Using the INCA-Hg model of mercury cycling to simulate total and methyl mercury concentrations in forest streams and catchments.

We present a new, catchment-scale, process-based dynamic model for simulating mercury (Hg) in soils and surface waters. The Integrated Catchments Model for Mercury (INCA-Hg) simulates transport of gaseous, dissolved and solid Hg and transformations between elemental (Hg(0)), ionic (Hg(II)) and methyl (MeHg) Hg in natural and semi-natural landscapes. The mathematical description represents the model as a series of linked, first-order differential equations describing chemical and hydrological processes in catchment soils and waters which we believe control surface water Hg dynamics. The model simulates daily time series between one and 100 years long and can be applied to catchments ranging in size from <1 to ~10,000 km(2). Here we present applications of the model to two boreal forest headwater catchments in central Canada where we were able to reproduce observed patterns of stream water total mercury (THg) and MeHg fluxes and concentrations. Model performance was assessed using Monte Carlo techniques. Simulated in-stream THg and MeHg concentrations were sensitive to hydrologic controls and terrestrial and aquatic process rates.

[1]  Miriam Diamond,et al.  Development of a fugacity/aquivalence model of mercury dynamics in lakes , 1999 .

[2]  Andrew J. Wade,et al.  Simulating metals and mine discharges in river basins using a new integrated catchment model for metals: pollution impacts and restoration strategies in the Aries-Mures river system in Transylvania, Romania , 2009 .

[3]  Andrew J. Wade,et al.  The Integrated Catchments model of Phosphorus dynamics (INCA-P), a new approach for multiple source assessment in heterogeneous river systems: model structure and equations , 2002 .

[4]  M. Ravichandran,et al.  Interactions between mercury and dissolved organic matter--a review. , 2004, Chemosphere.

[5]  A. Wade,et al.  Towards an improved understanding of the nitrate dynamics in lowland, permeable river-systems: Applications of INCA-N , 2006 .

[6]  M. Futter,et al.  Stream Nitrate Responds Rapidly to Decreasing Nitrate Deposition , 2011, Ecosystems.

[7]  K. Xia,et al.  Distribution of mercury, methyl mercury and organic sulphur species in soil, soil solution and stream of a boreal forest catchment , 2003 .

[8]  R. B. Ambrose,et al.  An environmental simulation model for transport and fate of mercury in small rural catchments , 1999 .

[9]  J. Rudd,et al.  Importance of Wetlands as Sources of Methyl Mercury to Boreal Forest Ecosystems , 1994 .

[10]  Heather E. Golden,et al.  Simulated watershed mercury and nitrate flux responses to multiple land cover conversion scenarios , 2011, Environmental toxicology and chemistry.

[11]  J. Lester,et al.  Modelling the Long-Term Fate of Mercury in a Lowland Tidal River. I. Description of Two Finite Segment Models , 2010, Archives of environmental contamination and toxicology.

[12]  K. Devito,et al.  Episodic sulphate export from wetlands in acidified headwater catchments: Prediction at the landscape scale , 1999 .

[13]  J. Stoddard,et al.  Dissolved organic carbon trends resulting from changes in atmospheric deposition chemistry , 2007, Nature.

[14]  E. J. Wilson,et al.  A semi-distributed ntegrated itrogen model for multiple source assessment in tchments (INCA): Part I — model structure and process equations , 1998 .

[15]  R. Ambrose,et al.  Modeling Mercury Fluxes and Concentrations in a Georgia Watershed Receiving Atmospheric Deposition Load from Direct and Indirect Sources , 2005, Journal of the Air & Waste Management Association.

[16]  R. Hunt,et al.  Comparison of total mercury and methylmercury cycling at five sites using the small watershed approach. , 2008, Environmental pollution.

[17]  Lars Håkanson,et al.  Mercury in the Swedish environment — Recent research on causes, consequences and corrective methods , 1991 .

[18]  I. Tsiros A screening model-based study of transport fluxes and fate of airborne mercury deposited onto catchment areas. , 2001, Chemosphere.

