HRMS-based suspect screening of pharmaceuticals and their transformation products in multiple environmental compartments: An alternative to target analysis?
J.M. Castaño-Ortiz, Pablo Gago-Ferrero, Damià Barceló, Sara Rodríguez‐Mozaz, Rubén Gil‐Solsona
Abstract
The comprehensive monitoring of pharmaceutically active compounds (PhACs) in the environment is challenging given the myriad of substances continuously discharged, the increasing number of new compounds being produced (and released), or the variety of the associated human metabolites and transformation products (TPs). Approaches such as high-resolution mass spectrometry (HRMS)-based suspect analysis have emerged to overcome the drawbacks of classical target analytical methods, e.g., restricted chemical coverage. In this study, we assess the readiness of HRMS-based suspect screening to replace or rather complement target methodologies by comparing the performance of both approaches in terms of i) detection of PhACs in various environmental samples (water, sediments, biofilm, fish plasma, muscle and liver) in a field study; ii) PhACs (semi)quantification and iii) prediction of their environmental risks. Our findings revealed that target strategies alone significantly underestimate the variety of PhACs potentially impacting the environment. However, relying solely on suspect strategies can misjudge the presence and risk of low-level but potentially risky PhACs. Additionally, semiquantitative approaches, despite slightly overestimating concentrations, can provide a realistic overview of PhACs concentrations. Hence, it is recommended to adopt a combined strategy that first evaluates suspected threats and subsequently includes the relevant ones in the established target methodologies. The ubiquity and ecotoxicological risks of pharmaceutical residues demand suitable analytical methodologies for their determination in the environment. By comparing the performance of target analysis and HRMS-based suspect screening, it was shown that target analysis alone can underestimate the environmental risk of a variety of pharmaceuticals, whereas the impacts of low-level compounds might be overlooked by HRMS-based suspect screening. Therefore, although the newest more sensitive HRMS instrumentation could narrow the gap between the two strategies, a combined strategy involving a preliminary screening followed by an accurate quantification of levels and risk is recommended for a comprehensive assessment of pharmaceutical pollution.