title: Tracing gadolinium-based contrast agents from surface water to drinking water by means of speciation analysis.
abstract: In recent decades, a significant amount of anthropogenic gadolinium has been released into the environment as a result of the broad application of contrast agents for magnetic resonance imaging (MRI). Since this anthropogenic gadolinium anomaly has also been detected in drinking water, it has become necessary to investigate the possible effect of drinking water purification on these highly polar microcontaminats. Therefore, a novel highly sensitive method for speciation analysis of gadolinium is presented. For that purpose, the hyphenation of hydrophilic interaction liquid chromatography (HILIC) and inductively coupled plasma-mass spectrometry (ICP-MS) was employed. In order to enhance the detection power, sample introduction was carried out by ultrasonic nebulization. In combination with a novel HILIC method using a diol-based stationary phase, it was possible to achieve superior limits of detection for frequently applied gadolinium-based contrast agents below 20pmol/L. With this method, the contrast agents Gd-DTPA, Gd-DOTA and Gd-BT-DO3A were determined in concentrations up to 159pmol/L in samples from several waterworks in a densely populated region of Germany alongside the river Ruhr as well as from a waterworks near a catchment lake. Thereby, the direct impact of anthropogenic gadolinium species being present in the surface water on the amount of anthropogenic gadolinium in drinking water was shown. There was no evidence for the degradation of contrast agents, the release of Gd(3+) or the presence of further Gd species.
authors.affiliation: University of Münster, Institute of Inorganic and Analytical Chemistry, Corrensstraße 28/30, 48149 Münster, Germany.
authors.forename: Marvin
authors.initials: M
authors.lastname: Birka
authors.affiliation: University of Münster, Institute of Inorganic and Analytical Chemistry, Corrensstraße 28/30, 48149 Münster, Germany.
authors.forename: Christoph A
authors.initials: CA
authors.lastname: Wehe
authors.affiliation: University of Münster, Institute of Inorganic and Analytical Chemistry, Corrensstraße 28/30, 48149 Münster, Germany.
authors.forename: Oliver
authors.initials: O
authors.lastname: Hachmöller
authors.affiliation: University of Münster, Institute of Inorganic and Analytical Chemistry, Corrensstraße 28/30, 48149 Münster, Germany; European Virtual Institute for Speciation Analysis (EVISA), Mendelstraße 11, 48149 Münster, Germany.
authors.forename: Michael
authors.initials: M
authors.lastname: Sperling
authors.affiliation: University of Münster, Institute of Inorganic and Analytical Chemistry, Corrensstraße 28/30, 48149 Münster, Germany. Electronic address: uk@uni-muenster.de.
authors.forename: Uwe
authors.initials: U
authors.lastname: Karst
mesh_terms: D002623:Chemistry Techniques, Analytical / Q000379:methods*; D002853:Chromatography, Liquid; D003287:Contrast Media / Q000032:analysis* / Q000737:chemistry*; D060766:Drinking Water / Q000737:chemistry*; D004784:Environmental Monitoring; D019786:Gadolinium DTPA / Q000032:analysis / Q000737:chemistry; D005858:Germany; D006571:Heterocyclic Compounds / Q000032:analysis / Q000737:chemistry; D057927:Hydrophobic and Hydrophilic Interactions; D013058:Mass Spectrometry; D009942:Organometallic Compounds / Q000032:analysis / Q000737:chemistry; D045483:Rivers / Q000737:chemistry*; D014874:Water Pollutants, Chemical / Q000032:analysis* / Q000737:chemistry
chemical_list: D003287:Contrast Media; D060766:Drinking Water; D006571:Heterocyclic Compounds; D009942:Organometallic Compounds; D014874:Water Pollutants, Chemical; C050823:gadolinium 1,4,7,10-tetraazacyclododecane-N,N',N'',N'''-tetraacetate; D019786:Gadolinium DTPA
keywords: Contrast agents; Drinking water; Gadolinium; LC-ICP-MS; Speciation analysis