Redox Processes and Water Quality of Selected Principal Aquifer Systems
P.B. McMahon,
F.H. Chapelle,
Corresponding Author
P.B. McMahon
U.S. Geological Survey, Denver, CO 80225; (303) 236-4882 x286; fax (303) 236-4912; [email protected]Search for more papers by this authorP.B. McMahon,
F.H. Chapelle,
Corresponding Author
P.B. McMahon
U.S. Geological Survey, Denver, CO 80225; (303) 236-4882 x286; fax (303) 236-4912; [email protected]Search for more papers by this authorAbstract
Reduction/oxidation (redox) conditions in 15 principal aquifer (PA) systems of the United States, and their impact on several water quality issues, were assessed from a large data base collected by the National Water-Quality Assessment Program of the USGS. The logic of these assessments was based on the observed ecological succession of electron acceptors such as dissolved oxygen, nitrate, and sulfate and threshold concentrations of these substrates needed to support active microbial metabolism. Similarly, the utilization of solid-phase electron acceptors such as Mn(IV) and Fe(III) is indicated by the production of dissolved manganese and iron. An internally consistent set of threshold concentration criteria was developed and applied to a large data set of 1692 water samples from the PAs to assess ambient redox conditions. The indicated redox conditions then were related to the occurrence of selected natural (arsenic) and anthropogenic (nitrate and volatile organic compounds) contaminants in ground water. For the natural and anthropogenic contaminants assessed in this study, considering redox conditions as defined by this framework of redox indicator species and threshold concentrations explained many water quality trends observed at a regional scale. An important finding of this study was that samples indicating mixed redox processes provide information on redox heterogeneity that is useful for assessing common water quality issues. Given the interpretive power of the redox framework and given that it is relatively inexpensive and easy to measure the chemical parameters included in the framework, those parameters should be included in routine water quality monitoring programs whenever possible.
Supporting Information
The following supplementary materials are available for this article:
Figure S1. Maps showing the distribution of domestic, public-supply, and monitoring (agricultural and urban land uses) wells used in this study.
Table S1. Number of samples, by well type, for each Principal Aquifer.
These materials are available as part of the online article from: http://www.blackwell-synergy.com/doi/abs/10.1111/j.1745-6584.2007.00385.x
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References
- Abacus Concepts. 1996. StatView Reference. Berkeley, California: Abacus Concepts Inc.
- Achtnich, C., F. Bak, and R. Conrad. 1995. Competition for electron donors among nitrate reducers, ferric iron reducers, sulfate reducers, and methanogens in anoxic paddy soil. Biology and Fertility of Soils 19, no. 1: 65–72.
- Alewell, C., S. Paul, G. Lischeid, K. Küsel, and M. Gehre. 2006. Characterizing the redox status in three different forested wetlands with geochemical data. Environmental Science & Technology 40, no. 24: 7609–7615.
- Back, W., and I. Barnes. 1965. Relation of electrochemical potentials and iron content to groundwater flow patterns. U.S. Geological Survey Professional Paper no. 498-C. Reston, Virginia: USGS.
- Baedecker, M.J., and W. Back. 1979. Hydrogeological processes and chemical reactions at a landfill. Ground Water 17, no. 5: 429–437.
- Beller, H.R., V. Madrid, G.B. Hudson, W.W. McNab, and T. Carlsen. 2004. Biogeochemical and natural attenuation of nitrate in ground water at an explosives test facility. Applied Geochemistry 19, no. 9: 1483–1494.
-
Berner, R.A. 1980. Early Diagenesis: A Theoretical Approach. Princeton, New Jersey: Princeton University Press.
10.1515/9780691209401 Google Scholar
- Böhlke, J.K., I.M. Verstraeten, and T.F. Kraemer. 2007. Effects of surface-water irrigation on sources, fluxes, and residence times of water, nitrate, and uranium in an alluvial aquifer. Applied Geochemistry 22, no. 1: 152–174.
- Böhlke, J.K., R. Wanty, M. Tuttle, G. Delin, and M. Landon. 2002. Denitrification in the recharge area and discharge area of a transient agricultural nitrate plume in a glacial outwash sand aquifer, Minnesota. Water Resources Research 38, no. 7: doi: 10.1029/2001WR00063.
- Bradley, P.M. 2003. History and ecology of chloroethene biodegradation: A review. Bioremediation Journal 7, no. 2: 81–109.