[19]  A. Paterson,et al.  Temporal analysis of net fluvial methylmercury loading in a dystrophic and a clear water lake. , 2009, The Science of the total environment.

[20]  J. Rudd,et al.  Production and Loss of Methylmercury and Loss of Total Mercury from Boreal Forest Catchments Containing Different Types of Wetlands , 1996 .

[21]  Alexandre J. Poulain,et al.  Influence of temperate mixed and deciduous tree covers on Hg concentrations and photoredox transformations in snow , 2007 .

[22]  D. F. Grigal Mercury sequestration in forests and peatlands: a review. , 2003, Journal of environmental quality.

[23]  Robert A. Goldstein,et al.  Model Calculations of Total Maximum Daily Loads of Mercury for Drainage Lakes 1 , 2008 .

[24]  J. Munthe,et al.  MERCURY AND METHYLMERCURY IN RUNOFF FROM A FORESTED CATCHMENT - CONCENTRATIONS, FLUXES, AND THEIR RESPONSE TO MANIPULATIONS , 2004 .

[25]  M. Lucotte,et al.  Mercury and lead profiles and burdens in soils of Quebec (Canada) before and after flooding , 1995 .

[26]  H. Yao,et al.  Long-term declines in phosphorus export from forested catchments in south-central Ontario , 2009 .

[27]  C. Driscoll,et al.  Mercury in Freshwater Fish of Northeast North America – A Geographic Perspective Based on Fish Tissue Monitoring Databases , 2005, Ecotoxicology.

[28]  R. Shia,et al.  Multiscale modeling of the atmospheric fate and transport of mercury , 2001 .

[29]  I. Creed,et al.  Modeling dissolved organic carbon mass balances for lakes of the Muskoka River Watershed , 2009 .

[30]  Véronique Beaujouan,et al.  A nitrogen model for European catchments: INCA, new model structure and equations , 2002 .

[31]  Martyn N. Futter,et al.  Modeling the mechanisms that control in‐stream dissolved organic carbon dynamics in upland and forested catchments , 2007 .

[32]  R. Mason,et al.  Annual and seasonal trends in mercury deposition in Maryland , 2000 .

[33]  G. Mierle Aqueous inputs of mercury to precambrian shield lakes in ontario , 1990 .

[34]  C. Driscoll,et al.  A synthesis of rates and controls on elemental mercury evasion in the Great Lakes Basin. , 2012, Environmental pollution.

[35]  T. Holsen,et al.  Assessment of modeled mercury dry deposition over the Great Lakes region. , 2012, Environmental pollution.

[36]  J. Munthe,et al.  Mobilization of Mercury and Methylmercury from Forest Soils after a Severe Storm-Fell Event , 2007, Ambio.

[37]  B. Branfireun,et al.  Controls on the fate and transport of methylmercury in a boreal headwater catchment, northwestern Ontario, Canada , 2002 .

[38]  Katri Rankinen,et al.  An application of the GLUE methodology for estimating the parameters of the INCA-N model. , 2006, The Science of the total environment.

[39]  L. Barrie,et al.  Wet deposition of methyl mercury in northwestern Ontario compared to other geographic locations , 1995 .

[40]  Pierre Y. Julien,et al.  Metals fate and transport modelling in streams and watersheds: state of the science and USEPA workshop review , 2008 .

[41]  A. Dastoor,et al.  Global circulation of atmospheric mercury: a modelling study , 2004 .

[42]  D. Mackay,et al.  The development and application of a mass balance model for mercury (total, elemental and methyl) using data from a remote lake (Big Dam West, Nova Scotia, Canada) and the multi-species multiplier method , 2008 .

[43]  M. Futter,et al.  A long-term simulation of the effects of acidic deposition and climate change on surface water dissolved organic carbon concentrations in a boreal catchment. , 2009 .

[44]  Andrew Heyes,et al.  Whole-ecosystem study shows rapid fish-mercury response to changes in mercury deposition , 2007, Proceedings of the National Academy of Sciences.

