 0.39 1.78 0.85 1.08 1980 0.43 1.99 0.95 1.21 1981 0.45 2.08 1.00 1.27 1982 0.45 2.09 1.00 1.27 1983 0.59 2.73 1.31 1.66 1984 0.70 3.23 1.54 1.97 1985 0.88 4.03 1.93 2.45 1986 0.85 3.90 1.87 2.38 1987 1.07 4.93 2.36 3.00 1988 1.12 5.13 2.46 3.12 1989 1.15 5.31 2.54 3.23 1990 1.14 5.27 2.52 3.21 1991 1.18 5.43 2.60 3.30 1992 1.20 5.50 2.63 3.35 1993 1.20 5.52 2.64 3.36 1994 1.18 5.44 2.60 3.31 1995 1.20 5.54 2.65 3.37 1996 1.29 5.94 2.84 3.61 1997 1.30 5.99 2.87 3.65 1998 1.31 6.02 2.88 3.66 1999 1.24 5.69 2.72 3.47 2000 1.31 6.02 2.88 3.67 66 Table 15. Florida mercury in cleaned coal, 1930-2000 in Mg/yr (Eastern coal was cleaned. Assumed 21% Hg removed at mines). YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 16th perc. 0.07 0.06 0.05 0.05 0.06 0.06 0.07 0.07 0.06 0.07 0.07 0.09 0.10 0.12 0.12 0.12 0.10 0.11 0.10 0.09 0.08 0.08 0.07 0.07 0.06 0.07 0.07 0.07 0.06 0.06 0.04 0.05 0.06 0.06 0.07 0.08 0.11 0.15 0.16 0.16 0.18 0.18 0.20 0.24 0.23 0.21 0.22 0.25 0.27 0.31 0.34 0.36 0.36 0.47 0.55 0.69 0.67 0.85 0.88 0.91 0.90 0.93 0.95 0.95 0.93 0.95 1.02 1.03 1.03 0.98 1.03 84th perc 0.30 0.26 0.22 0.24 0.26 0.27 0.31 0.32 0.27 0.30 0.34 0.40 0.46 0.53 0.55 0.53 0.48 0.50 0.47 0.39 0.39 0.39 0.34 0.32 0.28 0.32 0.33 0.31 0.29 0.29 0.18 0.25 0.27 0.29 0.32 0.38 0.50 0.69 0.74 0.75 0.85 0.84 0.90 1.09 1.06 0.95 1.00 1.14 1.23 1.41 1.57 1.64 1.65 2.16 2.55 3.18 3.08 3.90 4.06 4.20 4.16 4.29 4.35 4.36 4.30 4.37 4.69 4.74 4.75 4.50 4.76 Medain 0.14 0.12 0.10 0.11 0.12 0.13 0.15 0.15 0.13 0.14 0.16 0.19 0.22 0.25 0.26 0.25 0.23 0.24 0.23 0.19 0.19 0.19 0.16 0.15 0.13 0.15 0.16 0.15 0.14 0.14 0.09 0.12 0.13 0.14 0.15 0.18 0.24 0.33 0.35 0.36 0.40 0.40 0.43 0.52 0.50 0.46 0.48 0.55 0.59 0.67 0.75 0.79 0.79 1.03 1.22 1.52 1.47 1.86 1.94 2.01 1.99 2.05 2.08 2.08 2.06 2.09 2.24 2.26 2.27 2.15 2.28 Mean 0.18 0.16 0.13 0.15 0.16 0.16 0.19 0.20 0.17 0.18 0.21 0.24 0.28 0.32 0.33 0.32 0.29 0.30 0.29 0.24 0.24 0.24 0.21 0.19 0.17 0.19 0.20 0.19 0.17 0.18 0.11 0.15 0.16 0.18 0.20 0.23 0.30 0.42 0.45 0.45 0.51 0.51 0.55 0.67 0.64 0.58 0.61 0.69 0.75 0.86 0.96 1.00 1.00 1.31 1.55 1.94 1.88 2.37 2.47 2.55 2.53 2.61 2.65 2.65 2.62 2.66 2.85 2.88 2.89 2.74 2.90 67 Table 16. Florida fuel mercury 1930-2000 in Mg/yr ( ftp://ftp.eia.doe.gov/pub/state.data/data/ from 1960-1999, and BOM for 1930-1960. YEAR Asphalt Aviation gas Distillate f Jet fuel Kerosene