- Bradley, P.M. 2000. Microbial degradation of chloroethenes in groundwater systems. Hydrogeology Journal 8, no. 1: 104–111.
- Champ, D.R., J. Gulens, and R.E. Jackson. 1979. Oxidation-reduction sequences in groundwater flow systems. Canadian Journal of Earth Sciences 16, no. 1: 12–23.
- Chapelle, F.H., and D.R. Lovley. 1992. Competitive exclusion of sulfate reduction by Fe(III)-reducing bacteria: A mechanism for producing discrete zones of high-iron ground water. Ground Water 30, no. 1: 29–36.
- Chapelle, F.H., and P.B. McMahon. 1991. Geochemistry of dissolved inorganic carbon in a coastal plain aquifer. 1. Sulfate from confining beds as an oxidant in microbial CO2 production. Journal of Hydrology 127, no. 1–4: 85–108.
- Chapelle, F.H., P.M. Bradley, D.R. Lovley, K. O’Neill, and J.E. Landmeyer. 2002. Rapid evolution of redox processes in a petroleum hydrocarbon-contaminated aquifer. Ground Water 40, no. 4: 353–360.
- Chapelle, F.H., P.B. McMahon, N.M. Dubrovsky, R.F. Fujii, E.T. Oaksford, and D.A. Vroblesky. 1995. Deducing the distribution of terminal electron-accepting processes in hydrologically diverse groundwater systems. Water Resources Research 31, no. 2: 359–371.
- Chen, F., Q. Xia, and L.K. Ju. 2003. Aerobic denitrification of Pseudomonas aeruginosa monitored by online NAD(P)H fluorescence. Applied and Environmental Microbiology 69, no. 11: 6715–6722.
-
Christensen, T.H.,
P.L. Bjerg,
S.A. Banwart,
R. Jakobsen,
G. Heron, and
H.-H. Albrechtsen. 2000. Characterization of redox conditions in groundwater contaminant plumes.
Journal of Contaminant Hydrology
45, no. 3–4: 165–241.
10.1016/S0169-7722(00)00109-1 Google Scholar
- Dzombak, D.A., and F.M.M. Morel. 1990. Surface Complexation Modeling—Hydrous Ferric Oxide. New York: John Wiley & Sons.
- Elliot, T., J.N. Andrews, and W.M. Edmunds. 1999. Hydrochemical trends, palaeorecharge, and groundwater ages in the fissured Chalk aquifer of the London and Berkshire Basins, UK. Applied Geochemistry 14, no. 3: 333–363.
- Engstrom, P., T. Dalsgaard, S. Hulth, and R.C. Aller. 2005. Anaerobic ammonium oxidation by nitrite (anammox): Implications for N2 production in coastal marine sediments. Geochimica et Cosmochimica Acta 69, no. 8: 2057–2065.
- Froelich, P.N., G.P. Klinkhammer, M.L. Bender, N.A. Luedtke, G.R. Heath, D. Cullen, P. Dauphin, D. Hammond, B. Hartman, and V. Maynard. 1979. Early oxidation of organic matter in pelagic sediments of the eastern equatorial Atlantic: Suboxic diagenesis. Geochimica et Cosmochimica Acta 43, no. 7: 1075–1090.
- Hunter, K.S., Y. Wang, and P. Van Cappellen. 1998. Kinetic modeling of microbially-driven redox chemistry of subsurface environments: Coupling transport, microbial metabolism and geochemistry. Journal of Hydrology 209, no. 1: 53–80.
- Jakobsen, R., H.J. Albrechtsen, M. Rasmussen, H. Bay, P.L. Bjerg, and T.H. Christensen. 1998. H2 concentrations in a landfill leachate plume (Grindsted, Denmark): In situ energetics of terminal electron acceptor processes. Environmental Science & Technology 32, no. 14: 2142–2148.
- Knowles, R. 1982. Denitrification. Microbiological Reviews 46, no. 1: 43–70.
- Kölle, W., O. Strebel, and J. Böttcher. 1985. Formation of sulfate by microbial denitrification in a reducing aquifer. Water Supply 3: 35–40.
- Korom, S.F. 1992. Natural denitrification in the saturated zone: A review. Water Resources Research 28, no. 6: 1657–1668.
