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Comparisons of watershed sulfur budgets in southeast Canada and northeast US: new approaches and implications

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Abstract

Most of eastern North America receives elevated levels of atmospheric deposition of sulfur (S) that result from anthropogenic SO2 emissions from fossil fuel combustion. Atmospheric S deposition has acidified sensitive terrestrial and aquatic ecosystems in this region; however, deposition has been declining since the 1970s, resulting in some recovery in previously acidified aquatic ecosystems. Accurate watershed S mass balances help to evaluate the extent to which atmospheric S deposition is retained within ecosystems, and whether internal cycling sources and biogeochemical processes may be affecting the rate of recovery from decreasing S atmospheric loads. This study evaluated S mass balances for 15 sites with watersheds in southeastern Canada and northeastern US for the period 1985 to 2002. These 15 sites included nine in Canada (Turkey Lakes, ON; Harp Lake, ON; Plastic Lake, ON; Hermine, QC; Lake Laflamme, QC; Lake Clair, QC; Lake Tirasse, QC; Mersey, NS; Moosepit, NS) and six in the US (Arbutus Lake, NY; Biscuit Brook, NY; Sleepers River, VT; Hubbard Brook Experimental Forest, NH; Cone Pond, NH; Bear Brook Watershed, ME). Annual S wet deposition inputs were derived from measured bulk or wet-only deposition and stream export was obtained by combining drainage water fluxes with SO4 2− concentrations. Dry deposition has the greatest uncertainty of any of the mass flux calculations necessary to develop accurate watershed balances, and here we developed a new method to calculate this quantity. We utilized historical information from both the US National Emissions Inventory and the US (CASTNET) and the Canadian (CAPMoN) dry deposition networks to develop a formulation that predicted SO2 concentrations as a function of SO2 emissions, latitude and longitude. The SO2 concentrations were used to predict dry deposition using relationships between concentrations and deposition flux derived from the CASTNET or CAPMoN networks. For the year 2002, we compared the SO2 concentrations and deposition predictions with the predictions of two continental-scale air quality models, the Community Multiscale Air Quality (CMAQ) model and A Unified Regional Air-quality Modeling System (AURAMS) that utilize complete inventories of emissions and chemical budgets. The results of this comparison indicated that the predictive relationship provides an accurate representation of SO2 concentrations and S deposition for the region that is generally consistent with these models, and thus provides confidence that our approach could be used to develop accurate watershed S budgets for these 15 sites. Most watersheds showed large net losses of SO4 2− on an annual basis, and the watershed mass balances were grouped into five categories based on the relative value of mean annual net losses or net gains. The net annual fluxes of SO4 2− showed a strong relationship with hydrology; the largest net annual negative fluxes were associated with years of greatest precipitation amount and highest discharge. The important role of catchment hydrology on S budgets suggests implications for future predicted climate change as it affects patterns of precipitation and drought. The sensitivity of S budgets is likely to be greatest in watersheds with the greatest wetland area, which are particularly sensitive to drying and wetting cycles. A small number of the watersheds in this analysis were shown to have substantial S sources from mineral weathering, but most showed evidence of an internal source of SO4 2−, which is likely from the mineralization of organic S stored from decades of increased S deposition. Mobilization of this internal S appears to contribute about 1–6 kg S ha−1 year−1 to stream fluxes at these sites and is affecting the rate and extent of recovery from acidification as S deposition rates have declined in recent years. This internal S source should be considered when developing critical deposition loads that will promote ecosystem recovery from acidification and the depletion of nutrient cations in the northeastern US and southeastern Canada.

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References

  • Aherne JM, Futter MN, Dillon PJ (2008) The impacts of future climate change and sulphur emission reductions on acidification recovery at Plastic Lake, Ontario. Hydrol Earth Syst Sci 12:383–392

    Google Scholar 

  • Alewell C, Gehre M (1999) Patterns of stable S isotopes in a forested catchment as indicators for biological S turnover. Biogeochemistry 47:319–333

    Google Scholar 

  • Alewell C, Manderscheid B, Lükewille A et al (1996) Describing SO4 2-dynamics in the Solling roof project with two different modelling approaches. Water Air Soil Pollut 85:1806–1810

    Google Scholar 

  • Alewell C, Mitchell M, Likens GE et al (1999) Sources of stream sulfate at the Hubbard Brook Experimental Forest: long-term analysis using stable isotopes. Biogeochemistry 44:281–299

    Google Scholar 

  • Alewell C, Mitchell M, Likens GE et al (2000) Assessing the origin of sulfate deposition at the Hubbard Brook Experimental Forest. J Environ Qual 29:759–767

    Google Scholar 

  • Appel KW, Roselle SJ (2009) Evaluation of CMAQ v4.7 sulfate predictions for 2002-2006. In: 8th annual community modeling and analysis (CMAS) conference, Chapel Hill, NC

  • Bailey SW, Mayer B, Mitchell MJ (2004) Evidence for the influence of mineral weathering on stream water sulphate in Vermont and New Hampshire. Hydrol Proc 18:1639–1653

    Google Scholar 

  • Bailey SW, Horsley SB, Long RP (2005) Thirty years of change in forest soils of the Allegheny Plateau, Pennsylvania. Soil Sci Soc Am J 69:681–690

