Modelling coupled water flow, solute transport and geochemical reactions affecting heavy metal migration in a podzol soil

Many or most subsurface pollution problems at the field scale involve such simultaneous processes as water flow, multicomponent solute transport, heat transport and biogeochemical processes and reactions. Process-based models that integrate these various processes can be valuable tools for investigating the mobility of a wide range of inorganic and organic contaminants subject to different hydrologic and geochemical conditions. The HP1 reactive transport simulator, obtained by weak coupling of HYDRUS-1D and PHREEQC-2, was developed and designed to address multicomponent geochemical transport processes in the vadose zone. In this paper we discuss a hypothetical HP1 application involving the transport of major cations and heavy metals in a soil during transient flow over a period of 30 years. Results show that variations in water content and water fluxes can significantly influence the speciation, and thus the mobility and availability, of elements. Decreasing water contents near the soil surface lowered pH of the soil solution and produced new cation exchange equilibrium conditions. The upward transport of Cl during summer due to increased evapotranspiration, and subsequent accumulation of Cl near the soil surface, caused an increase in the total aqueous Cd concentration because of the formation of Cd–Cl complexes. Coupled reactive transport codes for the unsaturated zone, such as HP1, are promising tools to unravel the complex interaction between soil physical and biogeochemical processes for all kinds of problems, including the impact of natural processes and antropogenic activities on soil evolution. © 2008 Elsevier B.V. All rights reserved.

[1]  G. T. Yeh,et al.  3DHYDROGEOCHEM: A 3-dimensional model of density-dependent subsurface flow and thermal multispecies-multicomponent hydrogeochemical transport. Final report , 1999 .

[2]  H. L. Penman Natural evaporation from open water, bare soil and grass , 1948, Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences.

[3]  L. Ma,et al.  Modeling the Transport and Retention of Cadmium in Soils: Multireaction and Multicomponent Approaches , 1992 .

[4]  Henry Lin,et al.  Hydropedology: Bridging Disciplines, Scales, and Data , 2003 .

[5]  H. Jenny,et al.  Factors of Soil Formation , 1941 .

[6]  M. V. Genuchten,et al.  Review and comparison of models for describing non-equilibrium and preferential flow and transport in the vadose zone , 2003 .

[7]  David W. Blowes,et al.  Multicomponent reactive transport modeling in variably saturated porous media using a generalized formulation for kinetically controlled reactions , 2002 .

[8]  D. L. Parkhurst,et al.  User's guide to PHREEQC (Version 2)-a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations , 1999 .

[9]  C. Appelo,et al.  Geochemistry, groundwater and pollution , 1993 .

[10]  Y. Le Gallo,et al.  Coupled reaction-flow modeling of diagenetic changes in reservoir permeability, porosity and mineral compositions , 1998 .

[11]  D Mallants,et al.  Operator-splitting errors in coupled reactive transport codes for transient variably saturated flow and contaminant transport in layered soil profiles. , 2006, Journal of contaminant hydrology.

[12]  D. Lapen,et al.  Placic and Ortstein Horizon Genesis and Peatland Development, Southeastern Newfoundland , 1999 .

[13]  Craig Rasmussen,et al.  Modeling energy inputs to predict pedogenic environments using regional environmental databases , 2005 .

[14]  Peter C. Lichtner,et al.  Continuum formulation of multicomponent-multiphase reactive transport , 1996 .

[15]  G. Kluitenberg,et al.  Effects of Thirty Years of Irrigation on the Genesis and Morphology of Two Semiarid Soils in Kansas , 2004 .

[16]  Werner Lutze,et al.  Scientific basis for nuclear waste management , 1979 .

[17]  J. Ryan,et al.  Colloid Movement in Unsaturated Porous Media: Recent Advances and Future Directions , 2004 .

[18]  E. Smolders,et al.  Chloride increases cadmium uptake in Swiss chard in a resin-buffered nutrient solution , 1996 .

[19]  James A. Davis,et al.  Assessing conceptual models for subsurface reactive transport of inorganic contaminants , 2004 .

[20]  G. Gaines,et al.  Adsorption Studies on Clay Minerals. II. A Formulation of the Thermodynamics of Exchange Adsorption , 1953 .

[21]  Van Genuchten,et al.  A closed-form equation for predicting the hydraulic conductivity of unsaturated soils , 1980 .

