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Assessment of Trends in Hg-Related Data Sets & Critical
Assessment of Cause & Effect for Trends in Hg
Concentrations in Florida Biota
C.D. Pollman, Tetra TechD.B. Porcella, Environmental Science & Management
R. Husar, Lantern CorporationJ. Husar Lantern CorporationR. Roberson, RMB Associates
P. Frederick, University of FloridaM. Spalding, University of Florida
13 December 2001
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HOW IT ALL STARTED:
Biota Trend #1 - Recent Declines in Hg in Largemouth Bass collected from the Florida
Everglades. Data from T. Lange (2000).
L-67A CanalAdjusted LS Means
1990 1992 1994 1996 1998 2000
Fille
t Hg
(µg
/g)
0.00
1.00
2.00
3.00
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HOW IT ALL STARTED:
Biota Trend #2 - Concomitant Declines in Hg in Feathers of Everglades Great Egret Nestlings.
Data from P. Frederick (2000).
0
5
10
15
20
25
30
1994 1995 1997 1998 1999
Mea
n f
eath
er m
ercu
ry (
mg
/kg
@8c
m b
ill) 3B Mud
JW1
Hidden
Alley North
L-67
*
*
*
*
**
**
*
*
*
Hg in Great Egret Nestling Feathers
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HOW IT ALL STARTED:
Biota Trend #3 - Comparatively Rapid Response By Aquatic Biota in Everglades Predicted to Occur in Response to
Reductions in Atmospheric Loading Rates of Hg.
0
0.2
0.4
0.6
0.8
1
1.2
1.4
1.6
1.8
0 10 20 30 40 50 60 70
Time After Load Reduction (Years)
Fis
h H
g (u
g/g
wet
mus
cle)
25% Reduction 50% Reduction
75% Reduction 85% Reduction
System Response Time to Load Reduction: E-MCM
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HOW IT ALL STARTED:Comparision of measured MSW Hg emissions (concentrations)
in south Florida with the national inventory on MSW emissions compiled by Franklin and Kearney for USEPA
MSW Hg vs. S. Fla. Hg Emissions
0
100
200
300
400
500
600
700
800
1988
1989
1990
1991
1992
1993
1994
1995
1996
1997
1998
1999
2000
years
To
ns
0
200
400
600
800
1000
1200
[Hg
} u
g/m
3
National Inventory Flux
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Primary Objective BASIC PREMISE: If changes in Hg emissions and deposition have occurred,
and if this in turn produces a comparatively rapid change in biota, contemporaneous trends in a number of media also should be evident, including:
trends in emissions;
trends in atmospheric chemistry and deposition; and
trends in Hg accumulation rates in recent sediments.
OBJJECTIVE: Examine whether the trends in Hg concentrations in south Florida biota are significant, whether the trends (or lack thereof) are consistent with the available data on trends in Hg emissions, atmospheric deposition, and accumulation, and whether other factors need to be invoked to explain the data.
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Secondary Objectives
Examine data pertaining to long-range transport and deposition of Hg and establish whether there have been changes in the signal to south Florida from these sources.
Using E-MCM, verify through model hindcasting whether the trends in largemouth bass are consistent with our understanding of changes in atmospheric loadings of Hg in south Florida.
Explore alternative hypotheses using E-MCM: For example, do other perturbations to the Everglades such as hydrologic changes and changes in sulfate loadings offer equally plausible or better explanations of the observed biotic trends.
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Overall ApproachTest the hypothesis that recent trends in biota Hg concentrations in south Florida are a direct result of emissions
reductions in the region as well.
CRITICALLY ANALYZE TRENDS IN BIOTA
RECONSTRUCT TRENDS IN LOCAL
EMISSIONS
ESTABLISH LINK BETWEEN THE TIMING AND MAGNITUDE OF EMISSIONS AND THE TIMING
AND MAGNITUDE OF BIOTIC RESPONSE.
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Material Flows Hg Trend Reconstruction - Update
Phase I work supported by FDEP and conducted March – May 2001.
Developed trends in Hg emissions drivers for period 1980 – 2000.
At May 10 meeting in WPB, scope expanded from analysis of emission drivers to a broader scale Hg budgeting.