[45]  T. Larssen,et al.  Mercury budget of a small forested boreal catchment in southeast Norway. , 2008, The Science of the total environment.

[46]  Christopher D. Knightes,et al.  Development and test application of a screening-level mercury fate model and tool for evaluating wildlife exposure risk for surface waters with mercury-contaminated sediments (SERAFM) , 2008, Environ. Model. Softw..

[47]  G. Aiken,et al.  Binding of mercury(II) to dissolved organic matter: the role of the mercury-to-DOM concentration ratio. , 2002, Environmental science & technology.

[48]  Katri Rankinen,et al.  An assessment of the fine sediment dynamics in an upland river system: INCA-Sed modifications and implications for fisheries. , 2010, The Science of the total environment.

[49]  G. Mierle,et al.  The role of humic substances in the mobilization of mercury from watersheds , 1991 .

[50]  L. Liao,et al.  Mercury adsorption-desorption and transport in soils. , 2009, Journal of environmental quality.

[51]  J. Dvonch,et al.  Spatial patterns and temporal trends in mercury concentrations, precipitation depths, and mercury wet deposition in the North American Great Lakes region, 2002-2008. , 2012, Environmental pollution.

[52]  E. J. Wilson,et al.  A semi-distributed integrated flow and nitrogen model for multiple source assessment in catchments (INCA): Part II — application to large river basins in south Wales and eastern England , 1998 .

[53]  M. Murray,et al.  Effects of Environmental Methylmercury on the Health of Wild Birds, Mammals, and Fish , 2007, Ambio.

[54]  S. Nelson,et al.  A review of mercury concentration and deposition in snow in eastern temperate North America , 2010 .

[55]  H. Hakola,et al.  Atmospheric and catchment mercury concentrations and fluxes in Fennoscandia , 2010 .

[56]  J. Munthe,et al.  Do concepts about catchment cycling of methylmercury and mercury in boreal catchments stand the test of time? Six years of atmospheric inputs and runoff export at Svartberget, northern Sweden. , 2000, The Science of the total environment.

[57]  D. Mackay,et al.  Quantifying the fate of mercury in the Great Lakes Basin: toward an ecosystem approach. , 2004, Environmental research.

[58]  T. Holsen,et al.  Mercury dynamics and transport in two Adirondack Lakes , 2009 .

[59]  Petri Porvari,et al.  Forestry practices increase mercury and methyl mercury output from boreal forest catchments. , 2003, Environmental science & technology.

[60]  D. Butterfield,et al.  A simple model for predicting soil temperature in snow-covered and seasonally frozen soil: model description and testing , 2004 .

[61]  W. de Vries,et al.  Critical levels of atmospheric pollution: criteria and concepts for operational modelling of mercury in forest and lake ecosystems. , 2003, The Science of the total environment.

[62]  Charles T Driscoll,et al.  Mercury cycling in litter and soil in different forest types in the Adirondack region, New York, USA. , 2007, Ecological applications : a publication of the Ecological Society of America.

[63]  C. Watras,et al.  Mercury pollution : integration and synthesis , 1994 .

[64]  R. Canuel,et al.  Mercury cycling and human health concerns in remote ecosystems in the Americas , 2009 .

[65]  M. Futter,et al.  Simulating Dissolved Organic Carbon Dynamics at the Swedish Integrated Monitoring Sites with the Integrated Catchments Model for Carbon, INCA-C , 2011, AMBIO.

[66]  D. F. Grigal Inputs and outputs of mercury from terrestrial watersheds: a review , 2002 .

[67]  U. Skyllberg,et al.  Competition among thiols and inorganic sulfides and polysulfides for Hg and MeHg in wetland soils and sediments under suboxic conditions: Illumination of controversies and implications for MeHg net production , 2008 .

[68]  Nicolas S. Bloom,et al.  On the Chemical Form of Mercury in Edible Fish and Marine Invertebrate Tissue , 1992 .