Lubric Motor gaso Residual fuel Other 1930 0.000 0.000 0.001 0.000 0.000 0.000 0.000 0.004 0.001 1931 0.000 0.000 0.001 0.000 0.000 0.000 0.000 0.005 0.001 1932 0.000 0.000 0.001 0.000 0.000 0.000 0.000 0.006 0.001 1933 0.000 0.000 0.001 0.000 0.000 0.000 0.000 0.007 0.001 1934 0.000 0.000 0.001 0.000 0.000 0.000 0.001 0.007 0.001 1935 0.000 0.000 0.001 0.000 0.000 0.000 0.001 0.008 0.001 1936 0.000 0.000 0.001 0.000 0.000 0.000 0.001 0.009 0.001 1937 0.000 0.000 0.001 0.000 0.000 0.000 0.002 0.010 0.001 1938 0.000 0.000 0.001 0.000 0.000 0.000 0.002 0.010 0.001 1939 0.000 0.000 0.001 0.000 0.000 0.000 0.002 0.011 0.001 1940 0.000 0.000 0.001 0.000 0.000 0.000 0.002 0.011 0.001 1941 0.000 0.000 0.002 0.000 0.000 0.000 0.003 0.014 0.001 1942 0.000 0.000 0.002 0.000 0.000 0.000 0.003 0.013 0.001 1943 0.000 0.000 0.002 0.000 0.000 0.000 0.003 0.015 0.001 1944 0.000 0.000 0.002 0.000 0.000 0.000 0.002 0.019 0.001 1945 0.000 0.000 0.002 0.000 0.000 0.000 0.003 0.020 0.001 1946 0.000 0.000 0.002 0.000 0.000 0.001 0.004 0.019 0.001 1947 0.000 0.000 0.003 0.000 0.000 0.001 0.004 0.021 0.001 1948 0.000 0.000 0.003 0.000 0.000 0.002 0.005 0.022 0.001 1949 0.000 0.000 0.003 0.000 0.000 0.002 0.005 0.021 0.001 1950 0.000 0.000 0.003 0.000 0.000 0.002 0.006 0.023 0.001 1951 0.000 0.000 0.004 0.000 0.000 0.003 0.006 0.028 0.001 1952 0.000 0.000 0.005 0.000 0.000 0.003 0.007 0.034 0.001 1953 0.000 0.000 0.005 0.000 0.000 0.003 0.007 0.037 0.001 1954 0.000 0.000 0.006 0.000 0.000 0.003 0.008 0.039 0.001 1955 0.000 0.000 0.007 0.000 0.000 0.004 0.009 0.044 0.001 1956 0.000 0.000 0.007 0.000 0.000 0.004 0.010 0.048 0.001 1957 0.000 0.000 0.007 0.000 0.000 0.004 0.011 0.049 0.001 1958 0.000 0.000 0.006 0.000 0.000 0.005 0.011 0.051 0.001 1959 0.000 0.000 0.006 0.000 0.000 0.006 0.012 0.045 0.001 1960 0.000 0.001 0.006 0.003 0.000 0.007 0.012 0.041 0.001 1961 0.000 0.001 0.006 0.003 0.000 0.007 0.012 0.044 0.001 1962 0.000 0.001 0.007 0.004 0.000 0.007 0.013 0.052 0.001 1963 0.000 0.002 0.007 0.004 0.000 0.008 0.013 0.050 0.001 1964 0.000 0.001 0.008 0.004 0.000 0.009 0.014 0.054 0.002 1965 0.000 0.001 0.008 0.005 0.000 0.008 0.014 0.059 0.002 1966 0.000 0.001 0.010 0.005 0.000 0.008 0.015 0.057 0.001 1967 0.000 0.001 0.009 0.006 0.000 0.008 0.016 0.053 0.002 1968 0.000 0.001 0.010 0.007 0.000 0.009 0.018 0.055 0.002 1969 0.000 0.001 0.010 0.007 0.000 0.010 