Preliminary results of two-dimensional multicomponent reactive transport modelling to understand the controlling factors on uranium mobility in a siliciclastic aquifer in Hungary

In Hungary, the drinking water supply relies upon groundwater resources of up to 98%. As a drinking water resource, groundwater must meet strict quality requirements in order to minimise any health effects arising from daily water consumption. Water-rock interactions enrich groundwater not only with essential elements (e.g. Ca, Mg) but also with undesired substances such as heavy metals or radioactive elements. In the last few years, a thorough drinking water quality monitoring campaign was carried out in Hungary, revealing that some parts of the country are characterised by relatively high uranium concentrations. The causes of these elevated activities have not been properly investigated, yet. However, understanding the controls of the release and mobility of uranium is critical in proper groundwater management.

Baják et al (2022) developed a one-dimensional (1-D) geochemical model using the code PHREEQC (Parkhurst and Appelo, 2013) to examine the processes that determine the fate of uranium in the siliciclastic Miocene-Quaternary aquifer system near Velence Hills, some 50 km off Budapest. Here, the geological build-up (granitic rocks on the surface) favours the high uranium content in groundwater, which is characterised by oxidising conditions. The 1-D model included redox-controlled kinetic reactions as well as other potential uranium-controlling processes (e.g., surface complexation). The results suggested that uranium distribution is sensitive to redox changes in the aquifer and its mobility in groundwater especially depends on the residence time of water compared to the reaction times controlling the consumption of oxidising species.

This study introduces a two-dimensional multicomponent reactive transport model developed using the PHT3D code (Prommer et al., 2003), which is a coupling between MODFLOW and PHREEQC. The model builds on and extends the capability of the 1-D model to simulate uranium mobility across the multiple flow paths of the aquifer systems. The model calibration accounts for 30 groundwater samples collected from drinking water wells in the study area. Physico-chemical parameters (temperature, pH, specific electric conductivity, redox potential) were measured on-site, and the samples were analysed for natural tracers (δ¹⁶O, δ²H, ²³⁴U, ²³⁸U, ²²⁶Ra) to gain further insight into the geochemical processes of the aquifer system.

This research was supported by the ÚNKP-23-4 New National Excellence Program of the Ministry for Culture and Innovation from the source of the National Research, Development and Innovation Fund and was supported by the János Bolyai Research Scholarship of the Hungarian Academy of Sciences. The research is part of a project which was funded by the National Multidisciplinary Laboratory for Climate Change, RRF-2.3.1-21-2022-00014.

References:

Baják, P., Csondor, K., Pedretti, D., Muniruzzaman, M., Surbeck, H., Izsák, B., Vargha, M., Horváth, Á., Pándics, T., Erőss, A., 2022. Refining the conceptual model for radionuclide mobility in groundwater in the vicinity of a Hungarian granitic complex using geochemical modeling. Applied Geochemistry 137, 105201.

Parkhurst, D.L., Appelo, C.A.J., 2013. Description of Input and Examples for PHREEQC Version 3—A Computer Program for Speciation, Batch-Reaction, One-Dimensional Transport, and Inverse Geochemical Calculations. (USGS Technical No. 6(A)43). U.S. Geological Survey, Denver, CO, USA.

Prommer H, Barry, D.A., Zheng, C. (2003). MODFLOW/MT3DMS based reactive multi-component transport modeling. Ground Water, 41(2).