[22]  Jirka Šimůnek,et al.  Multicomponent solute transport in soil lysimeters irrigated with waters of different quality , 2006 .

[23]  Diederik Jacques,et al.  MULTICOMPONENT GEOCHEMICAL TRANSPORT MODELING USING HYDRUS‐1D AND HP11 , 2006 .

[24]  Karsten Pruess,et al.  Role of Competitive Cation Exchange on Chromatographic Displacement of Cesium in the Vadose Zone beneath the Hanford S/SX Tank Farm , 2004 .

[25]  D. Mallants,et al.  Grid lysimeter study of steady state chloride transport in two Spodosol types using TDR and wick samplers. , 2001, Journal of contaminant hydrology.

[26]  D. Mallants,et al.  Modelling uranium leaching from agricultural soils to groundwater as a criterion for comparison with complementary safety indicators , 2006 .

[27]  C. I. Steefel,et al.  New Direction in Hydrogeochemical Transport Modeling: Incorporating Multiple Kinetic and Equilibrium Reaction Pathways , 2000 .

[28]  K. Noack,et al.  Comparison of the solution behaviour of a pyrite-calcite mixture in batch and unsaturated sand column. , 2007, Journal of contaminant hydrology.

[29]  K. Mayer,et al.  A numerical model for multicomponent reactive transport in variably saturated porous media , 1999 .

[30]  Donald L. Suarez,et al.  Modeling of Carbon Dioxide Transport and Production in Soil 1. Model Development , 1993 .

[31]  L. Lake,et al.  A Physical Model of Cementation and Its Effects on Single-Phase Permeability , 1995 .

[32]  Marcel R. Hoosbeek,et al.  Towards the quantitative modeling of pedogenesis — a review , 1992 .

[33]  J. Quirk,et al.  Permeability of porous solids , 1961 .

[34]  D. Langmuir Aqueous Environmental Geochemistry , 1997 .

[35]  J. Verstraten,et al.  Influence of pH and metal/carbon ratios on soluble organic complexation of Fe(II), Fe(III) and Al(III) in soil solutions determined by diffusive gradients in thin films , 2002 .

[36]  Vicky L. Freedman,et al.  A Film Depositional Model of Permeability for Mineral Reactions in Unsaturated Media , 2004 .

[37]  S. Brantley Reaction Kinetics of Primary Rock-forming Minerals under Ambient Conditions , 2003 .

[38]  R. Arkley CALCULATION OF CARBONATE AND WATER MOVEMENT IN SOIL FROM CLIMATIC DATA , 1963 .

[39]  H. Ilvesniemi,et al.  Prediction of Near-Saturated Hydraulic Conductivity in Three Podzolic Boreal Forest Soils , 2000 .

[40]  J. Ryan,et al.  Colloid Movement in Unsaturated Porous Media: Recent Advances and Future Directions , 2004 .

[41]  R. Mosé,et al.  Operator-splitting procedures for reactive transport and comparison of mass balance errors. , 2004, Journal of contaminant hydrology.

[42]  A. N. D. R E A S V O E G E L I N, † V I J A,et al.  Reaction-Based Model Describing Competitive Sorption and Transport of Cd , Zn , and Ni in an Acidic Soil , 2022 .

[43]  R. Evershed,et al.  Mat Res Soc Symp Proc , 1995 .

[44]  Liping Pang,et al.  Colloid‐Facilitated Solute Transport in Variably Saturated Porous Media: Numerical Model and Experimental Verification , 2006 .

[45]  J. Hopmans,et al.  Porous Media With Linearly Variable Hydraulic Properties , 1991 .

[46]  Hans-Jörg Vogel,et al.  Hydropedology: Synergistic integration of pedology and hydrology , 2006 .

[47]  W. G. Gray,et al.  Computational methods in water resources X , 1994 .

[48]  E. Smolders,et al.  Cadmium fixation in soils measured by isotopic dilution , 1999 .

[49]  V. Metz,et al.  TRePro 2002 - modelling of coupled transport reaction processes. Workshop of the Forschungszentrum Karlsruhe held at 20th and 21st of March 2002 , 2002 .

[50]  Janet G. Hering,et al.  Principles and Applications of Aquatic Chemistry , 1993 .