Shift from Atmospheric Deposition to Climatic Regulation of Sulfur - - PowerPoint PPT Presentation
Shift from Atmospheric Deposition to Climatic Regulation of Sulfur Budgets in Forested Watersheds By: Myron J. Mitchell SUNY ESF, Syracuse, NY Collaborators S. Bailey S. Kahl F. Beall G. Likens D. Burns G. Lovett D.
By:
Myron J. Mitchell SUNY‐ESF, Syracuse, NY
Sulfur atmospheric emissions have decreased in North America and Europe
1900 1990
18 4 30 10 North America Europe
YEAR Emissions Tg S yr-1
4
2‐ and NO3 ‐) result in the
mobilization of cations.
Especially important for some tree species such as sugar maple.
surface waters.
vegetation (i.e., fine roots)
Effects of Mobile Anions on Cation Leaching in Soil
Nutrients Toxic to Biota
Organic Sulfur Adsorbed Sulfate Wet Deposition Dry Deposition Sulfur Minerals Weathering Drainage Waters Losses Mineralization Immobilization Uptake Litter Inputs Adsorption Desorption
Largest S pool in most temperate forested watersheds Only important in highly weathered soils
Organic Sulfur Adsorbed Sulfate Wet Deposition Dry Deposition Sulfur Minerals Weathering Drainage Waters Losses Mineralization Immobilization Uptake Litter Inputs Adsorption Desorption Sulfur Budget Discrepancy = Atmospheric Deposition (Wet+Dry) – Drainage Water Losses
southeast Canada and the northeast United States in areas known to highly sensitive to acidification from atmospheric inputs of S.
conditions of decreasing S emissions.
amounts and types of information that can be used in evaluating sulfur budgets.
I. Northeast U.S. and Southeast Canada (15 sites from ~1985 to 2002)
(15 sites, 15 watersheds from 1984 to 2010)
New Hampshire (1 site, 4 watersheds from 1966 to 2008 )
Larger Spatial Scale Longer Period of Record
Mitchell, M.J., G. Lovett, S. Bailey, F. Beall, D. Burns,
Eimers, D. Jeffries, S. Kahl, G. Likens, M.D. Moran, C. Rogers, D. Schwede, J. Shanley, K. Weathers and R.
in Southeast Canada and Northeast US: New Approaches and Implications. Biogeochemistry103:181‐207
Selected well studied forested watershed sites with data sets on sulfur budgets.
Period
Study
SO2 Emissions Data (EPA)
Year
1900 1920 1940 1960 1980 2000
SO2 (tons x 1000)
5000 10000 15000 20000 25000 30000 35000 Regions 1-5 (East USA) Total US
1985-2002
Watershed
B i s c u i t B r
C
e P
d H B E F
6 A r b u t u s M e r s e y M
e p i t S l e e p e r s R i v e r B e a r B r
P l a s t i c L a k e H a r p L a k e H e r m i n e L a k e C l a i r T u r k e y L a k e s L a k e L a f l a m m e L a k e T i r a s s e
kg S ha-1 yr-1
10 20
Precipitation kg S ha-1 yr-1 Discharge kg S ha-1 yr-1 Difference
Without Dry Deposition
1985-2002
Watershed
B i s c u i t B r
C
e P
d H B E F
6 A r b u t u s M e r s e y M
e p i t S l e e p e r s R i v e r B e a r B r
P l a s t i c L a k e H a r p L a k e H e r m i n e L a k e C l a i r T u r k e y L a k e s L a k e L a f l a m m e L a k e T i r a s s e
kg S ha-1 yr-1
2 4 6 8
Deposition Equation 2 (CASTNET) Deposition Equation 3 (CAPMoN) Discrepancy using Equation 2 Discrepancy using Equation 3
With Dry Deposition
Contribution of Internal S Sources to Drainage Water Sulfate
Watershed
S l e e p e r s R i v e r H a r p L a k e B e a r B r
A r b u t u s C
e P
d L a k e L a f l a m m e L a k e C l a i r P l a s t i c L a k e H B E F
6 B i s c u i t B r
T u r k e y L a k e s M e r s e y L a k e T i r a s s e M
e p i t H e r m i n e
μmol SO4
2- L-1
10
Category I Category II Category III Category IV Category V Equation 2 (CASTNET) Equation 3 (CAPMoN) More sulfur is being lost than being added by atmospheric deposition when normalized for discharge
1 to 6 kg S ha‐1 year‐1
1985 ‐2002
Mitchell, M.J., C.T. Driscoll, P.J. McHale, K. M. Roy and Zheng Dong. 2012. Lake‐Watershed Sulfur Budgets and Their Response to Decreases in Atmospheric Sulfur Deposition: Watershed and Climate Controls. Hydrological Processes (in press). Sub‐objective: Extrapolate sulfur budgets to those watersheds with limited direct measurements of hydrology and S deposition.