0.019 0.060 0.002 1970 0.000 0.001 0.011 0.007 0.000 0.011 0.021 0.073 0.002 1971 0.000 0.001 0.011 0.007 0.000 0.010 0.022 0.085 0.002 1972 0.000 0.001 0.013 0.008 0.000 0.011 0.025 0.104 0.002 1973 0.000 0.001 0.016 0.008 0.000 0.011 0.027 0.111 0.002 1974 0.000 0.001 0.015 0.006 0.000 0.010 0.027 0.102 0.003 1975 0.000 0.001 0.016 0.007 0.000 0.010 0.027 0.108 0.003 1976 0.000 0.000 0.017 0.007 0.000 0.011 0.028 0.122 0.003 1977 0.000 0.000 0.020 0.007 0.000 0.012 0.029 0.113 0.003 1978 0.000 0.000 0.021 0.008 0.000 0.011 0.031 0.121 0.003 1979 0.000 0.000 0.020 0.009 0.000 0.012 0.030 0.131 0.005 1980 0.000 0.000 0.020 0.010 0.000 0.015 0.030 0.132 0.004 1981 0.000 0.000 0.020 0.010 0.000 0.014 0.031 0.123 0.004 1982 0.000 0.000 0.016 0.009 0.000 0.012 0.031 0.088 0.003 1983 0.000 0.000 0.019 0.008 0.000 0.012 0.032 0.080 0.003 1984 0.000 0.000 0.020 0.007 0.000 0.012 0.033 0.058 0.004 1985 0.000 0.000 0.021 0.006 0.000 0.014 0.034 0.052 0.004 1986 0.000 0.000 0.022 0.007 0.000 0.014 0.036 0.079 0.005 1987 0.000 0.000 0.022 0.007 0.000 0.012 0.038 0.062 0.004 1988 0.000 0.000 0.023 0.009 0.000 0.011 0.039 0.074 0.004 1989 0.000 0.000 0.024 0.009 0.000 0.011 0.039 0.073 0.004 1990 0.000 0.000 0.023 0.009 0.000 0.011 0.039 0.074 0.004 1991 0.000 0.000 0.021 0.007 0.000 0.011 0.039 0.081 0.005 1992 0.000 0.000 0.024 0.007 0.000 0.011 0.039 0.082 0.005 1993 0.000 0.000 0.016 0.007 0.000 0.011 0.041 0.096 0.005 1994 0.000 0.000 0.023 0.008 0.000 0.010 0.042 0.091 0.005 1995 0.000 0.000 0.027 0.008 0.000 0.011 0.043 0.065 0.005 1996 0.000 0.000 0.027 0.008 0.000 0.011 0.043 0.065 0.015 1997 0.000 0.000 0.029 0.008 0.000 0.008 0.044 0.068 0.036 1998 0.000 0.000 0.031 0.008 0.000 0.009 0.046 0.097 0.045 1999 0.000 0.000 0.032 0.008 0.000 0.010 0.047 0.090 0.045 2000 68 Table 17. Florida mercury in agriculture, Mg/yr. YEAR # Golf C. Golf C. acres Veget, acres %US Vegeta 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 102 117 132 149 157 164 172 186 203 234 246 254 263 269 354 438 461 502 524 510 538 562 550 707 739 696 700 712 834 749 712 736 796 829 948 917 913 948 1,055 1,110 1,180 1,261 7,145 6,800 6,800 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,623 6,665 6,699 6,706 6,759 6,827 6,876 6,903 7,096 7,287 7,552 7,813 8,160 9,360 10,560 11,920 12,560 13,120 13,760 14,880 16,240 18,720 19,680 20,320 21,040 21,520 28,320 35,040 