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Suspect and non-targeted screening approaches are a matter of increasing interest notably with regard to the Exposome contextual framework, but their application to human samples still remains limited at this date. The aim of the present study was to develop a non-targeted workflow from sample preparation to data processing and method assessment to characterise the human internal chemical exposure at early life stage. The method was focused on human milk to investigate mother and newborn exposure to known organic contaminants and to extend the characterisation to unknown compounds. We specifically focused on halogenated biomarkers of exposure due to persistence and potential toxicological impact reasons. The newly developed approach was based on a simple and fast sample preparation followed by a comprehensive analysis by both liquid and gas phase chromatography coupled to high resolution mass spectrometry. Critical steps of the non-targeted workflow as the method assessment have been addressed with a reference mix of 30 chlorinated and brominated contaminants encompassing various substances groups and a statistical approach. Data processing until the identification of biomarkers of exposure was possible with homemade bioinformatics tools. On the other hand, the method was validated by the identification of historical chemicals as hexachlorobenzene and p,p'-DDE and emerging chemical as 4-hydroxychlorothalonil. This approach opens the door to further extensions and consolidations to offer new capabilities for exposomics and environmental health research. Image 1 • To 5 highlights; Maximum 85 characters including spaces per bullet point. • Non-targeted screening workflow development and assessment. • LC- and GC-HRMS complementarity with dedicated data processing. • Human milk investigation to support the European project HBM4EU. • Identification of historical and emerging contaminants by NTS approach. [ABSTRACT FROM AUTHOR]

• Chemicals of Emerging Concern (CECs) are a growing concern in HBM. • Suspect and non-targeted screening (NTS) approaches offer new capabilities for capturing CECs in human matrices. • These new approaches applied to HBM come with a number of technical and scientific issues to be addressed. • Harmonisation is required at international level to reinforce NTS methods comparability and performance assessment. Large-scale suspect and non-targeted screening approaches based on high-resolution mass spectrometry (HRMS) are today available for chemical profiling and holistic characterisation of biological samples. These advanced techniques allow the simultaneous detection of a large number of chemical features, including markers of human chemical exposure. Such markers are of interest for biomonitoring, environmental health studies and support to risk assessment. Furthermore, these screening approaches have the promising capability to detect chemicals of emerging concern (CECs), document the extent of human chemical exposure, generate new research hypotheses and provide early warning support to policy. Whilst of growing importance in the environment and food safety areas, respectively, CECs remain poorly addressed in the field of human biomonitoring. This shortfall is due to several scientific and methodological reasons, including a global lack of harmonisation. In this context, the main aim of this paper is to present an overview of the basic principles, promises and challenges of suspect and non-targeted screening approaches applied to human samples as this specific field introduce major specificities compared to other fields. Focused on liquid chromatography coupled to HRMS-based data acquisition methods, this overview addresses all steps of these new analytical workflows. Beyond this general picture, the main activities carried out on this topic within the particular framework of the European Human Biomonitoring initiative (project HBM4EU, 2017–2021) are described, with an emphasis on harmonisation measures. [ABSTRACT FROM AUTHOR]