Adirondack Mountains of New York State
SO2 Emissions Data (EPA)
Year
1900 1920 1940 1960 1980 2000
SO2 (tons x 1000)
5000 10000 15000 20000 25000 30000 35000
Mt x 1000
5000 10000 15000 20000 25000 30000 35000 40000 Regions 1-5 (East USA) Total US
Period
All Lakes (ALTM) Year
1990 2000 2010
SO4
2- μmolc L-1
50 100 150 200 250
Windfall West Otter Heart Moss Rondaxe Squash Dart Constable Cascade Bubb Black Big Moose Arbutus Little Echo Barnes Seepage Drainage
16 Watersheds
Monthly Concentrations
chemistry for all watersheds.
from Arbutus/Huntington (NADP/NTN).
across the Adirondacks of wet S deposition and discharge using formulations from Ito et al. (2002, Atmospheric Environment). See next slide for examples of spatial patterns for precipitation and S deposition in the Adirondacks.
formulations of Mitchell et al. (2011, Biogeochemistry) for each watershed.
and discharge from direct measurements at Arbutus Watershed to extrapolate temporally for all sites.
greatest to least discrepancies in S budgets as shown in the next slide.
S Budgets
Watersheds
Arbutus Black Windfall Constable Cascade Moss Otter Big Moose Dart Rondaxe Bubb Heart West Squash
kg S ha-1 yr-1
5 10 15
Total Deposition Discharge Budget Discrepancy
Arbutus
1985 1990 1995 2000 2005 2010 2 4 6 8 10 12
Total S Deposition
1985 1990 1995 2000 2005 2010
kg S ha-1 yr-1
2 4 6 8 10 12 14 16 18 20
Discharge (SO4 2-)
Year
1985 1990 1995 2000 2005 2010
2
S Budget Discrepancy
y= -0.237x + 484, r2=0.345 p=0.0013 y = -0.22x +445.2, r2=0.812 p<.0001
Regression not significant
Big Moose
1985 1990 1995 2000 2005 2010 2 4 6 8 10 12 14 16
Total S Deposition Plot 1 Regr
1985 1990 1995 2000 2005 2010
kg S ha-1 yr-1
2 4 6 8 10 12 14 16 18 20
Discharge (SO4 2-)
Year
1985 1990 1995 2000 2005 2010
2 4
S Budget Discrepancy
y= -0.295x + 601, r2=0.470 p<0.0001
Regression not significant
y = -0.29x +582.4, r2=0.806 p<.0001
Squash
1985 1990 1995 2000 2005 2010 2 4 6 8 10 12 14 16 18
Total S Deposition
1985 1990 1995 2000 2005 2010
kg S ha-1 yr-1
2 4 6 8 10 12 14 16 18
Discharge (SO4 2-)
Year
1985 1990 1995 2000 2005 2010
2 4 6
S Budget Discrepancy
y= -0.263x + 536, r2=0.444 p<0.0001
Regression not significant
y = -0.32x +655.2, r2=0.796 p<.0001
Otter Windfall West Heart Moss Rondaxe Squash Dart Constable Cascade Bubb Black Big Moose Arbutus
Drainage Lakes Discharge cm year-1 (log scale)
100
SO42- Discrepancy μmolc L-1
20 40 60
y= -88.1x + 48.8 r ²=0.473 p<0.0001 20 Windfall West Heart Moss Rondaxe Squash Dart Constable Cascade Bubb Black Big Moose Arbutus Otter
S discrepancy and volume-weighted ANC
Volume-weighted ANC (μeq/L)
50 100 150 200 250
S discrepancy (μeq/L)
5 y = -0.08x - 5.973 R² = 0.4617
Windfall West Otter Heart Moss Rondaxe Squash Dart Constable Cascade Bubb Black Big Moose Arbutus
Symbols: square: deep till; circle: medium till; triangle: thin till; inverted triangle, carbonate influenced.