36,880 40,160 41,920 40,800 43,040 44,960 44,000 56,560 59,120 55,680 56,000 56,960 66,720 59,920 56,960 58,880 63,680 66,320 75,840 73,360 73,040 75,840 84,400 88,800 94,400 100,880 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 171,380 220,730 229,958 223,291 210,013 210,845 282,600 292,050 299,200 322,850 334,700 321,550 323,050 331,150 312,450 274,716 271,919 277,957 265,000 284,100 284,150 278,000 289,550 300,245 301,515 284,950 269,600 265,820 268,306 201,817 200,003 204,995 192,119 193,017 195,319 197,341 182,322 121,800 119,300 128,100 5.9 6.4 7.1 7.1 5.9 5.4 5.4 5.2 5.4 5.9 5.5 5.1 4.7 4.9 4.4 5.8 5.6 6.0 6.0 6.0 7.6 7.7 7.9 8.4 8.8 8.6 8.5 9.0 8.7 8.0 8.0 8.0 7.8 10.6 8.7 8.4 8.5 8.4 8.4 8.6 8.4 8.4 Golf Hg Vegetable and Other Hg 0.31 0.30 0.30 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.30 0.30 0.30 0.31 0.32 0.33 0.34 0.35 0.41 0.46 0.52 0.55 0.57 0.60 0.65 0.71 0.81 0.86 0.88 0.92 0.94 1.23 1.52 1.60 1.75 1.82 1.77 1.87 1.96 0.82 1.82 3.81 1.22 2.60 4.12 3.97 7.59 2.73 1.80 2.56 1.35 0.52 5.32 0.94 2.38 2.06 3.21 2.17 4.28 Agriculture Hg 0.30 0.30 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 1.11 2.11 0.29 0.29 4.11 1.52 2.89 4.42 4.28 7.91 3.06 2.14 2.91 1.76 0.98 5.83 1.49 2.95 2.66 0.65 3.92 2.98 0.86 0.88 5.19 0.94 1.23 1.52 1.60 1.75 1.82 1.77 1.87 1.96 69 Table 18. Florida mercury flow trend, Mg/yr. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Coal Petroleum 0.18 0.16 0.13 0.14 0.16 0.16 0.19 0.19 0.17 0.18 0.20 0.24 0.28 0.32 0.33 0.32 0.29 0.30 0.29 0.24 0.24 0.23 0.20 0.19 0.17 0.19 0.20 0.19 0.17 0.18 0.11 0.15 0.16 0.18 0.19 0.23 0.30 0.42 0.45 0.45 0.51 0.51 0.55 0.66 0.64 0.58 0.61 0.69 0.74 0.85 0.95 1.00 1.00 1.31 1.54 1.93 1.87 2.36 2.46 2.54 2.52 2.60 2.63 2.64 2.60 2.65 2.84 2.87 2.88 2.72 2.88 0.006 0.007 0.008 0.009 0.010 0.011 0.012 0.013 0.014 0.015 0.016 0.019 0.019 0.020 0.024 0.026 0.027 0.030 0.032 0.032 0.035 0.041 0.049 0.054 0.057 0.064 0.070 0.072 0.074 0.070 0.070 0.074 0.085 0.085 0.091 0.097 0.097 0.095 0.101 0.109 0.125 0.139 0.163 0.176 0.164 0.172 0.189 0.186 0.195 0.208 0.211 0.202 0.160 0.155 0.134 0.131 0.163 0.146 0.160 0.160 0.161 0.164 0.167 0.176 0.179 0.158 0.169 0.194 0.235 0.233 Pharm Agricult. 