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Proc Natl Acad Sci U S A. 2019 Feb 12;116(7):2494-2499. doi: 10.1073/pnas.1816892116. Epub 2019 Jan 28.

Stratification of reactivity determines nitrate removal in groundwater.

Author information

Centre National de la Recherche Scientifique (CNRS), Géoscience Rennes - UMR 6118, Université de Rennes, 35042 Rennes, France;
Centre National de la Recherche Scientifique (CNRS), Géoscience Rennes - UMR 6118, Université de Rennes, 35042 Rennes, France.
Centre National de la Recherche Scientifique (CNRS), Institut National de la Recherche Agronomique (INRA), Observatoire des Sciences de l'Univers de Rennes (OSUR) - UMR 3343, Université de Rennes, 35042 Rennes, France.
Department of Plant and Wildlife Sciences, Brigham Young University, Provo, UT 84604.
Centre National de la Recherche Scientifique (CNRS), ECOBIO - UMR 6553, Université de Rennes, 35042 Rennes, France.
Water Mission Area, US Geological Survey, Menlo Park, CA.
Department of Hydrogeology, Helmholtz Centre for Environmental Research - Zentrum für Umweltforschung (UFZ), 04318 Leipzig, Germany.
Division of Hydrologic Modeling, University of Bayreuth, 95447 Bayreuth, Germany.
Ecole Nationale du Génie Rural, des Eaux et des Forêts (ENGREF), Agroparistech, 75231 Paris, France.
Department of Hydrology, Bayreuth Center of Ecology and Environmental Research, 95447 Bayreuth, Germany.
Institut National de la Recherche Agronomique (INRA), Sol Agro et Hydrosystème Spatialisation, UMR 1069, Agrocampus Ouest, 35042 Rennes, France.
Institut National de Recherche en Sciences et Technologies pour l'Environnement et l'Agriculture (Irstea), RiverLy, Centre de Lyon-Villeurbanne, 69625 Villeurbanne, France.


Biogeochemical reactions occur unevenly in space and time, but this heterogeneity is often simplified as a linear average due to sparse data, especially in subsurface environments where access is limited. For example, little is known about the spatial variability of groundwater denitrification, an important process in removing nitrate originating from agriculture and land use conversion. Information about the rate, arrangement, and extent of denitrification is needed to determine sustainable limits of human activity and to predict recovery time frames. Here, we developed and validated a method for inferring the spatial organization of sequential biogeochemical reactions in an aquifer in France. We applied it to five other aquifers in different geological settings located in the United States and compared results among 44 locations across the six aquifers to assess the generality of reactivity trends. Of the sampling locations, 79% showed pronounced increases of reactivity with depth. This suggests that previous estimates of denitrification have underestimated the capacity of deep aquifers to remove nitrate, while overestimating nitrate removal in shallow flow paths. Oxygen and nitrate reduction likely increases with depth because there is relatively little organic carbon in agricultural soils and because excess nitrate input has depleted solid phase electron donors near the surface. Our findings explain the long-standing conundrum of why apparent reaction rates of oxygen in aquifers are typically smaller than those of nitrate, which is energetically less favorable. This stratified reactivity framework is promising for mapping vertical reactivity trends in aquifers, generating new understanding of subsurface ecosystems and their capacity to remove contaminants.


denitrification; groundwater; reaction times; reactivity pattern; transit times

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