- Lapham, W.W., P.A. Hamilton, and D.N. Myers. 2005. National water-quality assessment program—Cycle II regional assessments of aquifers. U.S. Geological Survey Fact Sheet 2005-3013. Reston, Virginia: USGS.
- Lloyd, D., L. Boddy, and K.J.P. Davies. 1987. Persistence of bacterial denitrification capacity under aerobic conditions: The rule rather than the exception. FEMS Microbiology Ecology 45: 185–190.
- Lovley, D.R., and S. Goodwin. 1988. Hydrogen concentrations as an indicator of the predominant terminal electron-accepting reactions in aquatic sediments. Geochimica et Cosmochimica Acta 52, no. 12: 2993–3003.
- Lovley, D.R., and M.J. Klug. 1983. Sulfate reducers can outcompete methanogens at freshwater sulfate concentrations. Applied and Environmental Microbiology 45, no. 1: 187–192.
- Lovley, D.R., E.J.P. Phillips, Y.A. Gorby, and E.R. Landa. 1991. Microbial reduction of uranium. Nature 350, no. 6317: 413–416.
- Luther, G.W., B. Sundby, B.L. Lewis, P.J. Brendel, and N. Silverberg. 1997. Interactions of manganese with the nitrogen cycle: Alternative pathways to dinitrogen. Geochimica et Cosmochimica Acta 61, no. 19: 4043–4052.
- McMahon, P.B. 2001. Aquifer/aquitard interfaces: Mixing zones that enhance biogeochemical reactions. Hydrogeology Journal 9, no. 1: 34–43.
- McMahon, P.B., J.K. Böhlke, and S.C. Christenson. 2004. Geochemistry, radiocarbon ages, and paleorecharge conditions along a transect in the Central High Plains Aquifer, southwestern Kansas, USA. Appled Geochemistry 19, no. 11: 1655–1686.
- Murphy, E.M., and J.A. Schramke. 1998. Estimation of microbial respiration rates in groundwater by geochemical modeling constrained with stable isotopes. Geochimica et Cosmochimica Acta 62, no. 21/22: 3395–3406.
- Murray, J.W., H.W. Jannasch, S. Honjo, R.F. Anderson, W.S. Reeburgh, Z. Top, G.E. Friederich, L.A. Codispoti, and E. Izdar. 1989. Unexpected changes in the oxic/anoxic interface in the Black Sea. Nature 338, no. 6214: 411–413.
- Nolan, B.T., and K.J. Hitt. 2006. Vulnerability of shallow groundwater and drinking-water wells to nitrate in the United States. Environmental Science & Technology 40, no. 24: 7834–7840.
- Pabich, W.J., I. Valiela, and H.F. Hemond. 2001. Relationship between DOC concentration and vadose zone thickness and depth below water table in groundwater of Cape Cod, U.S.A. Biogeochemistry 55, no. 3: 247–268.
- Paschke, S.S., L.J. Kauffman, S.M. Eberts, and S.R. Hinkle. 2007. Overview of regional studies of the transport of anthropogenic and natural contaminants to public-supply wells. In Hydrogeologic Settings and Ground-Water Flow Simulations for Regional Studies of the Transport of Anthropogenic and Natural Contaminants to Public-Supply Wells—Studies Begun in 2001, ed. S.S. Paschke, 17. U.S. Geological Survey, Professional Paper no. 1737-A. Reston, Virginia: USGS.
- Plummer, L.N., J.F. Busby, R.W. Lee, and B.B. Hanshaw. 1990. Geochemical modeling of the Madison aquifer in parts of Montana, Wyoming, and South Dakota. Water Resources Research 26, no. 9: 1981–2014.
- Postma, D., C. Boesen, H. Kristiansen, and F. Larsen. 1991. Nitrate reduction in an unconfined sandy aquifer–water chemistry, reduction processes, and geochemical modeling. Water Resources Research 27, no. 8: 2027–2045.
- Ruddy, B.C., D.L. Lorenz, and D.K. Mueller. 2006. County-level estimates of nutrient inputs to the land surface of the conterminous United States, 1982–2001. U.S. Geological Survey Scientific Investigations Report 2006-5012, 17. Reston, Virginia: USGS.
- Scanlon, B.R., R.C. Reedy, D.A. Stonestrom, D.E. Prudic, and K.F. Dennehy. 2005. Impact of land use and land cover change on groundwater recharge and quality in the southwestern U.S. Global Change Biology 11, no. 10: 1577–1593.