1.40 4.54 9.31 5.46 7.24 2.48 1.86 2.06 2.14 3.83 1.84 0.97 1.33 1.39 1.23 1.32 1.53 1.30 1.60 1.67 2.49 3.41 4.21 0.36 0.43 0.25 0.32 0.48 0.82 0.81 0.83 0.72 0.79 0.82 0.59 0.08 0.31 0.30 0.30 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 0.29 1.11 2.11 0.29 0.29 4.11 1.52 2.89 4.42 4.28 7.91 3.06 2.14 2.91 1.76 0.98 5.83 1.49 2.95 2.66 0.65 3.92 2.98 0.86 0.88 5.19 0.94 1.23 1.52 1.60 1.75 1.82 1.77 1.87 1.96 Paints 0.35 0.68 1.72 1.59 1.07 0.60 0.46 0.60 1.04 2.00 1.66 0.83 0.48 0.39 0.57 0.43 0.51 0.53 3.28 4.06 5.99 4.73 6.84 6.81 8.99 9.55 7.81 11.75 11.05 11.99 10.29 10.17 9.83 9.16 9.48 10.79 11.65 12.70 14.51 12.86 10.79 10.58 9.56 7.49 8.06 8.70 9.80 9.92 9.83 1.15 LabUse Electrical 0.09 0.16 0.22 0.17 0.23 0.16 0.19 0.26 0.22 0.41 0.35 0.44 0.90 0.84 0.77 0.82 0.79 0.88 1.03 1.25 1.46 1.76 1.28 1.66 1.20 2.37 2.12 2.23 2.21 2.08 2.15 0.72 0.86 0.62 0.48 0.84 0.57 0.58 0.59 0.56 0.49 0.45 0.46 0.42 0.67 0.97 0.99 1.31 0.92 1.67 1.58 1.48 1.28 1.39 1.19 1.09 1.10 2.46 2.55 2.09 4.63 15.89 2.36 4.12 3.94 4.52 7.68 6.83 5.57 6.91 8.08 7.24 8.11 8.05 8.56 8.33 8.87 10.14 11.72 11.44 14.95 17.08 18.98 17.68 21.85 21.02 18.47 20.16 19.26 23.29 26.43 23.19 37.89 40.69 40.50 42.38 47.89 50.73 43.17 42.72 54.73 51.86 43.78 35.11 32.97 21.61 10.91 9.38 6.83 6.97 6.01 6.32 4.24 4.18 Control Dental 1.35 1.11 0.89 1.65 1.43 1.43 1.99 2.08 1.20 1.32 2.28 1.90 1.98 2.35 2.12 2.45 2.80 3.29 3.44 3.10 3.44 4.10 4.46 3.98 3.88 4.40 5.08 5.31 5.56 5.75 6.26 5.56 5.26 5.08 5.17 4.92 7.84 8.13 8.88 7.55 5.61 5.82 8.09 9.26 8.34 6.30 6.99 7.28 4.93 5.23 4.55 8.66 4.79 3.91 4.59 3.77 3.06 2.92 3.88 4.45 5.64 4.74 4.24 3.46 2.84 2.32 2.23 2.25 0.26 0.21 0.17 0.32 0.27 0.28 0.38 0.40 0.23 0.25 0.44 0.32 0.67 0.35 0.28 0.36 0.69 0.48 0.60 0.59 0.93 0.54 0.71 0.81 1.06 0.93 1.11 1.20 1.60 1.71 1.70 2.12 2.06 2.42 2.72 1.72 2.31 2.59 3.42 3.27 2.65 2.81 3.70 3.45 4.05 3.21 2.76 1.70 0.74 2.07 2.64 2.49 1.58 2.53 2.29 2.39 2.53 2.77 2.67 2.00 2.30 2.16 2.22 1.86 1.29 1.73 1.69 2.19 Total 2.11 1.78 1.50 2.40 2.16 2.17 2.86 2.98 1.90 2.05 3.23 7.07 11.17 16.68 14.90 27.88 9.68 11.83 13.34 12.17 18.84 19.71 14.75 17.55 20.28 19.68 25.06 20.71 20.81 24.88 25.74 28.97 35.03 33.02 34.91 37.34 42.35 43.07 52.14 47.34 43.14 47.89 44.30 49.56 51.76 45.60 61.90 64.59 62.17 67.71 71.63 74.36 61.73 60.64 71.20 68.80 61.06 54.10 53.35 41.51 24.34 21.05 19.37 16.38 14.31 14.20 12.26 12.77 70 Table 19. Florida mercury emission trend, Mg/yr. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Coal 0.062 0.053 0.045 0.049 0.053 0.055 0.063 0.066 0.056 0.062 0.070 0.081 0.095 0.109 0.112 0.109 0.098 0.103 0.097 0.081 0.080 0.080 0.070 0.066 0.057 0.065 0.068 0.064 0.059 0.060 0.037 0.051 0.056 0.060 0.066 0.079 0.102 0.142 0.152 0.154 0.174 0.174 0.185 0.225 0.217 0.196 0.206 0.234 0.252 0.289 0.324 0.338 0.339 0.444 0.525 0.655 0.634 0.802 0.834 0.863 0.856 0.882 0.894 0.896 0.884 0.899 0.964 0.974 0.977 0.925 0.979 Petroleum 0.006 0.007 0.008 0.009 0.010 0.011 0.012 0.013 0.014 0.015 0.016 0.019 0.019 0.020 0.024 0.026 0.027 0.030 0.032 0.032 0.035 0.041 0.049 0.054 0.057 0.064 0.070 0.072 0.074 0.070 0.070 0.074 0.085 0.085 0.091 0.097 0.097 0.095 0.101 0.109 0.125 0.139 0.163 0.176 0.164 0.172 0.189 0.186 0.195 0.208 0.211 0.202 0.160 0.155 0.134 0.131 0.163 0.146 0.160 0.160 0.161 0.164 0.167 0.176 0.179 0.158 0.169 0.194 0.235 0.233 Pharm Paints LabUse Electrical 0.42 1.36 2.79 1.64 2.17 0.74 0.56 0.62 0.64 1.15 0.55 0.29 0.40 0.42 0.37 0.40 0.46 0.39 0.48 0.51 0.73 0.96 1.14 0.09 0.11 0.06 0.07 0.11 0.18 0.17 0.16 0.13 0.13 0.13 0.09 0.01 0.26 0.51 1.29 1.19 0.81 0.45 0.34 0.45 0.78 1.50 1.25 0.62 0.36 0.29 0.43 0.33 0.38 0.40 2.46 3.04 4.49 3.55 5.13 5.11 6.74 7.17 5.86 8.81 8.29 8.99 7.71 7.63 7.37 6.87 7.11 8.09 8.74 9.53 10.88 9.65 8.10 7.93 7.17 5.62 6.05 6.52 7.35 7.44 7.37 0.86 0.03 0.05 0.07 0.05 0.07 0.05 0.06 0.08 0.06 0.12 0.10 0.13 0.27 0.25 0.23 0.25 0.24 0.26 0.31 0.38 0.43 0.50 0.35 0.43 0.30 0.57 0.49 0.50 0.47 0.43 0.42 0.13 0.14 0.10 0.07 0.11 0.07 0.06 0.06 0.05 0.05 0.05 0.05 0.05 0.08 0.12 0.13 0.18 0.14 0.27 0.27 0.33 0.29 0.31 0.28 0.25 0.24 0.74 0.77 0.63 1.39 4.77 0.71 1.24 1.18 1.36 2.30 2.05 1.67 2.07 2.42 2.17 2.43 2.41 2.57 2.50 2.72 2.97 3.30 3.09 3.87 4.25 4.55 4.08 4.86 4.51 3.83 3.90 3.47 3.90 4.10 3.32 4.99 4.92 4.46 4.24 4.33 4.84 4.35 4.54 6.14 6.15 5.48 4.64 4.60 3.18 1.76 1.68 1.92 1.61 1.35 1.43 0.96 0.91 Control 0.41 0.33 0.27 0.49 0.43 0.43 0.60 0.62 0.36 0.39 0.68 0.57 0.60 0.71 0.64 0.74 0.84 0.99 1.03 0.93 1.03 1.23 1.34 1.19 1.16 1.32 1.52 1.59 1.67 1.73 1.92 1.63 1.48 1.37 1.34 1.23 1.88 1.88 1.98 1.62 1.16 1.13 1.46 1.55 1.29 0.90 0.92 0.88 0.54 0.52 0.41 0.83 0.48 0.42 0.51 0.45 0.38 0.39 0.54 0.66 0.91 0.81 0.94 0.80 0.64 0.54 0.51 0.49 Dental 0.08 0.06 0.05 0.09 0.08 0.08 0.11 0.12 0.07 0.08 0.13 0.10 0.20 0.11 0.09 0.11 0.21 0.14 0.18 0.18 0.28 0.16 0.21 0.24 0.32 0.28 0.33 0.36 0.48 