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Gadolinium-based MRI contrast agents found intact in the outlet of a waste water treatment plant

(17.04.2009)


Background:
Gadolinium chelates are used as contrast agents for medical magnetic resonance imaging (MRI) since the 80's. About 20,000,000 patienst per year are investigated by this diagnostic tool, each one receiving typically around 1.2 g of gadolinium. Most of the Gd is extreted by the patients within the first day after application with urine entering the environment via waste water.

Gd is one of the rare earth elements (REE) that normally show a characteristic distribution pattern within the environment. Anthropogenic emission of Gd into the aquatic environment can therefore relatively easily be detected via the disturbance of the characteristic natural REE distribution pattern.

Since Gd-based contrast agents are very stable complexes, they are excreted in unmetabolized form and are suspected not to be biodegradable in the aquatic environment. In order to study the fate of these compounds within waste water treatment plants, Gd speciation analysis at ultratrace levels would be helpful.

The new study:
Researchers from the University of Münster developed a new method based on ICP-MS detection to follow the Gd-contrast agents through the waste water treatment plant.

In order to allow the separation of the different Gd-based contrast agents, the ICP-MS was coupled with a hydrophilic interaction chromatography (HILIC) system.

Waste water and sewage samples were taken at different stations of the Münster central waste water treatment plant. The hyphenated system consisted of an Agilent 1200 series HPLC system coupled to an PerkinElmer Sciex ELAN 6000 quadrupole ICP-MS. The detection limit of the hyphenated system was around 1x 10-9 mol/l, while the detection limit for total Gd was around 2 x 10-10 mol/l. Sorption losses of Gd-chelates to container walls were significantly reduced by using silanized glass in most steps of sample preparation and sample storage.

The method was able to detect different Gd-based contrast agents at the primary clarifier of the wastewater treatment plant. The most often applied macrocyclic Gd- based agend Gd-BT-DO3A could be traced even to the outlet of the plant. The researchers conclude their report by expressing their hope that the newly developed method will help to investigate the behaviour of Gd-contrast agents during wastewater treatment.

The Original study

Jens Künnemeyer, Lydia Terborg, Björn Meermann, Christine Brauckmann, Ines Möller, Andy Scheffer, Uwe Karst, Speciation Analysis of Gadolinium Chelates in Hospital Effluents and Wastewater Treatment Plant Sewage by a Novel HILIC/ICP-MS Method, Environ. Sci. Technol., 43/8 (2009) 2884-2890. DOI: 10.1021/es803278n

Michael G. Lawrence, Christoph Ort, Comment on "Speciation Analysis of Gadolinium Chelates in Hospital Effluents and Wastewater Treatment Plant Sewage by a Novel HILIC/ICP-MS Method", Environ. Sci. Technol., 2009, asap. DOI: 10.1021/es901406g

Jens Künnemeyer, Lydia Terborg, Björn Meermann, Christine Brauckmann, Ines Möller, Andy Scheffer, Uwe Karst, Response to Comment on "Speciation Analysis of Gadolinium Chelates in Hospital Effluents and Wastewater Treatment Plant Sewage by a Novel  HILIC/ICP-MS Method", Environ. Sci. Technol., 2009, asap. DOI: 10.1021/es901550c


Related studies

Michael Bau, Peter Dulski, Anthropogenic origin of positive gadolinium anomalies in river waters, Earth Planet. Sci. Lett. , 143/1-4 (1996) 245-255. doi:10.1016/0012-821X(96)00127-6

Klaus Kümmerer, Eckard Helmers, Hospital Effluents as a Source of Gadolinium in the Aquatic Environment, Environ. Sci. Technol., 34/2 (2000) 573-577. doi: 10.1021/es990633h

Françoise Elbaz-Poulichet, Jean-Luc Seidel, Clara Othoniel, Occurrence of an anthropogenic gadolinium anomaly in river and coastal waters of Southern France, Water Research, 36/4 (2002) 1102-1105. doi:10.1016/S0043-1354(01)00370-0

Peter Möller, Giulio Morteani, Peter Dulski, Anomalous Gadolinium, Cerium, and Yttrium Contents in the Adige and Isarco River Waters and in the Water of Their Tributaries (Provinces Trento and Bolzano/Bozen, NE Italy), Acta Hydrochim. Hydrobiol., 31/3 (2003) 225-239. DOI: 10.1002/aheh.200300492

Andrea Knappe, Peter Möller, Peter Dulski, Asaf Pekdeger, Positive gadolinium anomaly in surface water and ground water of the urban area Berlin, Germany, Chem. Erde Geochem., 65/2 (2005) 167-189. doi:10.1016/j.chemer.2004.08.004

Serkan Kulaksiz, Michael Bau, Contrasting behaviour of anthropogenic gadolinium and natural rare earth elements in estuaries and the gadolinium input into the North Sea, Earth Planet. Sci. Lett., 260/1-2 (2007) 361-371. doi:10.1016/j.epsl.2007.06.016


Related EVISA Resources

Link Database: Toxicity of Gadolinium compounds
Materials Database: Gadolinium Materials
Brief Summary: ICP-MS: A versatile detection system for speciation analysis
Brief Summary: LC-ICP-MS: The most often used hyphenated system for speciation analysis


Related EVISA News (Newest first)

March 14, 2016: Tracing Gadolinium-based Contrast Agents from Wastewater, via Surface Water to Drinking Water
March 4, 2015: Detection of Gd-based contrast agent in the skin of a patient eight years after administration
October 29, 2012: Identification and quantification of potential metabolites of Gd-based contrast agents 
October 18, 2012: The behavior of Gd-based contrast agents during wastewater treatment
September 15, 2010: US FDA Announces Gadolinium-Based MRI Contrast Agent Warning
March 25, 2010: Publication on the separation of Gd-based contrast agents awarded
May 4, 2009: Gadolinium speciation analysis in search for the cause of nephrogenic systemic fibrosis (NSF) 



last time modified: March 23, 2016









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