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Wastewater-based epidemiology applies the analysis of human metabolic excretion products of xenobiotics in wastewater to estimate the community-wide use of these compounds. A new bioanalytical method was developed, optimised and validated for the analysis of a broad range of antidepressants and their metabolites at trace concentrations in influent wastewater. The assay was based on solid-phase extraction and liquid chromatography coupled to tandem mass spectrometry. For most compounds, Oasis® HLB cartridges were used for sample preparation. Oasis® MCX cartridges were used for extraction of normirtazapine, moclobemide, sertraline, and melitracen in particular. The Kinetex XBC18 column with a gradient elution resulted in appropriate separation for the analytes under investigation. Validation was done according to the European Medicines Agency guidelines on bioanalytical method validation. For 27 compounds, the performance criteria met the requirements for method validation. For these analytes, the lower limit of quantification (LLOQ) ranged between 1 and 25 ng/L. Furthermore, all targeted biomarkers showed high in-sample stability during 24 h, with the exception of mianserin. The validated assay was applied to influent wastewater samples collected from four wastewater treatment plants in Belgium. Among these four locations, a total of 18 out of 27 biomarkers for antidepressant use were present in the samples in concentrations above the LLOQ. Additionally, the proposed methodology proved capable of analysing high resolution spatio-temporal trends. Mann-Kendall trend analyses showed that antidepressant use is stable throughout the week, except for trazodone which increased throughout the week. fx1 • Fully validated method for 27 antidepressants analysis in wastewater. • Different matrix effects for 5 antidepressants vs deuterated standard. • High in-sample stability for all targeted biomarkers. • Successfully applied to influent wastewater samples. [ABSTRACT FROM AUTHOR]

Wastewater-based epidemiology (WBE) employs the analysis of human metabolic biomarkers in influent wastewater (IWW) to estimate community-wide exposure to xenobiotics (e.g. prescription opioids). The low ng/L range of concentrations of these biomarkers and the complex matrix composition pose bioanalytical challenges related to sample preparation and detection/quantification. Therefore, a sensitive analytical method for the detection and analysis of 19 opioid biomarkers was optimized and validated according to the European Medicines Agency guidelines. Oasis HLB cartridges were used for sample concentration and an Atlantis T3 column with gradient elution resulted in sufficient separation of the analytes. Absolute recoveries (RE) were highly reproducible and ranged between 50 and 93% with the exception of 2-ethylidene-1,5-dimethyl-3,3-diphenylpyrrolidine (EDDP). The lower limit of quantification (LLOQ) ranged between 1 and 100 ng/L and was based on the analyte concentrations found in IWW. Process efficiency was acceptable for all biomarkers for which an isotope-labelled deuterated analogue was available. All biomarkers showed high benchtop stability with the exception of buprenorphine, EDDP, fentanyl and normorphine. Apart from buprenorphine and hydrocodone, all analytes under investigation were detected at least once above LLOQ levels in five locations in Belgium. The highest population-normalized mass loads were found for tramadol, O-desmethyltramadol and codeine. The proposed methodology was able to evaluate spatial differences in opioid use. [Display omitted] • Validation of an analytical method for quantification of 19 opioids in wastewater. • Process efficiency acceptable for all analytes when deuterated analogue was available. • High in-sample stability for 15 opioid biomarkers. • Spatial differences in opioid use between five Belgian catchment areas. [ABSTRACT FROM AUTHOR]