Kinetics of N2O production and reduction in a nitrate-contaminated aquifer inferred from laboratory incubation experiments

摘要

Knowledge of the kinetics of N2O production and reduction in groundwater is essential for the assessment of potential indirect emissions of the greenhouse gas. In the present study, we investigated this kinetics using a laboratory approach. The results were compared to field measurements in order to examine their transferability to the in situ conditions. The study site was the unconfined, predominantly sandy Fuhrberger Feld aquifer in northern Germany. A special characteristic of the aquifer is the occurrence of the vertically separated process zones of heterotrophic denitrification in the near-surface groundwater and of autotrophic denitrification in depths beyond 2–3 m below the groundwater table, respectively. The kinetics of N2O production and reduction in both process zones was studied during long-term anaerobic laboratory incubations of aquifer slurries using the 15N tracer technique. We measured N2O, N2, NO3-, NO2-, and SO42- concentrations as well as parameters of the aquifer material that were related to the relevant electron donors, i.e. organic carbon and pyrite. The laboratory incubations showed a low denitrification activity of heterotrophic denitrification with initial rates between 0.2 and 13 μg N kg?1 d?1. The process was carbon limited due to the poor availability of its electron donor. In the autotrophic denitrification zone, initial denitrification rates were considerably higher, ranging between 30 and 148 μg N kg?1 d?1, and NO3- as well as N2O were completely removed within 60 to 198 days. N2O accumulated during heterotrophic and autotrophic denitrification, but maximum concentrations were substantially higher during the autotrophic process. The results revealed a satisfactory transferability of the laboratory incubations to the field scale for autotrophic denitrification, whereas the heterotrophic process less reflected the field conditions due to considerably lower N2O accumulation during laboratory incubation. Finally, we applied a conventional model using first-order-kinetics to determine the reaction rate constants k1 for N2O production and k2 for N2O reduction, respectively. The goodness of fit to the experimental data was partly limited, indicating that a more sophisticated approach is essential to describe the investigated reaction kinetics satisfactorily.