Distribution of six anticancer drugs and a variety of other pharmaceuticals, and their sorption onto sediments, in an urban Japanese river

Abstract

The distributions of 31 pharmaceuticals grouped into nine therapeutic classes, including six anticancer drugs, were investigated in the waters and sediments of an urban river in Japan. The coefficients of sorption (logK ) to the river sediments were also determined from the results of a field survey and laboratory-scale experiment. Three anticancer drugs-bicalutamide, doxifluridine, and tamoxifen-were detected in the river sediments at maximum concentrations of 391, 392, and 250 ng/kg, respectively. In addition, the transformation products of psychotropic carbamazepine (2-hydroxy carbamazepine, acridine, and acridone) were detected in the range of 108 ng/kg (2-hydroxy carbamazepine) to 2365 ng/kg (acridine), and the phytoestrogen glycitein was detected in the range of N.D. to 821 ng/kg. The logK values of the targeted pharmaceuticals in river sediments in the field survey ranged from 0.5 (theophylline) to 3.3 (azithromycin). These results were in accord with those of the laboratory-scale sorption experiment. To the best of our knowledge, this is the first report of the detection of the anticancer drugs bicalutamide and tamoxifen, the transformation products of carbamazepine (2-hydroxy carbamazepine, acridine, and acridone), and the phytoestrogen genistein in river sediments.

Distribution of Anticancer Drugs in River Waters and Sediments of the Yodo River Basin, Japan

“…Recent in-depth quantification of these drugs together with the other anticancer drugs was achieved by the simultaneous combination of procedures known as solid-phase extraction (SPE) and liquid chromatography-mass spectrometry (LC-MS/MS) [16,[45][46][47], with special care taken for differences in the protocols applied for the liquid and the solid samples. The concentration and purification steps of the anticancer drugs in the liquid samples were performed by SPE [13,31]. In the case of the river sediments and the suspended solids (solid state samples), solvent extraction of the adsorbed materials was achieved by sonication and filtration [31,48,49] prior to analysis.…”

“…The concentration and purification steps of the anticancer drugs in the liquid samples were performed by SPE [13,31]. In the case of the river sediments and the suspended solids (solid state samples), solvent extraction of the adsorbed materials was achieved by sonication and filtration [31,48,49] prior to analysis.…”

“…The occurrences of anticancer drugs in the solid state samples (river sediments and suspended solids) at Suita Bridge (R5) and Hirakata Bridge (R6) are summarized in Figure 2 [31]. Three anticancer drugs (BLT, TAM, and CAP) were detected at appreciably higher concentrations in the suspended solids at 628, 13-658, and 231 µg/kg, respectively, with higher levels at the Hirakata Bridge than at the Suita Bridge.…”

“…The sorption property of the present anticancer drugs on the river sediments was further characterized by a sorption experiment [31]. The measured logK d values varied in a range from −0.4 to 2.1 ( Table 6).…”

“…At present, the pollution aspect of anticancer drugs in Japan has been analyzed only in the very limited area surrounding the Yodo River since 2009 [13,[28][29][30][31]. Their occurrence in the river water and sediments, including from hospital and sewage treatment effluents [13,28,32], their fate after discharge [31], and their attenuation properties [29,30], were reported in a separate fashion. The time has come to make an overview of the status of anticancer drugs in the environmental water of the Yodo River basin.…”