    Google Scholar 

  • Baumgardner RE, Lavery TF, Rogers CM et al (2002) Estimates of the atmospheric deposition of sulfur and nitrogen species: Clean Air Status and Trends Network, 1990–2000. Environ Sci Technol 36:2614–2629

    Google Scholar 

  • Baumgardner RE, Isil SS, Lavery TF et al (2003) Estimates of cloud water deposition at mountain acid deposition program sites in the Appalachian Mountains. J Air Waste Manage Assoc 53:291–308

    Google Scholar 

  • Beall FD, Semkin RG, Jeffries DS (2001) Trends in the output of first-order basins at Turkey Lakes Watershed, 1982–96. Ecosystems 4:514–526

    Google Scholar 

  • Bélanger N, Courchesne F, Côté B et al (2002) Simulation of soil chemistry and nutrient availability in a forested ecosystem of southern Quebec. Part II. Application of the SAFE model. Environ Model Softw 17:447–465

    Google Scholar 

  • Biron P, Roy AG, Courchesne F et al (1999) The effects of antecedent moisture conditions on the relationship of hydrology to hydrochemistry in a small forested watershed. Hydrol Proc 13:1541–1555

    Google Scholar 

  • Brook JR, Zhang L, Li Y et al (1999) Description and evaluation of a model of deposition velocities for routine estimates of dry deposition over North America. Part II: review of past measurements and model results. Atmos Environ 33:5053–5070

    Google Scholar 

  • Burns DA, Blett T, Haeuber R, Pardo LH (2008) Critical loads as a policy tool for protecting ecosystems from the effects of air pollutants. Front Ecol Environ 6:156–159

    Google Scholar 

  • Butler TJ, Likens GE, Stunder BJB (2001) Regional-scale impacts of Phase I of the Clean Air Act Amendments in the USA: the relation between emissions and concentrations, both wet and dry. Atmos Environ 35:1015–1028

    Google Scholar 

  • Byun DW, Schere KL (2006) Review of the governing equations, computational algorithms, and other components of the models-3 community multiscale air quality (CMAQ) modeling system. Applied mechanics reviews. Am Soc Mech Eng 59(2):51–77

    Google Scholar 

  • Campbell JL, Mitchell MJ, Mayer B (2006) Isotopic assessment of NO3 − and SO4 2− mobility during winter in two adjacent watersheds in the Adirondack Mountains, New York. J Geophys Res 111:G04007. doi:10.1029/2006JG000208

    Google Scholar 

  • Campbell JL, Rustad LE, Boyer EW et al (2009) Consequences of climate change for biogeochemical cycling in forests of northeastern North America. Can J For Res 39:264–284

    Google Scholar 

  • Canada-United States Air Quality Agreement: 1992 Progress report. ISBN:0-662-19759-3, 79 pp. http://www.ec.gc.ca/pdb/can_us/qual/1992/english/index_e.html

  • Canada-United States Air Quality Agreement: 2008 Progress report. ISSN 1487-1033, ISBN: 978-1-100-10516-1, 72 pp. http://www.ec.gc.ca/cleanair-airpur/83930AC3-60EE-4A14-A241-A10A83D3B055/US_Canada_2008_En_web.pdf

  • Chen L, Driscoll CT, Gbondo-Tugbawa S et al (2004) The application of an integrated biogeochemistry model (PnET-BGC) to five forested watersheds in the Adirondack and Catskill Regions of New York. Hydrol Proc 18:2631–2650

    Google Scholar 

  • Church MR, Thornton KW, Shaffer PW et al (1989) Direct/delayed response project: future effects of long term sulfur deposition on surface water chemistry in the northeastern and southern Blue Ridge province. In: EPA/600/3-89/061. U.S. Environmental Protection Agency, Washington, DC

  • Church MR, Shaffer PW, Thornton KW et al (1992) Direct/delayed response project: future effects of long term sulfur deposition on stream chemistry in the mid-Appalachian region of the eastern United States. In: EPA/600/R-92/186. U.S. Environmental Protection Agency, Washington, DC

  • Clair TA, Dillon PJ, Ion J et al (1995) Regional precipitation and surface water chemistry trends in southeastern Canada (1983–1991). Can J Fish Aquat Sci 52(1):197–212

    Google Scholar 

  • Clarke JF, Edgerton ES, Martin BE (1997) Dry deposition calculations for the CASTNET. Atmos Environ 31:3667–3678

    Google Scholar 

  • Cosby BJ, Ryan PF, Webb JR (1991) Mountains of western Virginia. In: Charles DF et al (eds) Acidic deposition and aquatic ecosystems: regional case studies. Springer-Verlag, New York

    Google Scholar 

  • Courchesne F (1992) Relationships between soil chemical properties and sulfate sorption kinetics in Podzolic soils from Quebec. Can J Soil Sci 72:467–480

    Google Scholar 

  • Courchesne F, Hendershot WH (1990) The role of basic aluminum sulfate minerals in controlling sulfate retention in acid forest soils in Quebec. Soil Sci 150:571–578

    Google Scholar 

  • Courchesne F, Côté B, Fyles J et al (2005) Recent changes in soil chemistry in a forested ecosystem of southern Québec, Canada. Soil Sci Soc Am J 69:1298–1313

    Google Scholar 

  • Creed IF, Band LE (1998) Export of nitrogen from catchments within a temperate forest: evidence for a unifying mechanism regulated by variable source area dynamics. Water Resour Res 34:3079–3093

