Sorption properties and behaviour at laboratory scale of selected pharmaceuticals using batch experiments.

Despite the increasing public concern about the frequent occurrence of pharmaceuticals in the water bodies, their transport and fate are not yet well known; in particular in groundwater. In this laboratory study, batch experiments were conducted to investigate the sorption behaviour of selected pharmaceuticals. The choice of compounds was motivated by their chemical properties as well as by their occurrence at the relevant field sites. It included: antipyrine, atenolol, caffeine, carbamazepine, ciprofloxacin, diclofenac, ketoprofen, ofloxacin, and sulfamethoxazole. Sorption behaviour has already been investigated for some of these compounds (e.g. carbamazepine), but for the others (e.g. antipyrine, ketoprofen), extensive studies are missing so far. For the experiments, artificial and actual aquifer materials from complementary field sites were selected: technical coarse quartz sand and sediments from alluvial Vistrenque Aquifer, France (sandy loam), and fluvio-deltaic Baix Fluvià Aquifer, Spain (sandy clay loam, clay, and medium sand). In these field sites occurrence of pharmaceuticals in groundwater was previously stated, and the presented laboratory experiments were complementary to the field investigations. Five concentration steps for determining the sorption isotherms were investigated. Correlation analysis showed dependencies of K-coefficients of individual compounds and sediment properties; however, no clear, universal patterns for all compounds were found. Batch experiments suggest that sorption behaviour was governed by compound-specific properties rather than by sediment properties. These results contribute to the understanding sorption behaviour of pharmaceuticals in heterogeneous sediments, although some inconsistencies were revealed between laboratory scale results and field scale observations.

Spatial distribution of triazine residues in a shallow alluvial aquifer linked to groundwater residence time.

At present, some triazine herbicides occurrence in European groundwater, 13 years after their use ban in the European Union, remains of great concern and raises the question of their persistence in groundwater systems due to several factors such as storage and remobilization from soil and unsaturated zone, limited or absence of degradation, sorption in saturated zones, or to continuing illegal applications. In order to address this problem and to determine triazine distribution in the saturated zone, their occurrence is investigated in the light of the aquifer hydrodynamic on the basis of a geochemical approach using groundwater dating tracers (3H/3He). In this study, atrazine, simazine, terbuthylazine, deethylatrazine, deisopropylatrazine, and deethylterbuthylazine are measured in 66 samples collected between 2011 and 2013 from 21 sampling points, on the Vistrenque shallow alluvial aquifer (southern France), covered by a major agricultural land use. The frequencies of quantification range from 100 to 56 % for simazine and atrazine, respectively (LQ = 1 ng L-1). Total triazine concentrations vary between 15 and 350 ng L-1 and show three different patterns with depth below the water table: (1) low concentrations independent of depth but related to water origin, (2) an increase in concentrations with depth in the aquifer related to groundwater residence time and triazine use prior to their ban, and (3) relatively high concentrations at low depths in the saturated zone more likely related to a slow desorption of these compounds from the soil and unsaturated zone. The triazine attenuation rate varies between 0.3 for waters influenced by surface water infiltration and 4.8 for water showing longer residence times in the aquifer, suggesting an increase in these rates with water residence time in the saturated zone. Increasing triazine concentrations with depth is consistent with a significant decrease in the use of these pesticides for the last 10 years on this area and highlights the efficiency of their ban.