Trend of anthropogenic mercury in Florida

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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
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Finkelman, R. B., Oman, C. L. Bragg, L. J. and Tewalt, S. J. (1994) The U.S. Geological Survey
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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
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