Quantification Approaches in Non-Target LC/ESI/HRMS Analysis: An Interlaboratory Comparison

• Authors: MALM Louise; LIIGAND Jaanus; AALIZADEH Reza; ALYGIZAKIS Nikiforos; NG Kelsey Kwong Pui; FROKJAER Emil Egede; NANUSHA Mulatu Yohannes; HANSEN Martin; PLASSMANN Merle; BIEBER Stefan; LETZEL Thomas; BALEST Lydia; ABIS Pier Paolo; MAZZETTI Michele; KASPRZYK-HORDERN Barbara; CEOLOTTO Nicola; KUMARI Sangeeta; HANN Stephan; KOCHMANN Sven; STEININGER-MAIRINGER Teresa; SOULIER Coralie; MASCOLO Giuseppe; MURGOLO Sapia; GARCIA-VARA Manuel; DE ALDA Miren Lopez; HOLLENDER Juliane; ARTURI Katarzyna; COPPOLA Gianluca; PERUZZO Massimo; JOERSS Hanna; VAN DER NEUT-MARCHAND Carla; PIEKE Eelco N.; GAGO-FERRERO Pablo; GIL-SOLSONA Ruben; LICUL-KUCERA Viktoria; ROSCIOLI Claudio; VALSECCHI Sara; LUCKUTE Austeja; CHRISTENSEN Jan H.; TISLER Selina; VUGHS Dennis; MEEKEL Nienke; ANDUJAR Begona Talavera; AURICH Dagny; SCHYMANSKI Emma L.; FRIGERIO Gianfranco; MACHERIUS Andre; KUNKEL Uwe; BADER Tobias; ROSTKOWSKI Pawel; GUNDERSEN Hans; VALDECANAS Belinda; DAVIS W. Clay; SCHULZE Bastian; KASERZON Sarit; PIJNAPPELS Martijn; ESPERANZA Mar; FILDIER Aurelie; VULLIET Emmanuelle; WIEST Laure; COVACI Adrian; SCHONLEBEN Alicia Macan; BELOVA Lidia; CELMA Alberto; BIJLSMA Lubertus; CAUPOS Emilie; MEBOLD Emmanuelle; LE ROUX Julien; TROIA Eugenie; DE RIJKE Eva; HELMUS Rick; LEROY Gaela; HAELEWYCK Niels; CHRASTINA David; VERWOERT Milan; THOMAIDIS Nikolaos S.; KRUVE Anneli
• Year of publication: 2024
• Type: Article in Periodical
• Magazine / Source: Analytical chemistry
• MU Faculty or unit: Faculty of Science
• web: https://pubs.acs.org/doi/10.1021/acs.analchem.4c02902
• Doi: http://dx.doi.org/10.1021/acs.analchem.4c02902
• Keywords: ANALYSIS EMERGING CONTAMINANTS; IONIZATION-MASS SPECTROMETRY; ELECTROSPRAY-IONIZATION; LIQUID-CHROMATOGRAPHY; SEMI-QUANTIFICATION; EFFICIENCY; METABOLITES; ENVIRONMENT; POLLUTANTS; PRODUCTS
• Description: Nontargeted screening (NTS) utilizing liquid chromatography electrospray ionization high-resolution mass spectrometry (LC/ESI/HRMS) is increasingly used to identify environmental contaminants. Major differences in the ionization efficiency of compounds in ESI/HRMS result in widely varying responses and complicate quantitative analysis. Despite an increasing number of methods for quantification without authentic standards in NTS, the approaches are evaluated on limited and diverse data sets with varying chemical coverage collected on different instruments, complicating an unbiased comparison. In this interlaboratory comparison, organized by the NORMAN Network, we evaluated the accuracy and performance variability of five quantification approaches across 41 NTS methods from 37 laboratories. Three approaches are based on surrogate standard quantification (parent-transformation product, structurally similar or close eluting) and two on predicted ionization efficiencies (RandFor-IE and MLR-IE). Shortly, HPLC grade water, tap water, and surface water spiked with 45 compounds at 2 concentration levels were analyzed together with 41 calibrants at 6 known concentrations by the laboratories using in-house NTS workflows. The accuracy of the approaches was evaluated by comparing the estimated and spiked concentrations across quantification approaches, instrumentation, and laboratories. The RandFor-IE approach performed best with a reported mean prediction error of 15x and over 83% of compounds quantified within 10x error. Despite different instrumentation and workflows, the performance was stable across laboratories and did not depend on the complexity of water matrices.