Improving Target and Suspect Screening High-Resolution Mass Spectrometry Workflows in Environmental Analysis by Ion Mobility Separation

Celma, Alberto; Sancho, J.; Schymanski, Emma L.; Fabregat‐Safont, David; Ibáñez, María; Goshawk, Jeff; Barknowitz, Gitte; Hernández, Félix; Bijlsma, Lubertus

doi:10.1021/acs.est.0c05713

Cited by 94 publications

(160 citation statements)

References 57 publications

Supporting

Mentioning

129

Contrasting

Order By: Relevance

“…[56][57][58] Published collisional cross sections of vidarabine (156.4 Å² for [M+H] + ) and adenosine (156.9 Å² for [M+H] + ) measured on the same instrument are available, revealing a difference of only 0.5 Å² or 0.3%, which is too close to distinguish currently within the typical resolving power of ion mobility spectrometers. 59,60 M-H2O (18.0104) This study documents suspect screening efforts thus far for pharmaceuticals and their known TPs as a starting point for further understanding pharmaceutical levels in Luxembourgish surface waters. Other activities looking into different chemical classes such as pesticides 65 , industrial chemicals, and other emerging pollutants are ongoing.…”

Section: Spatio-temporal Distribution Of Pharmaceuticals Inmentioning

confidence: 67%

Occurrence and Distribution of Pharmaceuticals and their Transformation Products in Luxembourgish Surface Waters

Singh

Lai²,

Krier³

et al. 2021

Preprint

View full text Add to dashboard Cite

show abstract

Section: Spatio-temporal Distribution Of Pharmaceuticals Inmentioning

confidence: 67%

Occurrence and Distribution of Pharmaceuticals and their Transformation Products in Luxembourgish Surface Waters

Singh

Lai²,

Krier³

et al. 2021

Preprint

View full text Add to dashboard Cite

show abstract

“…Regarding identification of substances, the IM-derived CCS values can be used as further identification criteria in addition to m/z, retention time, isotopic pattern and fragment ions. It has been shown that CCS values are not affected by different matrices [34][35][36]. Thus, CCS values have a high potential to improve the confidence of compound identification [35].…”

Section: Introductionmentioning

confidence: 99%

“…It has been shown that CCS values are not affected by different matrices [34][35][36]. Thus, CCS values have a high potential to improve the confidence of compound identification [35]. Several studies have already published CCS databases for different compound classes [34][35][36][37][38][39][40][41][42], which can be used to compare experimental CCS values.…”

Section: Introductionmentioning

confidence: 99%

“…Thus, CCS values have a high potential to improve the confidence of compound identification [35]. Several studies have already published CCS databases for different compound classes [34][35][36][37][38][39][40][41][42], which can be used to compare experimental CCS values. However, especially in environmental analysis, only a few databases exist that can be used for such comparisons.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Target, suspect and non-target screening analysis from wastewater treatment plant effluents to drinking water using collision cross section values as additional identification criterion

2021

View full text Add to dashboard Cite

The anthropogenic entry of organic micropollutants into the aquatic environment leads to a potential risk for drinking water resources and the drinking water itself. Therefore, sensitive screening analysis methods are needed to monitor the raw and drinking water quality continuously. Non-target screening analysis has been shown to allow for a more comprehensive investigation of drinking water processes compared to target analysis alone. However, non-target screening is challenging due to the many features that can be detected. Thus, data processing techniques to reduce the high number of features are necessary, and prioritization techniques are important to find the features of interest for identification, as identification of unknown substances is challenging as well. In this study, a drinking water production process, where drinking water is supplied by a water reservoir, was investigated. Since the water reservoir provides surface water, which is anthropogenically influenced by wastewater treatment plant (WWTP) effluents, substances originating from WWTP effluents and reaching the drinking water were investigated, because this indicates that they cannot be removed by the drinking water production process. For this purpose, ultra-performance liquid chromatography coupled with an ion-mobility high-resolution mass spectrometer (UPLC-IM-HRMS) was used in a combined approach including target, suspect and non-target screening analysis to identify known and unknown substances. Additionally, the role of ion-mobility-derived collision cross sections (CCS) in identification is discussed. To that end, six samples (two WWTP effluent samples, a surface water sample that received the effluents, a raw water sample from a downstream water reservoir, a process sample and the drinking water) were analyzed. Positive findings for a total of 60 substances in at least one sample were obtained through quantitative screening. Sixty-five percent (15 out of 23) of the identified substances in the drinking water sample were pharmaceuticals and transformation products of pharmaceuticals. Using suspect screening, further 33 substances were tentatively identified in one or more samples, where for 19 of these substances, CCS values could be compared with CCS values from the literature, which supported the tentative identification. Eight substances were identified by reference standards. In the non-target screening, a total of ten features detected in all six samples were prioritized, whereby metoprolol acid/atenolol acid (a transformation product of the two β-blockers metoprolol and atenolol) and 1,3-benzothiazol-2-sulfonic acid (a transformation product of the vulcanization accelerator 2-mercaptobenzothiazole) were identified with reference standards. Overall, this study demonstrates the added value of a comprehensive water monitoring approach based on UPLC-IM-HRMS analysis. Graphical abstract