    Google Scholar 

  • David MB, Fuller RD, Fernandez IJ et al (1990) Spodosol variability and assessment of response to acidification. Soil Sci Soc Am J 54:541–548

    Google Scholar 

  • Dennis I, Clair T, Driscoll C et al (2005) Distribution patterns of mercury in lakes and rivers of Northeastern North America. Ecotoxicology 14:113–123

    Google Scholar 

  • Dillon PJ, LaZerte BD (1992) Response of the Plastic Lake catchment, Ontario, to reduced sulphur deposition. Environ Pollut 77:211–217

    Google Scholar 

  • Driscoll CT, Postek KM (1996) The chemistry of aluminum in surface waters. In: Sposito G (ed) The environmental chemistry of aluminum. CRC, Boca Raton, pp 363–418

    Google Scholar 

  • Driscoll CT, Likens GE, Church MR (1998) Recovery of surface waters in the northeastern U.S. from decreases in atmospheric deposition of sulfur. Water Air Soil Pollut 105:319–329

    Google Scholar 

  • Driscoll CT, Lawrence G, Bulger A et al (2001) Acidic deposition in the northeastern US: sources, inputs, ecosystem effects, and management strategies. BioScience 51:180–198

    Google Scholar 

  • Driscoll CT, Driscoll KM, Roy KM et al (2003) Chemical response of lakes in the Adirondack region to declines in acidic deposition. ES&T 37:2036–2042

    Google Scholar 

  • Duchesne L, Houle D (2006) Base cation cycling in a pristine watershed of the Canadian boreal forest. Biogeochemistry 78:195–216

    Google Scholar 

  • Dupont J, Clair TA, Gagnon C et al (2005) Estimation of critical loads of acidity for lakes in northeastern United States and eastern Canada. Envir Monit Assess 109:275–291

    Google Scholar 

  • Eaton JS, Likens GE, Bormann FH (1978) The input of gaseous and particulate sulfur to a forest ecosystem. Tellus 30:546–551

    Google Scholar 

  • Eimers MC, Dillon PJ (2002) Climate effects on sulphate export from forested catchments in south-central Ontario, Canada. Biogeochemistry 61:355–367

    Google Scholar 

  • Eimers C, Houle D (2005) Sources, transport and fate of S in Canadian watersheds. In: Houle D (ed) Effects on forests and soils. Chapter 5 Canadian acid deposition science assessment, 2004. Environment Canada, Ottawa, pp 168–173

    Google Scholar 

  • Eimers MC, Dillon PJ, Schiff SL (2004a) A S isotope approach to determine the relative contribution of redox processes to net SO4 export from upland and wetland dominated catchments. Geochim Cosmochim Acta 68:3665–3674

    Google Scholar 

  • Eimers MC, Dillon PJ, Schiff SL (2004b) Sulphate flux from an upland forested catchment in south-central Ontario, Canada. Water Air Soil Pollut 152:3–21

    Google Scholar 

  • Eimers MC, Dillon PJ, Watmough SA (2004c) Long-term (18-year) changes in sulphate concentrations in two Ontario headwater lakes and their inflows in response to decreasing deposition and climate variations. Hydol Proc 18:2617–2630

    Google Scholar 

  • Eimers MC, Watmough SA, Buttle JM et al (2007) Drought-induced sulphate release from a wetland in south-central Ontario. Environ Monit Assess 127:399–407

    Google Scholar 

  • Eimers MC, Buttle JM, Watmough SA (2008) Influence of seasonal changes in runoff and extreme events on dissolved organic carbon trends in wetland- and upland-draining streams. Can J Fish Aquat Sci 65:796–808

    Google Scholar 

  • EPA (2009) Risk and exposure assessment for review of the secondary national ambient air quality standards for oxides of nitrogen and oxides of sulfur. EPA-452/R-09-008a

  • Faseth WJ, David MB, Vance GF (1991) Sulfate retention and cation leaching of forest soils in response to acid additions. Can J For Res 21:32–41

    Google Scholar 

  • Fernandez IJ, Rustad LE, Norton SA et al (2003) Experimental acidification causes soil base cation depletion in a New England forested watershed. Soil Sci Soc Am J 67:1909–1919

    Google Scholar 

  • Finkelstein PL, Ellestad TG, Clarke JF et al (2000) Ozone and sulfur dioxide dry deposition to forests: observations and model evaluation. J Geophys Res Atmos 105:15365–15377

    Google Scholar 

  • Fowler D, Smith R, Muller J et al (2007) Long term trends in sulphur and nitrogen deposition in Europe and the cause of non-linearities. Water Air Soil Pollut 7:41–47

    Google Scholar 

  • Gauci V, Dise NB, Howell G et al (2008) Suppression of rice methane emission by sulfate deposition in simulated acid rain. J Geophys Res 113:G00A07. doi:10.1029/2007JG000501

  • Gbondo-Tugbawa SS, Driscoll CT, Mitchell MJ et al (2002) A model to simulate the response of a northern hardwood forest ecosystem to changes in S deposition. Ecol Appl 12:8–23

    Google Scholar 

  • Gélineau M, Carignan R, Tessier A (1989) Study of the transit of sulfate in a Canadian Shield lake watershed with stable oxygen isotope ratios. Appl Geochem 4:195–201