- Seitzinger, S., J.A. Harrison, J.K. Böhlke, A.F. Bouwman, R. Lowrance, B. Peterson, C. Tobias, and G. Van Drecht. 2006. Denitrification across landscapes and waterscapes: A synthesis. Ecological Applications 16, no. 6: 2064–2090.
- Simpkins, W.W., and T.B. Parkin. 1993. Hydrogeology and redox geochemistry of CH4 in a late Wisconsinan till and loess sequence in central Iowa. Water Resources Research 29, no. 11: 3643–3657.
- Skerman, V.B.D., and I.C. MacRae. 1957. The influence of oxygen availability on the degree of nitrate reduction by Pseudomonas denitrificans. Canadian Journal of Microbiology 3, no. 3: 505–530.
-
Smedley, P.L., and
D.G. Kinniburgh. 2002. A review of the source, behavior, and distribution of arsenic in natural waters.
Applied Geochemistry
17, no. 5: 517–568.
10.1016/S0883-2927(02)00018-5 Google Scholar
- Straub, K.L., M. Benz, B. Schink, and F. Widdel. 1996. Anaerobic, nitrate-dependent microbial oxidation of ferrous iron. Applied and Environmental Microbiology 62, no. 4: 1458–1460.
- Thorstenson, D.C., D.W. Fisher, and M.G. Croft. 1979. The geochemistry of the Fox Hills-Basal Hell Creek Aquifer in southwestern north Dakota and northwestern South Dakota. Water Resources Research 15, no. 6: 1479–1498.
-
Thurman, E.M. 1985. Organic Geochemistry of Natural Waters. Boston, Massachusetts: Martinus Nijhoff/DR W. Junk.
10.1007/978-94-009-5095-5 Google Scholar
- Tiedje J.M. 1988. Ecology of denitrification and dissimilatory nitrate reduction to ammonium. In Biology of Anaerobic Microorganisms, ed. A.J.B. Zehnder, 179–244. New York: John Wiley & Sons.
- USGS. 2006a. National Water-Quality Assessment (NAWQA) Program. http://water.usgs.gov/nawqa/index.html (accessed September 29, 2007).
- USGS. 2006b. National Water-Quality Assessment (NAWQA) Program method, sampling, and analytical protocols. http://water.usgs.gov/nawqa/protocols/methodprotocols.html (accessed September 29, 2007).
- USGS. 2003. Principal aquifers of the 48 conterminous United States, Hawaii, Puerto Rico, and the U.S. Virgin Islands. http://www.nationalatlas.gov/mld/aquifrp.html (accessed September 29, 2007).
- Vogel, J.C., A.S. Talma, and T.H.E. Heaton. 1981. Gaseous nitrogen as evidence for denitrification in groundwater. Journal of Hydrology 50: 191–200.
- Vroblesky, D.A., and F.H. Chapelle. 1994. Temporal and spatial changes of terminal electron-accepting processes in a petroleum hydrocarbon-contaminated aquifer and the significance for contaminant biodegradation. Water Resources Research 30, no. 5: 1561–1570.
- Vroblesky, D.A., P.M. Bradley, and F.H. Chapelle. 1996. Influence of electron donor on the minimum sulfate concentration required for sulfate reduction in a petroleum hydrocarbon-contaminated aquifer. Environmental Science & Technology 30, no. 4: 1377–1381.
- Warner, K.L., and T.L. Arnold. 2005. Framework for regional synthesis of water-quality data for the glacial aquifer system in the United States. U.S. Geological Survey Scientific Investigations Report 2005-5223, 6. Reston, Virginia: USGS.
- Welch, A.H., D.B. Westjohn, D.R. Helsel, and R.B. Wanty. 2000. Arsenic in groundwater of the United States: Occurrence and geochemistry. Ground Water 38, no. 4: 589–604.
- Winograd, I.J., and F.N. Robertson. 1982. Deep oxygenated ground water: Anomaly or common occurrence? Science 216, no. 4551: 1227–1230.
- Zogorski, J.S., J.M. Carter, T. Ivahnenko, W.W. Lapham, M.J. Moran, B.L. Rowe, P.J. Squillace, and P.L. Toccalino. 2006. Volatile organic compounds in the nation’s ground water and drinking-water wells. U.S. Geological Survey Circular 1292, 101. Reston, Virginia: USGS.