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Material Flows Hg Trend Reconstruction - Update
Independent estimate of atmospheric Hg emissions in S. Florida.
Accounting for the total mercury flow in Florida (air, land and water).
Re-examining, expanding and updating the national Hg budget with new data.
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Approach: Scaling of Development of Hg
Budgets
National
Florida
South Florida
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National Hg Trends in Hg Flow Much of analysis derived from
Sznopek and Goonan, 2000 which defines recent trend of the national mercury flow, including the primary production, consumption, recycling as well as mercury flow from stocks.
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Production – Consumption Cycle Showing Secondary Consumption
Mining Production Consumption
Recycling
Stock
Mine Production Secondary Production
Net Import
Stock Release
Mining Production Consumption
Recycling
Stock
Mine Production Secondary Production
Net Import
Stock Release
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National Hg Flow Trends Apparent Hg supply includes 1 and 2 production,
net imports, and government stockpile releases. 1970 – 1986: Main contributors to Hg flow were 1
mine production and imports. 1986 – 1992: Rapid decrease of apparent Hg
demand caused by reductions in mercury demand for batteries, paint and fungicide industries.
1993 to present: 1 mine production negligible; 2 production (recycling) increased and stock releases were terminated.
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National Hg Flow Trends
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National Hg Releases to Atmosphere, 1996
From Sznopek and Goonan, 2000; USEPA, 1997.
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National Hg Releases to Atmosphere, 1996
Materials flow schematics for 1996. 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, From Sznopek and Goonan, 2000.
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Hg in US Goods and Fuel, 1940 – 1995.
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Hg in US Goods and Fuel, 1940 – 1995.
1940-1970, consumption of Hg in consumer goods was not well characterized. In 1940 74% of Hg consumption was categorized as "Other".
1970-1990, electrical and electronic instruments category (including batteries) dominant Hg industrial use.
Hg demand for consumer goods drastically reduced beginning ca. 1989. Hg consumption in consumer and industrial goods declined from 1500 Mg/yr in 1989 to 500 Mg/yr in 1995 (U.S. Bureau of Mines, 1940-1995).
Hg mobilization in coal has increased since 1940, from ca. <6% of the total to ca. 20% in 1995.
Mercury mobilization by petroleum products (using 5 to 50 ppb Hg concentration for crude oil) increased since 1940. Wilhelm (in press) indicates range is more likely 5 – 15 ppb.
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Trend of Hg Consumption in Coal in Florida
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Trend of Hg Consumption in Petroleum in Florida
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Trend of Hg Consumption in Electrical Sector
On a national scale, electrical uses of Hg increased steadily between 1947 (< 200 Mg/yr and 1986 (1,000 Mg/yr).
1996 use of Hg was 78 Mg Hg use in electrical sector increased
from 14% in early 1960’s to its peak in 1985 of 63% of the total United States consumption.
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Trend of Hg Consumption in Electrical Sector – Approach (Lighting)
< 1978: U.S. Bureau of Mines (BOM) reported a single mercury consumption number for electrical uses.
1978 – Present: BOM gives inside electrical consumption, battery, switches/wiring, and lighting categories with their cumulative value representing the electrical consumption.
Reconstruct Hg in lighting using U.S. Bureau of Census fluorescent and HID lamps domestic shipments. Multiply by Hg content of fluorescent lamps (0.75, 0.55, 0.30) for different time periods, and HID mercury content (0.33 and 0.25) (EPA, 1992, Benazon Environmental, 1998).
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Trend of Hg Consumption in Electrical Sector – Approach (Batteries)
Approach I (Bureau of Mines Hg consumption data)
Electrical switches with Hg not manufactured < 1960 (USEPA, 1997)
Switching/wiring use > 1960 relatively stable ( 100 Mg/yr)
Prior to 1978: Calculate Battery Hg use:Hgbattery = HgTotal Electrical – Hgswitches, lighting
Prior to 1960:Hgbattery = HgTotal Electrical – Hglighting
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Trend of Hg Consumption in Electrical Sector – Approach (Batteries)
Approach II (retail battery sales) Based on work published by USEPA (1992) Use battery retail sales data from National
Electrical Manufacturers Association (NEMA) for 1983-1988, and estimates for 1989, and 1992
Based on, trend was established and used to estimate sales 1967-1982 and 1993-2000, respectively. The amount of mercury battery import was assumed at 15 %.