    Google Scholar 

  • Gilmour CC, Henry EA, Mitchell R (1992) Sulfate stimulation of mercury methylation in freshwater sediments. ES&T 26:2281–2287. doi:10.1021/es00035a029

    Google Scholar 

  • Haines B, Black M, Bayer C (1989) Sulfur emissions from roots of the rain forest tree Stryphnodendron excelsum. In: Saltzman ES, Cooper WJ (eds) Biogenic sulfur in the environment. A.C.S. symposium series 393, Washington, DC, pp 58–69

  • Hall J, Reynolds B, Langan S, Hornung M, et al. (2001) Investigating the uncertainties in the simple mass balance equation for acidity critical loads for terrestrial ecosystems in the United Kingdom. Water Air Soil Pollut Focus 1:43–56

    Google Scholar 

  • Harrison RB, Johnson DW, Todd DE (1989) Sulfate adsorption and desorption reversibility in a variety of forest soils. J Environ Qual 18:419–426

    Google Scholar 

  • Hicks BB, Baldocchi DD, Meyers TP et al (1987) A preliminary multiple resistance routine for deriving dry deposition velocities from measured quantities. Water Air Soil Pollut 36:311–330

    Google Scholar 

  • Hicks BB, Hosker RP, Meyers TP et al (1991) Dry deposition inferential measurement techniques. I. Design and tests of a prototype meteorological and chemical system for determining dry deposition. Atmos Environ 25:2345–2359

    Google Scholar 

  • Houle D, Carignan R (1992) Sulfur distribution and speciation in soils and aboveground biomass of a boreal coniferous forest. Biogeochemistry 16:63–82

    Google Scholar 

  • Houle D, Carignan R (1995) Role of SO4 adsorption and desorption in the long-term S budget of a coniferous catchment on the Canadian Shield. Biogeochemistry 28:162–182

    Google Scholar 

  • Houle D, Paquin R, Camiré C et al (1997) Response of the Lake Clair Watershed (Duchesnay, Québec) to change in precipitation chemistry (1988–1994). Can J For Res 27:1813–1821

    Google Scholar 

  • Houle D, Carignan R, Ouimet R (2001) Soil organic sulfur dynamics in a coniferous forest. Biogeochemistry 53:105–124

    Google Scholar 

  • Houle D, Gagnon C, Couture S et al (2004) Recent recovery of lake water quality in southern Quebec following reductions in sulfur emissions. Water Air Soil Pollut Focus 4:247–261

    Google Scholar 

  • Huntington TG, Hooper RP, Aulenbach BT (1994) Hydrologic processes controlling sulfur mobility: a small watershed approach. Water Resour Res 30:283–295

    Google Scholar 

  • Huntington TG, Richardson AD, McGuire K et al (2009) Climate and hydrological changes in the northeastern United States: recent trends and implications for forested and aquatic ecosystems. Can J For Res 39:199–212

    Google Scholar 

  • Inamdar SP, Christopher SF, Mitchell MJ (2004) Export mechanisms for dissolved organic carbon and nitrate during summer storm events in a glaciated forested catchment in New York, USA. Hydrol Proc 18:2651–2661

    Google Scholar 

  • IPCC (2001) Chapter 4. Atmospheric chemistry and greenhouse gases. In: Houghton JT, Ding Y, Griggs DJ, Noguer M, van der Linden PJ, Dai X, Johnson CA, Maskell K (eds) Climate change 2001: a scientific basis, intergovernmental panel on climate change. Cambridge University Press, Cambridge

  • Ito M, Mitchell MJ, Driscoll CT (2002) Spatial patterns of precipitation quantity and chemistry and air temperature in the Adirondack Region of New York. Atmos Environ 36:1051–1062

    Google Scholar 

  • Jeffries DS, Ouimet R (eds) (2005) Chapter 8: Critical loads—are they being exceeded? In: 2004 Canadian acid deposition science assessment, Environment Canada, Ottawa, ON, pp 341-368. http://www.msc-smc.ec.gc.ca/saib/acid/assessment2004/pg41_e.html#1

  • Jeffries DS, Kelso JRM, Morrison IK (1988) Physical, chemical, and biological characteristics of the Turkey Lakes watershed, central Ontario. Can J Fish Aquat Sci 45(Suppl 1):3–12

    Google Scholar 

  • Jeffries DS, Clair TA, Couture S et al (2003a) Assessing the recovery of lakes in southeastern Canada from the effects of acidic deposition. Ambio 32:176–182

    Google Scholar 

  • Jeffries DS, Brydges TG, Dillon PJ et al (2003b) Monitoring the results of Canada/U.S.A. acid rain control programs: some lake responses. Environ Monit Assess 88:3–19

    Google Scholar 

  • Johnson DW, Mitchell MJ (1998) Responses of forest ecosystems to changing sulfur inputs. In: Maynard D (ed) Sulfur in the environment. Marcel Dekker, Inc, New York, pp 219–262

    Google Scholar 

  • Johnson DW, Henderson GS, Huff DD et al (1982) Cycling of organic and inorganic sulphur in a chestnut oak forest. Oecologia 54:141–148

    Google Scholar 

  • Khana P, Prenzel J, Meiwes KJ et al (1987) Dynamics of sulfate retention by acid forest soils in an acidic environment. Soil Sci Soc Am J 51:446–452

