A reactive-transport model has been applied to investigate the dynamics of the sulfate-methane transition zone (SMTZ) in nearshore sediments of Aarhus Bay (Denmark). The sediments are influenced by seasonal variations of temperature and particulate organic carbon (POC) deposition flux at the sediment-water interface. Initially, the model was calibrated at steady state using field data collected at two sites (M1 and M5) in December 2004, and included a dynamic gas phase which determines the depth of the SMTZ. Simulations were then performed under transient conditions of heat propagation in the porous medium, which influenced the solubility of gaseous methane, the diffusion of solutes as well as the kinetic and bioenergetic constraints on redox conditions in the system. Results revealed important variations in local rates of anaerobic oxidation of methane (AOM) over a seasonal cycle due to temperature variation. Seasonal perturbations in POC depositional flux had no influence on AOM rates but did have a strong bearing on sulfate reduction rates in the surface layers of the simulations at both stations. At M5, where the SMTZ was located 63 cm below the sediment-water interface, depth integrated AOM rates varied between 76 and 178 nmol cm -2 d -1 . At M1, where the deeper SMTZ (221 cm) experienced less thermal variation, AOM rates varied relatively less (20 to 24 nmol cm -2 d -1 ). Furthermore, local and depth-integrated AOM rates over the year did not show a simple response to bottom water temperature but exhibited a hysteresis-type behavior related to time lags in solute transport and heat propagation. Overall, the solute concentration profiles were not very sensitive to the seasonal variability in rates or gas transport and the modeled vertical displacement of the SMTZ was limited to Ͻ1 cm at M1 and 2-3 cm at M5. The results suggest that the significantly larger apparent displacement observed in the field from repeated coring (80 cm and 16 cm at M1 and M5, respectively) must be attributed to other factors, of which spatial heterogeneity in gas transport rate appears to be the most likely.
A fully coupled, two-dimensional hydrodynamic and reactive-transport model of C, N, O 2 and Si along a river-estuarinecoastal zone system is presented. It is applied to the Scheldt continuum, a macrotidal environment strongly affected by anthropogenic perturbations. The model extends from the upper tidal river and its tributaries to the southern Bight of the North Sea. Five dynamically linked nested grids are used, with a spatial resolution progressively increasing from 33 m to 2.7 km. The biogeochemical reaction network consists of aerobic degradation, nitrification, denitrification, phytoplankton growth and mortality, as well as reaeration. Diagnostic simulations of a typical summer situation in the early 1990s are compared to field data taken from the OMES database (>300 samples per variable). Results demonstrate that the process rates in the tidal river are very high and far larger than in the saline estuary, with maximum nitrification rates in the water column up to 70 mM N day − 1 , and maximum aerobic respiration and denitrification up to 70 and 40 mM C day − 1 , respectively. Phytoplankton production is about one order of magnitude lower, a result which confirms the dominance of heterotrophic processes in this system. The influence of secondary and tertiary wastewater treatment in the catchment is then assessed. Results show a significant decrease of organic matter and ammonium concentrations above Antwerp, which in turn leads to a partial restoration of oxygen levels. The model also predicts a reduction of denitrification rates, which locally results in a 4-fold increase of the nitrate concentration. Mass budgets for carbon, nitrogen and oxygen are established for the saline estuary (km 0 to 100) and for the tidal river network (km 100 to 160). Three scenarios, corresponding to the situation in the early 1990s, the years 2000 and the situation expected in 2010 are considered. They show that the tidal river and the estuary contribute almost equally to the overall biogeochemical cycling of these elements, despite the very different water volumes involved. For the simulated periods, the large decrease in nitrogen input (> 55%) expected between 1990 and 2010 will not lead to a significant decrease of N export to the coastal zone during the summer period.
[1] A Knowledge-Based Reactive Transport Model (KB-RTM) for simulation of coupled transport and biogeochemical transformations in surface and subsurface flow environments is presented (http:// www.geo.uu.nl/$kbrtm). The scalable Web-distributed Knowledge Base (KB), which combines Information Technology (IT), an automatic code generator, and database management, facilitates the automated construction of complex reaction networks from comprehensive information stored at the level of biogeochemical processes. The reaction-centric approach of the KB-RTM system offers full flexibility in the choice of model components and biogeochemical reactions. The procedure coupling the reaction networks to a generalized transport module into RTMs is also presented. The workings of our KB-RTM simulation environment are illustrated by means of two examples of redox and acid-base chemistry in a typical shelf sediment and an aquifer contaminated by landfill plumes.
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