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

Published

September 24, 2024

Author(s)

Clay Davis, Anneli Kruve-Viil, Louise Malm, Jaanus Liigand, Reza Aalizadeh, Nikiforos Alygizakis, Emil Egede Fro̷kjær, Mulatu Yohannes Nanusha, Martin Hansen, Merle Plassmann, Stefan Bieber, Thomas Letzel, Lydia Balest, Pier Paolo Abis, Michele Mazzetti, Barbara Kasprzyk-Hordern, Nicola Ceolotto, Sangeeta Kumari, Stephan Hann, Sven Kochmann, Teresa Steininger-Mairinger, Coralie Soulier, Giuseppe Mascolo, Sapia Murgolo, Manuel Garcia-Vara, Miren López de Alda, Juliane Hollender, Katarzyna Arturi, Gianluca Coppola, Massimo Peruzzo, Hanna Joerss, Carla van der Neut-Marchand, Eelco N. Pieke, Ruben Gil-Solsona, Viktória Licul-Kucera, Claudio Roscioli, Sara Valsecchi, Austeja Luckute, Jan H. Christensen, Selina Tisler, Dennis Vughs, Nienke Meekel, Begoña Talavera Andújar, Dagny Aurich Dagny Aurich, Emma L. Schymanski, Gianfranco Frigerio, André Macherius, Uwe Kunkel, Tobias Bader, Pawel Rostkowski, Hans Gundersen, Belinda Valdecanas, Bastian Schulze, Sarit Kaserzon, Martijn Pijnappels, Mar Esperanza, Aurélie Fildier, Emmanuelle Vulliet, Laure Wiest, Adrian Covaci, Alicia Macan Schönleben, Lidia Belova, Alberto Celma, Lubertus Bijlsma, Emilie Caupos, Emmanuelle Mebold, Julien Le Roux, Eugenie Troia, Eva de Rijke, Rick Helmus, Gaëla Leroy, Niels Haelewyck, David Chrastina, Milan Verwoert, Nikolaos S. Thomaidis

Abstract

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 15× and over 83% of compounds quantified within 10× error. Despite different instrumentation and workflows, the performance was stable across laboratories and did not depend on the complexity of water matrices.

Citation

Analytical Chemistry

Pub Type

Journals

Keywords

Nontargeted screening, high-resolution mass spectrometry, interlaboratory comparison

Citation

Davis, C. , Kruve-Viil, A. , Malm, L. , Liigand, J. , Aalizadeh, R. , Alygizakis, N. , Fro̷kjær, E. , Nanusha, M. , Hansen, M. , Plassmann, M. , Bieber, S. , Letzel, T. , Balest, L. , Paolo Abis, P. , Mazzetti, M. , Kasprzyk-Hordern, B. , Ceolotto, N. , Kumari, S. , Hann, S. , Kochmann, S. , Steininger-Mairinger, T. , Soulier, C. , Mascolo, G. , Murgolo, S. , Garcia-Vara, M. , López de Alda, M. , Hollender, J. , Arturi, K. , Coppola, G. , Peruzzo, M. , Joerss, H. , van der Neut-Marchand, C. , Pieke, E. , Gil-Solsona, R. , Licul-Kucera, V. , Roscioli, C. , Valsecchi, S. , Luckute, A. , Christensen, J. , Tisler, S. , Vughs, D. , Meekel, N. , Talavera Andújar, B. , Dagny Aurich, D. , Schymanski, E. , Frigerio, G. , Macherius, A. , Kunkel, U. , Bader, T. , Rostkowski, P. , Gundersen, H. , Valdecanas, B. , Schulze, B. , Kaserzon, S. , Pijnappels, M. , Esperanza, M. , Fildier, A. , Vulliet, E. , Wiest, L. , Covaci, A. , Macan Schönleben, A. , Belova, L. , Celma, A. , Bijlsma, L. , Caupos, E. , Mebold, E. , Le Roux, J. , Troia, E. , de Rijke, E. , Helmus, R. , Leroy, G. , Haelewyck, N. , Chrastina, D. , Verwoert, M. and Thomaidis, N. (2024), Quantification Approaches in Non-Target LC/ESI/HRMS Analysis: An Interlaboratory Comparison, Analytical Chemistry (Accessed October 7, 2024)