    Google Scholar 

  • LaZerte BD (1993) The impact of drought and acidification on the chemical exports from a minerotrophic conifer swamp. Biogeochemistry 18:153–175

    Google Scholar 

  • Likens GE, Bormann FH (1995) Biogeochemistry of a forested ecosystem, 2nd edn. Springer-Verlag, New York, pp 159

  • Likens GE, Bormann FH, Hedin LO et al (1990) Dry deposition of sulfur: a 23-yr record for the Hubbard Brook Forest Ecosystem. Tellus 42B:319–329

    Google Scholar 

  • Likens GE, Driscoll CT, Buso DC (1996) Long-term effects of acid rain: response and recovery of a forest ecosystem. Science 272:244–246

    Google Scholar 

  • Likens GE, Driscoll CT, Buso DC et al (1998) The biogeochemistry of calcium at Hubbard Brook. Biogeochemistry 41:89–173

    Google Scholar 

  • Likens GE, Butler TJ, Buso DC (2001) Long- and short-term changes in sulfate deposition: effects of the 1990 Clean Air Act Amendments. Biogeochemistry 52:1–11

    Google Scholar 

  • Likens GE, Driscoll CT, Buso DC et al (2002) The biogeochemistry of sulfur at Hubbard Brook. Biogeochemistry 60:235–316

    Google Scholar 

  • Likens GE, Buso DC, Butler TJ (2005) Long-term relationships between SO2 and NOX emissions and SO4 2− and NO3 − concentration in bulk deposition at the Hubbard Brook Experimental Forest, New Hampshire. J Environ Monit 7(10):964–968

    Google Scholar 

  • Lovett GM (1984) Rates and mechanisms of cloud water deposition to a sub-alpine balsam fir forest. Atmos Environ 18:361–371

    Google Scholar 

  • Lovett GM (1994) Atmospheric deposition of nutrients and pollutants in North-America—an ecological perspective. Ecol Appl 4:629–650

    Google Scholar 

  • Lovett GM, Reiners WA, Olsen RK (1982) Cloud droplet deposition in sub-alpine balsam fir forests: hydrological and chemical inputs. Science 218:1303–1304

    Google Scholar 

  • Lükewille A, Malessa V, Alewell C (1996) Measured and modelled retention of inorganic sulfur in soils and bedrock (Harz Mountains, Germany). Water Air Soil Pollut 85:683–688

    Google Scholar 

  • Lynch JA, Bowersox VC, Grimm JW (1996) Trends in precipitation chemistry in the United States, 1983-94: an analysis of the effects in 1995 of phase I of the Clean Air Act Amendments of 1990, Title IV U.S. Geological Survey USGS 96-0346, Washington, DC, June 1996

  • Lynch JA, Bowersox VC, Grimm JW (2000) Changes in sulfate deposition in eastern USA following implementation of Phase I of Title IV of the Clean Air Act Amendments of 1990. Atmos Environ 34:1665–1680

    Google Scholar 

  • Martin CW, Likens GE, Buso DC (2000) Comparison of long-term precipitation chemistry measurements at the Hubbard Brook Experimental Forest, New Hampshire. Water Air Soil Pollut 120(3–4):359–379

    Google Scholar 

  • Mayer B, Feger KH, Gieseman A et al (1995) Interpretation of sulfur cycling in two catchments in the Black Forest (Germany) using stable sulfur and oxygen isotope data. Biogeochemistry 30:51

    Google Scholar 

  • Meyers TP, Finkelstein P, Clarke J et al (1998) A multilayer model for inferring dry deposition using standard meteorological measurements. J Geophys Res Atmos 103:22645–22661

    Google Scholar 

  • Mitchell MJ, Alewell C (2007) Sulfur transformations and fluxes. In: Chesworth W (ed) The encyclopedia of soil science. Springer-Verlag, Dordrecht, pp 757–764

    Google Scholar 

  • Mitchell MJ, David MB, Maynard DG et al (1986) Sulfur constituents in soils and streams of a watershed in the Rocky Mountains of Alberta. Can J For Res 16:315–320

    Google Scholar 

  • Mitchell MJ, Driscoll CT, Fuller RD et al (1989) Effect of whole-tree harvesting on the sulfur dynamics of a forest soil. Soil Sci Soc Am J 53:933–940

    Google Scholar 

  • Mitchell MJ, David MB, Harrison RB (1992a) Sulfur dynamics of forest ecosystems. In: Howarth RW, Stewart JWB, Ivanov MV (eds) Sulfur cycling on the continents. SCOPE vol 48. Wiley, New York

  • Mitchell MJ, Foster NW, Shepard JP et al (1992b) Nutrient cycling in Huntington Forest and Turkey Lakes deciduous stands: nitrogen and sulfur. Can J For Res 22:457–464

    Google Scholar 

  • Mitchell MJ, Mayer B, Bailey SW et al (2001a) Use of stable isotope ratios for evaluating sulfur sources and losses at the Hubbard Brook Experimental Forest. In: Proceedings of acid rain 2000, Japan. Water Air Soil Pollut 130:75–86

  • Mitchell MJ, McHale PJ, Inamdar S et al (2001b) Role of within lake processes and hydrobiogeochemical changes over 16 years in a watershed in the Adirondack Mountains of New York State, U.S.A. Hydrol Proc 15:1951–1965