Less affected by discrepancies ANC = Acid Neutralizing Capacity
Mitchell, M.J. and G.E. Likens. 2011. Watershed Sulfur Biogeochemistry: Shift from Atmospheric Deposition Dominance to Climatic Regulation. Environmental Science and Technology 45:5267‐5271 DOI: 10.1021/es200844n
Temperature and precipitation changes at the HBEF for ~50 years through 2008 from Campbell et al. (2011)
Hubbard Brook Is getting warmer and wetter within different watersheds
Long‐term trends in the annual water balance for (a) W3, (b) W6, (c) W7, and (d) W8 at the HBEF. (Campbell et al., 2011) Showing greater streamflow
SO2 Emissions Data (EPA)
Year
1900 1920 1940 1960 1980 2000
SO2 (tons x 1000)
5000 10000 15000 20000 25000 30000 35000 Regions 1-5 (East USA) Total US
Period of study
Time (year)
65 70 75 80 85 90 95 00 05
SO4
2- in discharge (μmol L-1)30 40 50 60 70 80
a. b.
1970 1980 1990 2000 5 10 15 20 25
Total Atmospheric Deposition Regression
1970 1980 1990 2000
kg S ha-1 yr-1
5 10 15 20 25 30
Discharge (SO4 2-) Regression
Year
1970 1980 1990 2000
2 4
Sulfur Budget Discrepancy Regressiony = -0.238x + 484 r2= 0.824 p = 0.001 y = -0.143x + 300 r2 = 0.218 p = 0.001 y = -0.094x + 184 r2 = 0.180 p = 0.04
a. b. c.
Watershed 6
‐
Soil Moisture Stream discharge
Soil Moisture
SO4
2‐
Desorption Soil Moisture Organic S Mineralization Soil Moisture Soil Moisture S Mineral Weathering Reduced S
Conceptual diagram showing the relationships between water availability and SO4
2‐
generation from various internal S sources in a watershed. All four internal S sources are predicted to show increases in SO4
2‐ mobilization with greater water availability as
predicted with climate change in the Northeast US.
Increasing contribution
Annual Discharge (mm) SO4
2- μmol L-1 Discrepancy
10 20 Watershed 1 Watershed 3 Watershed 5 Watershed 6 y = -48.2log10x + 130 r ² = 0.573 p<0.0001
500 1000 631 1260 794 1590
Atmospheric deposition of sulfur has shown a marked decline in southeastern Canada and the northeastern U.S. The decline in deposition has resulted in decreased concentrations of sulfate in surface waters (soils). There is a legacy of previously deposited sulfur that is being mobilized.
This mobilized sulfur may delay the recovery of ecosystems from the deleterious impacts of acidic deposition. For the Adirondacks those watersheds with greatest amount of internal S sources also have the highest capacity for buffering acidity and hence recovery from acidification. The mobilization of sulfate is closely coupled to watershed hydrology and hence climate change.
sources that will affect recovery from acidification?
greatest internal S sources also have the greatest ability to buffer acidity?
wetness effect the biogeochemistry of other important elements including calcium, nitrogen, aluminum, etc.?
This research was sponsored in part by the National Science Foundation (Ecosystem Studies), USDA Forest Service, York State Energy Research and Development Authority (NYSERDA), the Andrew W. Mellon Foundation, Environment Canada, Fonds de Recherche sur la nature et les technologuies (FQRNT) du Québec, National Resources Canada, Natural Sciences and Engineering Research Council (NSERC) of Canada, New York City Dept. of Environmental Protection, Northeast Ecosystem Research Cooperative (NERC), Ontario Ministry of Environment, US E.P.A., and US Geological Survey.