GEOCHEMISTRY, GROUNDWATER AND POLLUTION,

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1 GEOCHEMISTRY, GROUNDWATER AND POLLUTION, 2 ND EDITION C.A.J. APPELO Hydrochemical Consultant, Amsterdam, the Netherlands D. POSTMA Environment & Resources DTU, Technical University of Denmark, Kgs. Lyngby, Denmark A. A. BALKEMA PUBLISHERS Leiden/London/New York/Philadelphia/Singapore

2 Contents LIST OF EXAMPLES NOTATION XII XV 1 INTRODUCTION TO GROUNDWATER GEOCHEMISTRY Groundwater as drinking water Standards for drinking water Units of analysis Groundwater quality Sampling of groundwater Depth integrated or depth specific sampling Procedures for sampling of groundwater Chemical analysis of groundwater Field analyses and sample conservation Accuracy of chemical analysis 17 Problems 20 References 21 2 FROM RAINWATER TO GROUNDWATER The hydrological cycle The composition of rainwater Sources and transport of atmospheric pollutants Stable isotopes in rain Isotopic ratios and the 8 notation The Rayleigh process The isotopic composition of rain Dry deposition and evapotranspiration Mass balances and ecosystem dynamics Water quality profiles in the unsaturated soil Overall controls on water quality 51 Problems 58 References 59 3 FLOW AND TRANSPORT Flow in the unsaturated zone Flow in the saturated zone 64 VII

3 VIII Contents Darcy'slaw Flowlines in the subsoil Effects of non-homogeneity The aquifer as a chemical reactor Dating of groundwater Retardation The retardation equation Indifferent and broadening fronts Sharpening fronts Solid and solute concentrations Diffusion Diffusion coefficients Diffusion as a random process Diffusive transport Isotope diffusion Dispersion Column breakthrough curves Dispersion coefficients and dispersivity Macrodispersivity 107 Problems 113 References MINERALS AND WATER Equilibria and the solubility of minerals Corrections for solubility calculations Concentration and activity Aqueous complexes Combined complexes and activity corrections Calculation of saturation states Mass action constants and thermodynamics The calculation of mass action constants Calculation of mass action constants at different temperature Equilibrium calculations with PHREEQC Speciation calculations using PHREEQC The PHREEQC database Mineral equilibration Solid solutions Basic theory The fractionation factor for solid solutions Kinetic effects on the fractionation factor Kinetics of geochemical processes Kinetics and equilibrium Chemical reactions and rates Temperature dependency of reaction rates Mechanisms of dissolution and crystallization Rate laws for mineral dissolution and precipitation 162 Problems 169 References 171

4 Contents IX 5 CARBONATES AND CARBON DIOXIDE Carbonate minerals Dissolved carbonate equilibria The carbonic acid system Determining the carbonate speciation in groundwater Carbon dioxide in soils Calcite solubility and P C o Calcite dissolution in systems open and closed for CO 2 gas Two field examples Carbonate rock aquifers Dolomite and dedolomitization Pleistocene carbonate aquifers Kinetics of carbonate reactions Dissolution Precipitation Carbon isotopes Carbon-13 trends in aquifers C and groundwater age Retardation by sorption and stagnant zone diffusion 228 Problems 232 References ION EXCHANGE Cation exchange at the salt/fresh water interface Adsorbents in soils and aquifers Clay minerals Exchange equations Values for exchange coefficients Calculation of exchanger composition Calculation of exchanger composition with PHREEQC Determination of exchangeable cations Chromatography of cation exchange Field examples of freshening Salinity effects on cation exchange Quality patterns with salinization Fronts and chromatographic sequences Modeling chromatographic sequences with PHREEQC Physical non-equilibrium Modeling stagnant zones The Gouy-Chapman theory of the double layer Numerical integration of the double layer equations Practical aspects of double layer theory Irrigation water quality 299 Problems 303 References SORPTION OF TRACE METALS The origin and occurrence of heavy metals in groundwater Sorption isotherms and distribution coefficients 315

5 X Contents Distribution coefficients from ion exchange Variable charge surfaces Titration curves with suspended oxide particles Surface charge and point of zero charge, PZC Sorption edges Sorption, absorption, and coprecipitation Surface complexation Surface complexation models The ferrihydrite (Fe(OH) 3 ) database Diffuse double layer concentrations in surface complexation models Complexation to humic acids The ion association model Tipping and Hurley's discrete site model "WHAM" Distribution models Humic acids as carriers of trace elements Kinetics of surface complexation Extrapolation of adsorption kinetics for other metal ions Field applications 363 Problems 367 References SILICATE WEATHERING Weathering processes The stability of weathering products Incongruent dissolution of primary silicates The mass balance approach to weathering Kinetics of silicate weathering Field weathering rates Acid groundwater Buffering processes in aquifers 405 Problems 410 References REDOX PROCESSES Basic theory The significance of redox measurements Redox reactions and the pe concept Redox diagrams Stability of water The stability of dissolved species and gases: Arsenic The stability of minerals in redox diagrams Sequences of redox reactions and redox zoning Decomposition of organic matter Oxygen consumption Pyrite oxidation Kinetics of pyrite oxidation Oxygen transport and pyrite oxidation Nitrate reduction Nitrate reduction by organic matter oxidation Nitrate reduction by pyrite and ferrous iron 462

6 Contents XI 9.6 Iron reduction and sources of iron in groundwater Iron in aquifer sediments Reductive dissolution of iron oxides Sulfate reduction and iron sulfide formation The formation of iron sulfides The formation of methane 477 Problems 479 References POLLUTION BY ORGANIC CHEMICALS Gas-water exchange Evaporation of a pure organic liquid Transport of pure organic liquids through soil Sorption of organic chemicals Sorption of charged organic molecules Sorption in stagnant zones Release from stagnant zones and blobs Transformation reactions of organic chemicals Monod biotransformation kinetics Kinetic complexation of heavy metals on organics 529 Problems 535 References NUMERICAL MODELING Numerical modeling of transport Only diffusion Advection and diffusion/dispersion Non-linear reactions Examples of hydrogeochemical transport modeling Tritium-Helium age dating Toluene degradation in an aquifer Remediation of a BTEX polluted site Acid drainage from a Uranium mine In-situ iron removal from groundwater Arsenic in Bangladesh groundwater Fractionation of isotopes 590 References 595 APPENDIX A: HYDROGEOCHEMICAL MODELING WITH PHREEQC 599 APPENDIX B: ANSWERS TO PROBLEMS 617 INDEX 635

GEOCHEMISTRY, GROUNDWATER AND POLLUTION,

GEOCHEMISTRY, GROUNDWATER AND POLLUTION, GEOCHEMISTRY, GROUNDWATER AND POLLUTION, 2 ND EDITION C.A.J. APPELO Hydrochemical Consultant, Amsterdam, the Netherlands D.POSTMA Institute 01Environment & Resources DTU, Technical University 01Denmark,

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