    Google Scholar 

  • Mitchell MJ, Piatek KB, Christopher S et al (2006) Solute sources in stream water during consecutive fall storms in a northern hardwood forest watershed: a combined hydrological, chemical and isotopic approach. Biogeochemistry 78:217–246

    Google Scholar 

  • Mitchell MJ, Bailey SW, Shanley JB et al (2008) Evaluating storm events for three watersheds in the Northeastern United States: a combined hydrological, chemical and isotopic approach. Hydrol Proc 22:4023–4034

    Google Scholar 

  • Moldan B, Cerny J (eds) (1995) Biogeochemistry of small catchments: a tool for environmental research. SCOPE 51. Wiley, Chichester, 419 pp

  • Moran MD, Zheng Q, Pavlovic R et al (2008) Predicted acid deposition critical-load exceedances across Canada from a one-year simulation with a regional particulate-matter model. In: Proceedings of the 15th joint AMS/A&WMA conference on applications of air pollution meteorology, Jan 21–24, New Orleans, American Meteorological Society, Boston, 20 pp. Available from weblink http://ams.confex.com/ams/pdfpapers/132916.pdf

  • Morrison IK, Foster NW (2001) Fifteen-year change in forest floor organic and element content and cycling at the Turkey Lakes Watershed. Ecosystems 4:545–555

    Google Scholar 

  • Morrison IK, Foster NW, Nicolson JA (1992) Influence of acid deposition on element cycling in mature sugar maple forest, Algoma, Canada. Water Air Soil Pollut 61:243–252

    Google Scholar 

  • Murdoch PS, Shanley JB (2006) Detection of water quality trends at high, median, and low flow in a Catskill Mountain stream, New York, through a new statistical method. Water Resour Res 42:W08407. doi:10.1029/2004WR003892

  • Nilsson J, Grennfelt P (1988) Critical loads for sulphur and nitrogen: report from a workshop held at Stockloster, Sweden, 19–24 March 1988. Miljorapport 15, Nordic Council of Ministers, 418 pp

  • Nodvin SC, Driscoll CT, Likens GE (1986) The effect of pH on sulfate adsorption in a forest soil. Soil Sci 142:69–75

    Google Scholar 

  • Nordstrom SA (1982) The effect of sulfate on aluminum concentrations in natural waters: stability relations in the system Al2O3–SO3–H2O at 298 K. Geochim Cosmochim Acta 46:681–692

    Google Scholar 

  • Norton SA, Fernandez IJ (eds) (1999) The Bear Brook Watershed in Maine (BBWM)—a paired watershed experiment: the first decade (1987–1997). Kluwer Publication, Special Volume (55) of Environ Monit Assess

  • Novák M, Kirchner JW, Fottova D et al (2005) Isotopic evidence for processes of sulfur retention/release in 13 forested catchments spanning a strong pollution gradient (Czech Republic, Central Europe). Global Biogeochem Cycles 19: Art No GB4012

  • Novák M, Mitchell MJ, Jacková I et al (2007) Processes affecting oxygen isotope ratios of atmospheric and ecosystem sulfate in two contrasting forest catchments in Central Europe. ES&T 41:703–709. doi:10.1021/es0610028

    Google Scholar 

  • Ouimet R, Arp PA, Watmough SA et al (2006) Determination and mapping critical loads of acidity and exceedances for upland forest soils in Eastern Canada. Water Air Soil Pollut 172:57–66

    Google Scholar 

  • Park J, Mitchell MJ, McHale PJ et al (2003) Interactive effects of changing climate and atmospheric deposition on N and S biogeochemistry in a forested watershed of the Adirondack Mountains, New York State. Global Change Biol 9:1602–1619

    Google Scholar 

  • Piatek KB, Christopher SF, Mitchell MJ (2009) Spatial and temporal dynamics of stream chemistry in a forested watershed. Hydrol Earth Syst Sci 13:423–439

    Google Scholar 

  • Pleim JE, Xiu A, Finkelstein PL et al (2001) A coupled land-surface and dry deposition model and comparison to field measurements of surface heat, moisture, and ozone fluxes. Water Air Soil Pollut Focus 1:243–252

    Google Scholar 

  • Porter E, Blett T, Potter DU, Huber C (2005) Protecting resources on federal lands: implications of critical loads for atmospheric deposition of nitrogen and sulfur. Bioscience 55:603–612

    Google Scholar 

  • Prechtel A, Alewell C, Armbruster M et al (2001) Response of sulphur dynamics in European catchments to decreasing sulphate deposition. Hydrol Earth Syst Sci 5:311–325

    Google Scholar 

  • Reuss JO, Johnson DW (1986) Acid deposition and acidification of soils and waters. Springer-Verlag, New York, p 119

  • Richter DD, Lindberg SE (1988) Wet deposition estimates from long-term bulk and event wet-only samples of incident precipitation and throughfall. J Environ Qual 17:619–622

    Google Scholar 

  • Rochelle BP, Church MR, David MB (1987) Sulfur retention at intensively studied sites in the U.S. and Canada. Water Air Soil Pollut 33:73–83

    Google Scholar 

  • Schiff SL, Spoestra J, Semkin RG et al (2005) Drought induced pulses of SO4 2− from a Canadian shield wetland: use of 34S and 18O in SO4 2− to determine sources of sulfur. Appl Geochem 20:691–700

