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Screening for pharmaceutical transformation products formed in river sediment by combining ultrahigh performance liquid chromatography/high resolution mass spectrometry with a rapid data-processing method
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).ORCID iD: 0000-0002-2379-0768
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
2014 (English)In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 810, 61-70 p.Article in journal (Refereed) Published
Abstract [en]

While the occurrence of pharmaceuticals in the aquatic environment has been extensively investigated, their environmental fate is less thoroughly explored. Scarce information on their transformation pathways and transformation products (TPs) limits conventional target analytical approaches. In this study, samples from water/sediment tests were analyzed by ultrahigh performance liquid chromatography interfaced with quadrupole time-of-flight mass spectrometry (UHPLC/QToF-MS). A data processing method based on peak detection, time-trend filtration and structure assignment was established to provide an efficient way for identifying the key TPs in terms of persistence; all software used for the individual steps of this method is freely available. The accurate mass and meaningful time-trends were major contributors in facilitating the isolation of plausible TP peaks. In total, 16 TPs from 9 parent pharmaceuticals were identified. Eleven out of the 16 TPs were confirmed by corresponding reference standards; no standards were available for the remaining TPs. For additional 6 potential TPs, a molecular formula was suggested but no additional structural information could be generated. Among the TPs identified in the water/sediment tests, carbamazepine-10,11-epoxide (parent: carbamazepine), saluamine (parent: furosemide), chlorothiazide and 4-amino-6-chloro-1,3-benzenedisulfonamide (parent of both: hydrochlorothiazide), and 1-naphthol (parent: propranolol) accumulated over the entire incubation period of 35 days.

Place, publisher, year, edition, pages
2014. Vol. 810, 61-70 p.
Keyword [en]
pharmaceuticals, transformation products, water/sediment test, ultrahigh performance liquid chromatography/high resolution mass spectrometry, in silico data processing
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-100774DOI: 10.1016/j.aca.2013.12.012OAI: oai:DiVA.org:su-100774DiVA: diva2:696162
Available from: 2014-02-13 Created: 2014-02-13 Last updated: 2017-12-06Bibliographically approved
In thesis
1. An integrated approach to study pharmaceuticals and their microbial transformation products: formation and environmental behavior in water/sediment systems
Open this publication in new window or tab >>An integrated approach to study pharmaceuticals and their microbial transformation products: formation and environmental behavior in water/sediment systems
2014 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Pharmaceuticals are emerging organic micropollutants that are frequently detected in the aquatic environment. While information on their environmental occurrence is substantial, knowledge gaps exist with respect to their environmental transformation. This licentiate thesis focuses on this research deficit by (1) providing and applying tools for identifying biotransformation products, and (2) investigating the behavior of pharmaceuticals and their transformation products (TPs) in two different experimental systems.

Study I established a data-processing method based on peak detection, time-trend filtration and structure assignment, and provides an efficient and reliable way for TP identification. Water/sediment tests were carried out with 9 pharmaceuticals. The method for identifying TPs is based on accurate mass data obtained from high resolution mass spectrometry and a comprehensive data-processing workflow. In total, 16 TPs were identified, 11 of which were confirmed by reference standards. Five of the TPs showed a continuous accumulation over the entire incubation period of 35 days.

Study II aimed at studying the influence of water/sediment interactions on the environmental behavior of pharmaceuticals and their TPs. An artificial streaming channel was applied to simultaneously determine the concentrations of parent pharmaceuticals and key TPs in both surface water and sediment pore water under defined hydraulic conditions. All pharmaceuticals dissipated from the test system. The benefit from simultaneously analyzing parent compounds and TPs can be illustrated with carbamazepine, which is generally reported to be persistent. In study II, carbamazepine dissipated continuously from the test system, and the formation of a TP shows that this dissipation can be attributed to microbial biotransformation. The results also indicate that transformation predominantly occurs in the hyporheic zone, but also that TPs can be transported back into the streaming channel.

This thesis confirms the crucial role of the hyporheic zone for the elimination of organic micropollutants from rivers and streams. Moreover, the developed workflow for TP identification provides opportunities to efficiently identify TPs for additional micropollutants in laboratory and field studies. In future work, we will study the influence of hydraulic conditions on transformation kinetics and formation of characteristic TPs, and we will extend the work to additional pharmaceuticals. Moreover, we will test the applicability of using TPs as indicators for characterizing ongoing biotransformation in field settings, thereby providing a more efficient way of characterizing the environmental fate of pharmaceuticals.

Place, publisher, year, edition, pages
Stockholm: Department of Applied Environmental Science (ITM), Stockholm University, 2014. 24 p.
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-101184 (URN)
Presentation
2014-03-21, William-Olssonsalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2014-03-03 Created: 2014-02-28 Last updated: 2014-03-11Bibliographically approved
2. Fate of Pharmaceuticals and Their Transformation Products in Rivers: An integration of target analysis and screening methods to study attenuation processes
Open this publication in new window or tab >>Fate of Pharmaceuticals and Their Transformation Products in Rivers: An integration of target analysis and screening methods to study attenuation processes
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Pharmaceuticals are environmental contaminants causing steadily increasing concern due to their high usage, ubiquitous distribution in the aquatic environment, and potential to exert adverse effects on the ecosystems. After being discharged from wastewater treatment plants (WWTPs), pharmaceuticals can undergo transformation processes in surface waters, of which microbial degradation in river sediments is considered highly significant. In spite of a substantial number of studies on the occurrence of pharmaceuticals in aquatic systems, a comprehensive understanding of their environmental fate is still limited. First of all, very few consistent datasets from lab-based experiments to field studies exist to allow for a straightforward comparison of observations. Secondly, data on the identity and occurrence of transformation products (TPs) is insufficient and the relation of the behavior of TPs to that of their parent compounds (PCs) is poorly understood. In this thesis, these knowledge gaps were addressed by integrating the TP identification using suspect/non-target screening approaches and PC/TP fate determination. The overarching objective was to improve the understanding of the fate of pharmaceuticals in rivers, with a specific focus on water-sediment interactions, and formation and behavior of TPs. In paper I, 11 pharmaceutical TPs were identified in water-sediment incubation experiments using non-target screening. Bench-scale flume experiments were conducted in paper II to simultaneously investigate the behavior of PCs and TPs in both water and sediment compartments under more complex and realistic hydraulic conditions. The results illustrate that water-sediment interactions play a significant role for efficient attenuation of PCs, and demonstrate that TPs are formed in sediment and released back to surface water. In paper III the environmental behavior of PCs along stretches of four wastewater-impacted rivers was related to that of their TPs. The attenuation of PCs is highly compound and site specific. The highest attenuation rates of the PCs were observed in the river with the most efficient river water-pore water exchange. This research also indicates that WWTPs can be a major source of TPs to the receiving waters. In paper IV, suspect screening with a case-control concept was applied on water samples collected at both ends of the river stretches, which led to the identification of several key TPs formed along the stretches. The process-oriented strategies applied in this thesis provide a basis for prioritizing and identifying the critical PCs and TPs with respect to environmental relevance in future fate studies.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University, 2015. 24 p.
Keyword
pharmaceuticals, transformation products, fate, river, suspect screening, non-target screening
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-123752 (URN)978-91-7649-292-5 (ISBN)
Public defence
2016-02-05, De Geersalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Submitted. Paper 4: Manuscript.

Available from: 2016-01-13 Created: 2015-12-04 Last updated: 2016-01-14Bibliographically approved

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