show abstract

“…Moreover, in wide-scope screening approaches, the utilization of predictive CCS models facilitate and give more reliability to the tentative identification of suspect compounds ( Bijlsma et al, 2017( Bijlsma et al, , 2019Mullin et al, 2020 ). In front of this scenario, a refined workflow for target and suspect environmental analysis using IMS-HRMS data has been proposed (Celma et al, 2020 ), including complementary identification levels criteria for IMS and updating the criteria previously reported on confidence levels ( Schymanski et al, 2014 ).…”

Section: Introductionmentioning

confidence: 99%

Wide-scope screening of pharmaceuticals, illicit drugs and their metabolites in the Amazon River

Fabregat‐Safont¹,

Ibáñez²,

Bijlsma³

et al. 2021

Water Research

Self Cite

View full text Add to dashboard Cite

Only a limited number of households in the Amazon are served by sewage collection or treatment facilities, suggesting that there might be a significant emission of pharmaceuticals and other wastewater contaminants into freshwater ecosystems. In this work, we performed a wide-scope screening to assess the occurrence of pharmaceuticals, illicit drugs and their metabolites in freshwater ecosystems of the Brazilian Amazon. Our study included 40 samples taken along the Amazon River, in three of its major tributaries, and in small tributaries crossing four important urban areas (Manaus, Santarém, Macapá, Belém). More than 900 compounds were investigated making use of target and suspect screening approaches, based on liquid chromatography coupled to high-resolution mass spectrometry with ion mobility separation. Empirical collision-cross section (CCS) values were used to help and confirm identifications in target screening, while in the suspect screening approach CCS values were predicted using Artificial Neural Networks to increase the confidence of the tentative identification. In this way, 51 compounds and metabolites were identified. The highest prevalence was found in streams crossing the urban areas of Manaus, Macapá and Belém, with some samples containing up to 30 -40 compounds, while samples taken in Santarém showed a lower number (8 -11), and the samples taken in the main course of the Amazon River and its tributaries contained between 1 and 7 compounds. Most compounds identified in areas with significant urban impact belonged to the analgesics and antihypertensive categories, followed by stimulants and antibiotics. Compounds such as caffeine, cocaine and its metabolite benzoylecgonine, and cotinine (the metabolite of nicotine), were also detected in areas with relatively low anthropogenic impact and showed the highest total prevalence. This study supports the need to improve the sanitation system of urban areas in the Brazilian Amazon and the development of follow-up studies aimed at quantifying exposure levels and risks for Amazonian freshwater biodiversity.

show abstract

Improving Target and Suspect Screening High-Resolution Mass Spectrometry Workflows in Environmental Analysis by Ion Mobility Separation

Cited by 94 publications

References 57 publications

Occurrence and Distribution of Pharmaceuticals and their Transformation Products in Luxembourgish Surface Waters

Occurrence and Distribution of Pharmaceuticals and their Transformation Products in Luxembourgish Surface Waters

Target, suspect and non-target screening analysis from wastewater treatment plant effluents to drinking water using collision cross section values as additional identification criterion

Wide-scope screening of pharmaceuticals, illicit drugs and their metabolites in the Amazon River

Contact Info

Product

Resources

About