    Google Scholar 

  • Seip HM, Seip R, Dillon PJ et al (1985) Model of sulphate concentration in a small stream in the Harp Lake catchment, Ontario. Can J Fish Aquat Sci 42:927–937

    Google Scholar 

  • Shanley JB, Mayer B, Mitchell MJ et al (2005) Tracing sources of streamwater sulfate during snowmelt using S and O isotope ratios of sulfate and 35S activity. Biogeochemistry 76:161–185

    Google Scholar 

  • Shanley JB, Mayer B, Mitchell MJ et al (2008) Annual and event variations in 34S values of stream sulfate in a Vermont forested catchment: implications for S sources and cycling. Sci Total Environ 604:262–268

    Google Scholar 

  • Shepard JP, Mitchell MJ, Scott TJ et al (1989) Measurements of wet and dry deposition in a northern hardwood forest. Water Air Soil Pollut 48:225–238

    Google Scholar 

  • Sickles JE, Grimm JW (2003) Wet deposition from clouds and precipitation in three high-elevation regions of the Eastern United States. Atmos Environ 37:277–288

    Google Scholar 

  • Sickles JE, Shadwick DS (2007) Changes in air quality and atmospheric deposition in the eastern United States: 1990–2004. J Geophys Res 112:D17301. doi:10.1029/2006JD007843

    Google Scholar 

  • Smyth SC, Jiang W, Roth H et al (2007) A comparative performance evaluation of the AURAMS and CMAQ air quality modelling systems—revised, National Research Council, Ottawa, ON, Canada. ICPET technical report. PET-1577-07S, 114 pp

  • Smyth SC, Jiang W, Roth H et al (2008) A comparative performance evaluation of the AURAMS and CMAQ air quality modelling systems. Atmos Environ 43:1059–1070

    Google Scholar 

  • Staelens J, De Schrijver A, Van Avermaet P et al (2005) A comparison of bulk and wet-only deposition at two sites in Melle (Belgium). Atmos Environ 39:7–15

    Google Scholar 

  • Stam AC, Mitchell MJ, Krouse HR et al (1992) Dynamics of stable sulfur isotopes of sulfate in precipitation and stream solutions in a northern hardwoods watershed. Water Resour Res 28:231–236

    Google Scholar 

  • Stoddard JL, Murdoch PS (1991) Catskill mountains. In: Charles DF (ed) Acidic deposition and aquatic ecosystems. Springer-Verlag New York Inc, New York, pp 237–271

    Google Scholar 

  • Stoddard JL, Jeffries DS, Lukewille A et al (1999) Regional trends in aquatic recovery from acidification in North America and Europe. Nature 401:575–577

    Google Scholar 

  • Stoddard JL, Kahl JS, Deviney F et al (2003) Response of surface water chemistry to the Clean Air Act Amendments of 1990. EPA/620/R-03/001, U.S. Environmental Protection Agency, Corvallis, OR

  • Sullivan TJ, Cosby BJ (2005) Testing, improvement, and confirmation of a watershed model of acid-base chemistry. Water Air Soil Pollut 85:2607–2612

    Google Scholar 

  • Sullivan TJ, Fernandez IJ, Herlithy AT et al (2006) Acid-base characteristics of soil in the Adirondack Mountains, New York. Soil Sci Soc Am J 70:141–152

    Google Scholar 

  • Sverdrup H, de Vries W (1994) Calculating critical loads for acidity with the simple mass balance equation. Water Air Soil Pollut 72:143–162

    Google Scholar 

  • Vet R, Ro C-U (2008) Contribution of Canada–United States transboundary transport to wet deposition of sulphur and nitrogen oxides—a mass balance approach. Atmos Environ 42:2518–2529

    Google Scholar 

  • Vet R, Lear G, Narayan J et al (2005) Sulfur and nitrogen deposition across eastern North America. In: Abstract from Ecological Society of America meeting, August 9, 2005. Montreal, Canada

  • Watmough SA, Aherne J, Alewell C et al (2005) Sulphate, nitrogen and base cation budgets at 21 forested catchments in Canada, the United States and Europe. Environ Monit Assess 109:1–36

    Google Scholar 

  • Weathers KC, Lovett GM (1998) Acid deposition research and ecosystem science: synergistic successes. In: Pace ML, Groffman PM (eds) Successes, limitations, and frontiers in ecosystem science VII Cary conference. Springer-Verlag, New York, pp 195–219

    Google Scholar 

  • Weathers KC, Lovett GM, Likens GE (1995) Cloud deposition to a spruce forest edge. Atmos Environ 29:665–672

    Google Scholar 

  • Weathers KC, Lovett GM, Likens GE et al (2000) The effect of landscape features on deposition to Hunter Mountain, Catskill Mountains, New York. Ecol Appl 10:528–540

    Google Scholar 

  • Weathers KC, Butler TJ, Likens GE (2006a) Acid rain. In: Rom WN (ed) Environmental and occupational medicine. Lippincott, Williams, and Wilson, Philadelphia, pp 1507–1520

    Google Scholar 

  • Weathers KC, Simkin SM, Lovett SM et al (2006b) Empirical modeling of atmospheric deposition in mountainous landscapes. Ecol Appl 16:1590–1607