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Comparison of Hg Use in Batteries – National Scale
BOM data
NEMA data
Note: BOM data do not reflect the exports and imports of batteries.
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Trend of Hg Consumption in Electrical Sector - National
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Trend of Hg Consumption in Electrical Sector - Florida
BatteriesLighting
Switches/Wiring
Note: Scaled from National level data by annual population.
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Trend of Hg Consumption in Agricultural/Fungicide Use –
Approach
Hg consumption in agriculture compiled and reported by Jasinski (1994) and Murphy and Aucott (1999) based on BOM Yearbook data.
Hg consumption in fungicide compiled by Sharvelle (1961) and Murphy and Aucott (1999).
USDA annual Agricultural Statistics provides drivers for small seed (wheat, barley, oats, rye) consumption in USA.
Hg use in fungicides applied to golf courses was estimated by number of golf courses in USA (Scharff, 1970, Ross, 1979, NGF web site). Assume 80 acres/golf course treated with 43 g Hg/acre.
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Trend of Hg Consumption in Agricultural/Fungicide Use –
Approach
Golf courses routinely treated with fungicides late 1950s and 1960s.
Before late 1950s, literature all suggests only affected areas were treated with much higher concentrations of fungicides. In 1970s mercury fungicides were gradually substituted with non-mercury fungicides.
Hg use 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.
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Trend of Hg Consumption in Agricultural/Fungicide Use –
Approach Hg use for potato and vegetable seeds (tomatoes,
watermelon, beets), soil treatment for cabbage and cauliflower, and 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.
Production of wheat, barley, oats, rye and apples is not significant in Florida. Thus, only the Vegetable and Other portion of USA Hg consumption was prorated to Florida, using vegetable acreage ratio of Florida compared to USA vegetable acreage.
The golf course mercury fungicide was estimated using Florida golf course statistics (Bureau of Census, annual 1959-2000).
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Trend of Hg Consumption in Agricultural/Fungicide Use – Data
Sources
Seed Hg estimate Reference
Wheat, barley, oats, rye 0.3-0.6 g/bushel Sharvelle, 1961
Apples 4.5-9 g/acre Murphy and Aucott, 1999
Turf 43 gr/acre Sharvelle, 1961
Potatoes Seed soaking Sharvelle, 1961
Cabbage Soil treatment Sharvelle, 1961
Vegetables and Fruits Seed soaking, foilage treatment
Sharvelle, 1961
Bulbs and corms Bulbs and corms soaking
Sharvelle, 1961
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Trend of Hg Consumption in Agricultural/Fungicide Use - National
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Trend of Hg Consumption in Agricultural/Fungicide Use - Florida
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Trend of Hg Consumption in Paints – Approach
Late 1950s organomercury compounds (principally phenylmercuric acetate) were added to the water type paints to prolong the paint's shelf life.
Use the paint shipment driver and apply the estimated Hg concentration factor to paints.
Information on US paint shipments obtained from U.S. Bureau of Census annual Current Industrial Reports. The historical total paint shipments were obtained from U.S. Bureau of Census, 1975.
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Trend of Hg Consumption in Paints – National Trend in Driver
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Trend of Hg Consumption in Paints – National
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Trend of Hg Consumption in Paints – Florida
Note:Paint Hg estimate for Florida based on U.S. BOM Hg use and Florida population data. Data are subject to change as better information is obtained.
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Synthesis of Florida Trend in Hg Use
Use US data and apportion Hg consumption to Florida.
Cl2 and caustic soda manufacturing use of Hg omitted from Florida trends, since manufacturing is external to Florida and the products do not contain Hg.
“Other” category also omitted in Florida trend reconstruction. Category described in 1960 Bureau of Mines Yearbook as containing “the quantity of Hg to initiate new capacity of chlorine-caustic soda plants”.
Hg in coal for Florida included upper and lower estimates. Used average of the two estimates for trend reconstruction.