0.51 0.52 0.62 0.58 0.65 0.71 0.43 0.55 0.60 0.76 0.70 0.55 0.54 0.67 0.58 0.63 0.46 0.36 0.21 0.08 0.21 0.24 0.24 0.16 0.27 0.26 0.28 0.32 0.37 0.37 0.29 0.37 0.37 0.49 0.43 0.29 0.40 0.38 0.48 Total 0.6 0.5 0.4 0.6 0.6 0.6 0.8 0.8 0.5 0.5 0.9 2.2 3.6 5.7 5.1 8.8 3.1 3.5 3.7 4.1 6.5 5.5 4.4 4.7 5.0 4.9 5.4 5.6 5.9 8.1 9.2 11.0 10.5 11.9 11.7 13.2 15.0 13.2 17.3 16.0 15.4 14.2 13.8 14.1 13.5 12.3 14.9 15.2 15.1 16.4 15.2 14.6 13.5 13.0 13.2 13.8 13.6 13.8 14.1 12.7 5.2 4.2 4.7 4.2 3.7 3.7 3.2 3.3 71 Table 20. Broward County mercury flow trend, kg/yr. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Coal 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 Petrol 0 0 0 0 0 0 0 0 0 0 0 0 0 0 1 1 1 1 1 1 1 2 2 3 3 4 4 4 5 4 5 5 6 6 7 8 8 8 9 10 11 13 15 16 15 16 19 19 20 21 22 21 16 16 13 13 16 14 16 16 16 16 16 17 17 15 17 20 24 24 25 Pharm 30 101 198 123 178 66 52 60 64 114 67 41 64 73 68 77 91 80 103 111 172 244 314 28 35 21 27 42 73 73 77 67 73 77 57 8 Agric. 4 4 5 5 5 5 6 6 6 6 6 6 6 6 7 7 8 31 62 9 9 150 64 139 232 239 457 181 131 187 117 67 418 111 229 213 54 335 261 76 80 478 87 115 143 154 173 184 182 193 202 Paint LabUse Electrical 8 15 37 36 26 16 13 17 31 60 61 35 23 20 32 25 30 33 211 271 414 339 510 528 720 791 669 1,028 984 1,086 948 946 917 858 909 1,066 1,178 1,306 1,499 1,331 1,103 1,076 969 755 808 865 968 973 958 111 2 4 5 4 6 4 5 8 6 12 13 19 43 44 43 47 47 54 66 83 101 126 96 129 96 197 181 195 197 189 198 67 80 58 46 83 57 59 61 58 50 46 47 42 67 97 98 128 90 161 152 142 123 134 114 108 111 54 57 44 105 391 63 115 115 135 229 250 236 332 424 404 469 477 525 535 592 701 840 853 1,159 1,369 1,573 1,513 1,912 1,872 1,673 1,857 1,792 2,173 2,477 2,224 3,743 4,114 4,163 4,379 4,956 5,185 4,393 4,329 5,518 5,194 4,355 3,466 3,236 2,106 1,052 942 830 670 577 592 422 421 Control 18 16 14 28 25 27 38 41 24 27 47 41 44 50 48 60 75 92 100 93 103 150 189 191 203 246 294 315 341 370 417 384 377 379 401 395 649 696 777 673 508 536 752 864 782 605 691 736 507 540 471 885 488 396 463 377 304 288 380 434 544 456 407 333 273 223 222 227 Dental 4 3 3 5 5 5 7 8 5 5 9 7 15 7 6 9 18 13 17 18 28 20 30 39 56 52 64 71 98 110 113 147 147 180 211 138 191 222 299 291 240 258 344 322 380 308 272 172 76 213 273 254 161 256 231 239 251 274 262 195 221 208 214 179 124 166 168 221 Total 26 24 22 38 35 37 52 55 35 39 63 149 242 348 329 678 252 