    Google Scholar 

  • Yanni S, Keys K, Clair TA et al (2000) Fog and acidification impacts on ion budgets of basins in Nova Scotia, Canada. J Am Water Resour Assoc 36:619–631

    Google Scholar 

  • Zhang Y, Mitchell MJ, Christ M et al (1998) Stable sulfur isotopes at Hubbard Brook Experimental Forest, New Hampshire. Biogeochemistry 41:259–275

    Google Scholar 

  • Zhang L, Brook JR, Vet R et al (2001) Evaluation and Improvement of a dry deposition model using SO2 and O3 measurements over a mixed forest. Water Air Soil Pollut Focus 1:67–78

    Google Scholar 

  • Zhang L, Vet R, O’Brien JM et al (2009) Dry deposition of individual nitrogen species at eight Canadian rural sites. J Geophys Res 114:DO2301. doi:10.1029/2008JD010640

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Acknowledgments

This work was supported by 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, US National Science Foundation including the LTER and LTREB programs, New York City Department of Environmental Protection, New York State Energy Research Development Authority, Northeast Ecosystem Research Cooperative (NERC), Ontario Ministry of Environment, US Forest Services, US EPA, and US Geological Survey. We acknowledge funding support for sample collection and analysis by the U.S. Environmental Protection Agency’s Long-Term Monitoring program. The comments of Tom Huntington and J. E. Sickles on this manuscript were most helpful. Kim McEathron helped with some of the figures. The United States Environmental Protection Agency through its Office of Research and Development collaborated in the research described here. It has been subjected to Agency review and approved for publication.

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Authors and Affiliations

  1. College of Environmental Science and Forestry, SUNY, Syracuse, NY, 13210, USA

    Myron J. Mitchell

  2. Cary Institute of Ecosystem Studies, 2801 Sharon Turnpike, P.O. Box AB, Millbrook, NY, 12545-0129, USA

    Gary Lovett

  3. US Forest Service, Northern Research Station, 234 Mirror Lake Road, North Woodstock, NH, 02362, USA

    Scott Bailey

  4. Natural Resources Canada, Canadian Forest Service, 1219 Queen St. E, Sault Ste. Marie, ON, P6A 2E5, Canada

    Fred Beall

  5. US Geological Survey, 425 Jordan Road, Troy, NY, 12180, USA

    Doug Burns

  6. Cary Institute of Ecosystem Studies, 234 Mirror Lake Road, Hubbard Brook Forest Station, Campton, NH, 03223, USA

    Don Buso

  7. Water Science and Technology Branch, Environment Canada, P.O. Box 6227, Sackville, NB, E4L 1G6, Canada

    Thomas A. Clair

  8. Département de géographie, Université de Montréal, C.P. 6128, Succ. Centre-Ville, Montreal, QC, H3C 3J7, Canada

    Francois Courchesne

  9. Forêt Québec, Ministère des Ressources naturelles et de la Faune du Québec, 2700, rue Einstein, Quebec, QC, G1P 3W8, Canada

    Louis Duchesne

  10. Department of Geography, Trent University, Peterborough, ON, K9J 7B8, Canada

    Cathy Eimers

  11. Department of Plant, Soil, and Environmental Sciences, University of Maine, Orono, ME, 04469, USA

    Ivan Fernandez

  12. Direction de la recherche forestière, Forêt Québec, Ministère des Ressources naturelles et de la Faune du Québec, 2700, rue Einstein, Quebec, QC, G1P 3W8, Canada

    Daniel Houle

  13. Science and Technology Branch, Environment Canada, 8th floor, 105 McGill Street, Montreal, H2Y 2E, Canada

    Daniel Houle

  14. Aquatic Ecosystems Research Impacts Division, National Water Research Institute, Environment Canada, P.O. Box 5050, Burlington, ON, L7R4A6, Canada

    Dean S. Jeffries

  15. Cary Institute of Ecosystem Studies, 2801 Sharon Turnpike, P.O. Box AB, Millbrook, NY, 12545-0129, USA

    Gene E. Likens & Kathleen C. Weathers

  16. MACTEC Engineering & Consulting, Inc., 3901 Carmichael Ave., Jacksonville, FL, 32207, USA

    Christopher Rogers

  17. Atmospheric Modeling and Analysis Division, National Exposure Research Laboratory, US Environmental Protection Agency, Mail Drop E243-04, Research Triangle Park, NC, 27711, USA

    Donna Schwede

  18. US Geological Survey, P.O. Box 628, Montpelier, VT, 05601, USA

    Jamie Shanley

  19. Air Quality Research Division, Environment Canada, 4905 Dufferin Street, Toronto, ON, M3H 5T4, Canada

    Michael D. Moran & Robert Vet

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  1. Myron J. Mitchell
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  2. Gary Lovett
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  3. Scott Bailey
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  11. Ivan Fernandez
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  18. Jamie Shanley
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  19. Kathleen C. Weathers
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  20. Robert Vet
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Correspondence to Myron J. Mitchell.

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With the exception of Mitchell and Lovett, authors are listed alphabetically.

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Mitchell, M.J., Lovett, G., Bailey, S. et al. Comparisons of watershed sulfur budgets in southeast Canada and northeast US: new approaches and implications. Biogeochemistry 103, 181–207 (2011). https://doi.org/10.1007/s10533-010-9455-0

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