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Synthesis of Florida Trend in Hg Use
Hg in petroleum for Florida was reconstructed using Florida consumption data for petroleum products and mercury content of the particular product (Wilhelm, 2001).
The mercury in paints, pharmaceutical, electrical, control, and dental uses were prorated to Florida population.
The agricultural mercury was deconstructed, and only Florida specific uses were estimated.
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Trend of Hg Consumption in Florida
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Synthesis of Florida Trend in Hg Emissions
Use coal and petroleum consumption as described previously
Paint: Assume 75% is emitted to the atmosphere (Benazon Environmental, 1998).
Laboratory, Electrical, Dental, and Control products: Assume disposal as municipal solid waste. In 1980 there were 500 open dumps in Florida. Open burning of waste was a common method to save landfill space (Solid Waste Management in Florida, FL DEP, 1996 p63). In 1982 one WTE was operating in Florida. In 1995 there were 13 WTE.
For 1990-1998 percentage of municipal waste burned in WTE is available (Solid Waste Management in Florida, FL DEP). However, prior to 1980 percentage of municipal solid waste burned is not available. A 16% burning rate was assumed.
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Trend in Hg Emissions in Florida 1930 – 1999
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Trend in Hg Emissions in Florida 1990 – 1999
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Comparison of material flow-based estimates of Hg emissions with FDEP
direct emissions estimates
Note:FL DEP estimates of Hg emissions from municipal waste combustion facilities courtesy of Yi Zhu, FDEP.
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Major Florida Hg in Biota Data Sets
Lange et al. (FGFWFC) largemouth bass data (n sites = 12, total n = 2001)
Frederick et al. Great Egret nestling feather data (n sites = 7 sites; total n = 558; period 1994 - 2001)
Zillioux et al. raccoon data
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Summary of Fish Data Used in Trend Analysis
Data File: Task Through 2000.xls (Lange June 2001 Subsetted.xls)
Data Locations:
Big Lostmans Creek, East Lake Tohopekaliga, Fowlers Bluff, Indian Camp Creek-Rogers, L-35B Canal, Lake Tohopekaliga, Marsh-15, Marsh-GH, Marsh-OM, Marsh-U3, Miami Canal and L-67A, North Prong
Number of Data Points:
1464 measurements of Hg in Largemouth Bass
Number of Age Groups:
0, 1, 2, 3, 4, 5, 6, 7, 8, 9
Period Of Time:
10/31/1988 – 03/14/2001
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Statistical Analysis Methods Simple Linear Regression versus
Time
Mann-Kendall Slope Test-of-Sign
Median Slope (computed Sen Slope estimate)
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Mann-Kendall Slope Test-of-Sign
j k
j k
j k
j k
j k
C CSlope
T T
1 if C C 0
Sign 0 if C C 0
1 if C C 0
For all j and k such that j > k
where Cj is the mercury concentration at time Tj. If a total of n samples are collected over time, then there are n(n-1)/2 slope calculations.
Sen’s slope estimator is equal the median slope from that of the n(n-1)/2 slope calculations.