321 380 356 556 712 617 834 1,055 1,086 1,437 1,215 1,266 1,587 1,710 1,993 2,499 2,450 2,693 2,973 3,483 3,651 4,523 4,176 3,861 4,365 4,071 4,561 4,790 4,318 6,054 6,460 6,313 6,907 7,313 7,499 6,180 6,013 7,023 6,698 5,888 5,108 4,996 3,798 2,104 1,773 1,609 1,322 1,124 1,110 936 1,000 72 Table 21. Broward County mercury emission trend, kg/yr. YEAR 1930 1931 1932 1933 1934 1935 1936 1937 1938 1939 1940 1941 1942 1943 1944 1945 1946 1947 1948 1949 1950 1951 1952 1953 1954 1955 1956 1957 1958 1959 1960 1961 1962 1963 1964 1965 1966 1967 1968 1969 1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 Coal 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 Petrol 0 0 0 0 0 0 0 0 0 0 0 0 0 0 1 1 1 1 1 1 1 2 2 3 3 4 4 4 5 4 5 5 6 6 7 8 8 8 9 10 11 13 15 16 15 16 19 19 20 21 22 21 16 16 13 13 16 14 16 16 16 16 16 17 17 15 17 20 24 24 25 Pharm 0 0 0 0 0 0 0 0 0 0 0 9 30 59 37 53 20 15 18 19 34 20 12 19 22 21 23 27 24 31 34 51 69 85 7 9 5 6 9 16 15 15 12 12 12 8 1 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 Paint 0 0 0 0 0 0 0 0 0 0 0 6 11 27 27 20 12 10 13 23 45 46 26 17 15 24 19 23 24 158 203 311 254 383 396 540 594 501 771 738 815 711 710 688 644 681 800 883 979 1124 998 828 807 727 566 606 649 726 730 719 83 0 0 0 0 0 0 0 LabUse 0 0 0 0 0 0 0 0 0 0 0 1 1 1 1 2 1 2 2 2 4 4 6 13 13 13 14 14 16 20 26 30 36 26 33 24 47 42 43 42 39 38 12 13 9 7 11 7 7 6 5 5 5 5 5 8 12 13 18 13 14 14 74 59 46 54 41 34 Electrical 0 0 0 0 0 0 0 0 0 0 0 16 17 13 31 117 19 34 34 40 69 75 71 100 127 121 141 143 157 161 181 206 236 230 300 341 377 349 426 402 347 359 323 364 384 318 493 497 459 438 448 495 442 460 619 616 545 458 451 310 94 89 431 323 200 282 158 130 Control 6 5 4 8 8 8 12 12 7 8 14 12 13 15 14 18 22 27 30 28 31 45 57 57 61 74 88 94 102 111 128 113 106 102 104 98 156 161 173 145 105 104 136 145 121 87 91 89 56 54 43 84 49 42 52 45 38 38 53 64 48 43 212 160 95 106 83 70 Dental 1 1 1 2 1 2 2 2 1 2 3 2 4 2 2 3 6 4 5 5 8 6 9 12 17 16 19 21 29 33 35 43 41 49 55 34 46 51 67 62 50 50 62 54 59 44 36 21 8 21 25 24 16 27 26 28 31 36 37 29 20 20 111 86 43 79 63 69 Total 7 6 5 10 9 10 14 15 9 10 17 46 78 119 113 214 81 93 104 119 192 197 183 221 258 271 308 327 358 518 612 757 748 880 903 1054 1232 1119 1498 1415 1382 1290 1270 1292 1244 1162 1450 1516 1529 1665 1540 1456 1336 1277 1282 1315 1291 1285 1305 1150 275 182 844 646 401 537 362 323 73 74