Development of a Fully Coupled Biogeochemical Reactive Transport Model to Simulate Microbial Oxidation of Organic Carbon and Pyrite Under Nitrate-Reducing Conditions

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Authors

Institutes & Expert groups

  • TU Berlin - Institute of Applied Geosciences - Hydrogeology Department
  • HLNUG - Hessian Agency for Nature Conservation - Environment and Geology
  • Technical university Darmstadt - Technische Universität Darmstadt, Institut für Kernphysik - Germany

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DOI

Abstract

In regions with intensive agriculture nitrate is one of the most relevant contaminants in groundwater. Denitrification reduces elevated nitrate concentrations in many aquifers, yet the denitrification potential is limited by the concentration of available electron donors. The aim of this work was to study the denitrification potential and its limitation in natural sediments. A column experiment was conducted using sediments with elevated concentrations of organic carbon (total organic carbon 3,247 mg C/kg) and pyrite (chromium reducible sulfur 150 mg/kg). Groundwater with high nitrate concentration (100 mg/L) was injected. Measurements were taken over 160 days at five different depths including N- and S-isotope analysis for selected samples. A reactive transport model was developed, which couples nitrate reduction with the oxidation of organic carbon (heterotrophic denitrification) and pyrite (autolithotrophic denitrification), and considers also transport and growth of denitrifying microbes. The denitrification pathway showed a temporal sequence from initially heterotrophic to autolithotrophic. However, maximum rates were lower for heterotrophic (11 mmol N/(L*a)) than for autolithotrophic denitrification (48 mmol N/(L*a)). The modeling showed that denitrifying microbes initially preferred highly reactive organic carbon as the electron donor for denitrification but were also able to utilize pyrite. The results show that after 160 days nitrate increased again to 50 mg/L. At this time only 0.5% of the total organic carbon and 46% of the available pyrite was oxidized. This indicates that denitrification rates strongly decrease before the electron donors are depleted either by a low reactivity (total organic carbon) or a diminishing reactive surface possibly due to the presence of coatings (pyrite).

Details

Original languageEnglish
Pages (from-to)9264-9286
Number of pages23
JournalWater Resources Research
Volume54
Issue number11
DOIs
StatePublished - 1 Nov 2018

Keywords

  • nitrate, contaminants, groundwater, denitrification, natural sediments

ID: 5291776