Mann-Kendall routine is a non-parametric test for zero slope
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Why Use the Mann-Kendall Routine? Standard t-test of simple linear
regression is misleading when Seasonal cycles are present
Data are not normally distributed
Data are serially correlated
The above conditions over predict the significance of the slope when the true slope is actually zero
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Hg Concentration Data Availability for Largemouth Bass
Location/Age 0 1 2 3 4 5 6 7 8 9 Total
Big Lostmans Creek 8 42 25 20 9 0 0 0 0 0 104
East Lake Tohopekaliga 0 15 59 55 29 26 14 7 2 0 207
Fowlers Bluff 0 7 45 46 33 24 17 5 7 1 185
Indian Camp Creek-Rogers 1 5 4 2 4 5 0 1 0 0 22
L-35B Canal 1 36 41 41 19 17 11 1 1 0 168
Lake Tohopekaliga 0 4 57 39 45 24 12 2 2 3 188
Marsh-15 12 35 11 6 3 0 1 0 0 0 68
Marsh-GH 15 29 21 7 2 1 2 0 0 0 77
Marsh-OM 0 22 8 2 0 0 0 0 0 0 32
Marsh-U3 8 30 12 9 5 0 1 0 1 0 66
Miami Canal and L-67A 1 55 75 43 31 14 4 4 1 0 228
North Prong 3 29 31 26 19 11 0 0 0 0 119
Total 49 309 389 296 199 122 62 20 14 4 1464
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Trend-Adjusted Results of Mann-Kendall Test-of-Sign
Location/Age 0 1 2 3 4 5 6 7 8 9
Big Lostmans Creek 0 0 0 0 0
East Lake Tohopekaliga – – – – – – 0
Fowlers Bluff 0 0 – 0 0 – 0 0
Indian Camp Creek-Rogers 0 0 0 0
L-35B Canal 0 – – – – 0
Lake Tohopekaliga 0 – 0 – 0 0 0
Marsh-15 – – 0 0 0
Marsh-GH 0 – 0 –
Marsh-OM – –
Marsh-U3 + + + 0 0
Miami Canal and L-67A – – – – – 0 –
North Prong 0 – 0 – – 0
Blank = Insufficient data (54)
– Accept the alternative hypothesis of a downward trend (29)
+ Accept the alternative hypothesis of an upward trend (3)
0 Accept the null hypothesis of no trend (34)
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Typical Examples of Sen’s Non-parametric Estimator of Slope (µg
Hg/g/yr)
– Accept the alternative hypothesis of a downward trend
+ Accept the alternative hypothesis of an upward trend
Location/Age 0 1 2 3 4 5 6 7 8 9
East Lake Tohopekaliga -0.036 -0.042 -0.05 -0.046 -0.063 -0.072 -0.04
Marsh-U3 +0.347 +0.145 +0.106
East Lake Tohopekaliga Data
Marsh-U3 Data
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Cocoa Beach
Terra Ceia Bay
Teneroc
Clewiston
Orange Lake
Lake Griffin
Lake Mary Jane
Lake Kissimmee
Alley North
L-67TTW
Hidden
St. Martins
Seahorse Key
JW1
Location of Frederick et al. (2001) Great Egret and White Ibis Sampling
Sites
Long-term Great Egret monitoring stations, 1994 - 2000
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Hg Concentrations in Great Egret Nestling Feathers. Data courtesy of P Frederick (2001). N sites per
year ≤ 7.
Relative Hg Concentration
0.0
0.2
0.4
0.6
0.8
1.0
1.2
1992 1994 1996 1998 2000 2002
Ave
rage
Rel
ativ
e H
g C
once
ntra
tion
Year
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Zillioux et al. South Florida Raccoon Hair MMHg Study -
Hypotheses
Zillioux et al. South Florida Raccoon Hair MMHg Study -
Hypotheses MMHg levels in raccoon hair have
changed between museum and modern collections.
Raccoon hair MMHg levels are the same when collected from different sites having the same deposition.
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Location Museum (n) ug/g Modern (n) ug/g
North Key Largo 1.0 (15) 1.5 (17)
Flamingo 3.8 (20) 7.2 (21)
Long Pine Key 19.6 (9) 9.4 (11)
Shark Valley Sl. 8.0 (8) 14.9 (19)
South Florida Raccoon Hair MMHg South Florida Raccoon Hair MMHg
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South Florida Raccoon Hair MMHg Conclusions
Cannot conclude that there has been a temporal change in MMHg raccoon hair levels.
Strong differences between sites with relatively similar deposition.
Location is more important than time: Methylation Feeding behavior
Other factors do not seem important: size, life-stage, sex, other elements, analytical artifacts
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Study Tentative Conclusions Estimates of statewide emissions of Hg (based on
materials flow) indicates a large, rapid decline in Hg releases to atmosphere, driven predominantly by reductions in electrical use and cessation of paint product use.
Kendall tau test demonstrates significant declining trends LMB Hg concentrations for a number of sites across the state, but patterns are not ubiquitously observed. Canals appear to be the most consistent showing declining trends, while trends for marsh sites are not uniform.
