Mobility of pharmaceuticals carbamazepine, diclofenac, ibuprofen, and propyphenazone in miscible-displacement experiments.

Many pharmaceuticals pass the unsaturated zone before reaching an aquifer. Therefore, laboratory sand column transport experiments were conducted to study the transport behavior of carbamazepine, diclofenac, ibuprofen, and propyphenazone under unsaturated conditions. The test water was artificial sewage effluent to simulate the infiltration of reused wastewater. The test water was spiked with the pharmaceutically active compounds and the tracer LiCl. Afterwards it was passed through laboratory sand columns, one experiment for each pharmaceutical. The physical and chemical parameters were recorded and general ions measured. Pharmaceuticals were measured using solid phase extraction, derivatization, and detection with GC-MS. The column experiments indicate a significant elimination of ibuprofen (54%), propyphenazone (55%), and diclofenac (35%), whereas carbamazepine was not eliminated. Retardation factors varied between 1.84 for carbamazepine, 2.51 for propyphenazone, 3.00 for ibuprofen, and 4.80 for diclofenac. These results show that mobility and elimination of diclofenac, ibuprofen, and propyphenazone is about in the same range as for experiments under saturated conditions whereas carbamazepine had a significantly lower sorption and elimination under unsaturated conditions.

Determination of sorption coefficients of pharmaceutically active substances carbamazepine, diclofenac, and ibuprofen, in sandy sediments.

Laboratory batch studies were conducted to characterize the sorption behavior of three pharmaceutically active substances (carbamazepine, diclofenac, and ibuprofen) in different sediment types. The sediments were natural sandy sediments from the water saturated zone and the unsaturated zone in the Berlin (Germany) area. They are characterized as medium and fine-grained sands, both with low organic carbon content. The results of the experiments show that sorption coefficients were generally quite low. Distribution coefficients (K(d) values) determined by the batch experiments varied from 0.21 to 5.32 for carbamazepine, 0.55 to 4.66 for diclofenac, and 0.18 to 1.69 for ibuprofen. Comparison of the organic carbon normalized sorption coefficient K(OC) values based on correlation equations with actual experimental data revealed that the calculated data for carbamazepine is of the same order as the experimental data. For diclofenac and ibuprofen the calculated values are much higher than the experimental data, showing a much higher mobility of diclofenac and ibuprofen in natural aquifer sediments than indicated by correlation equations based on octanol water distribution coefficients.

Transport of pharmaceutically active compounds in saturated laboratory columns.

Occurrences of pharmaceutically active compounds in surface water and sewage water have been widely reported. Investigations show the presence of several classes of pharmaceuticals such as antirheumatics (e.g., diclofenac), analgesics (e.g., propyphenazone), and blood lipid regulators (clofibric acid), even in ground water. Compared to their occurrences in surface water, however, the reported incidences of drugs in ground water are much rarer. This may be due to the input, but also to transport processes and degradation in the aquifer. In field studies investigating ground water sampled at a bank infiltration site at Lake Tegel, Berlin, Germany, clofibric acid was found at concentrations up to 290 ng/L, and propyphenazone up to 250 ng/L, whereas concentrations of diclofenac were around the detection limit. The aim of this study was to investigate the ground water transport behavior of the pharmaceuticals clofibric acid, propyphenazone, and diclofenac with a laboratory soil column experiment. Results show that clofibric acid exhibits no degradation and almost no retardation (Rf = 1.1). Diclofenac (Rf = 2.0) and propyphenazone (Rf = 1.6) are retarded, whereas significant degradation was not observed for both pharmaceuticals under the prevailing conditions in the soil column. We conclude that the concentration distribution of the pharmaceuticals at the bank filtration site at Lake Tegel is controlled by sorption, desorption, and input variation, rather than by degradation.