Only one site, U3, in the entire data set shows increasing trends, and only for year classes 0 to 2
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Study Tentative Conclusions The widespread distribution of declining trends suggests
a regional factor, such as atmospheric deposition, or perhaps long-term climatic variables (e.g., changes in hydrology and concomitant effects on geochemistry.
Likewise, the within region variability in trends evidenced both in the LMB and raccoon data indicate local biogeochemistry and hydrology appears to play a strong role, perhaps more than deposition.
Declines may have stabilized, and limited data from one bird colony suggests perhaps an “uptick” in the trends.
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Project Timeline
July Aug Sept NovOct Dec Jan Feb Mar Apr
Jan 1, 2002Submit 1st Draft
To FCG
Feb 23, 2002Comments
Back From FCG
Mar 15, 2002Submit Final
To FCG
Aug 1 to Oct 31, 2001. Main Hg emission trend analysis.
Submit trends to Tt.
Nov 1 to Dec 31, 2001. Refine
analysis. Draft Report
Jul 1-31, 2001. Preliminary
analysis of LMB data
Oct 1 to Nov 15, 2001. Seasonal Kendall
analysis of fish trends.
Analyze bird data. Integrate
raccoon results.
Dec. 1 to Jan 1, 2002. Integrate biota and emission
trend results. Prepare
draft white paper
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Revised Project Timeline
July Aug Sept NovOct Dec Jan Feb Mar Apr
Materials Flow Analysis of Hg Trends. National and Florida scale
Preliminary analysis of LMB
data
Seasonal Kendall
analysis of fish trends.
Meet with FDEP and submit data request
Work with FDEP to try and expedite data
transfer
Obtain and analyze raw bird data. Integrate raccoon results.
? ?
Complete Regional (south
Florida) analysis.
Update and revise report
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QuickTime™ and aGIF decompressor
are needed to see this picture.
NADP/MDNSite
Assessment of Changes in Large-Scale Hg Signal - Phase II Analysis
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MD
NP
reci
pita
tion
Dep
th (
mm
)
0
20
40
60
80
100
120
140
0 20 40 60 80 100 120 140
Glass and SorensenPrecipitation Depth (mm)
Precipitation Depth
Comparison of Glass & Sorensen (1999) results for Ely, MN with MDN results from same site. Period of overlap is for 1/16/96 through 10/8/96 (n = 25)
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Comparison of Glass & Sorensen (1999) results for Ely, MN with MDN results from same site. Period of overlap is for 1/16/96 through 10/8/96 (n = 25)
MD
N H
g (n
g/L
)
0
20
40
60
80
100
120
0 20 40 60 80 100 120
Glass Hg (ng/L)
Hg in Wet Deposition
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0
2,000
4,000
6,000
8,000
10,000
1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000
Hg
Dep
osit
ion
(ng/
m2-
yr)
Year
Glass & Sorensen MDN
Annual Hg Deposition Rates, Ely, MN1990 - 2000
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0.0
2.0
4.0
6.0
8.0
10.0
0
20
40
60
80
100
1990 1992 1994 1996 1998 2000
SO
4 D
epos
itio
n (k
g/ha
)P
recipitation Depth (cm
)
Year
Precipitation
SO4 Deposition
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Parameter F Ratio Prob > F
Time 2.703 0.1010
Month (sin
transformed)
48.103 <0.0001
Precipitation (ln
transformed)
134.347 <0.0001
Results for ANOVA Model
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Plot of ANOVA Deposition Model Residuals vs. Time for Ely, MN. Data from Glass and Sorensen
(1999) and MDN.
m = +0.025p = 0.101
-4.00
-3.00
-2.00
-1.00
0.00
1.00
2.00
3.00
4.00
1990 1992 1994 1996 1998 2000 2002
Res
idua
l Ln
Hg
Dep
Time
DRAFT PRELIMINARY DATA SUBJECT TO CHANGE- DO NOT CITE OR QUOTE
-3.00
-2.00
-1.00
0.00
1.00
2.00
3.00
1990 1992 1994 1996 1998 2000
Res
idua
l Ln
SO
4 D
ep
Time
NADP Trend Analysis - Model Residuals vs. Time
m = -0.018p = 0.065