Occurrence of newly identified plasticizers in handwipes; development and validation of a novel analytical method and assessment of human exposure via dermal absorption.

A novel analytical method for the monitoring of four newly identified plasticizers, namely di-propylene glycol dibenzoate (DiPGDB), tri-n-butyl trimellitate (TBTM), isooctyl 2-phenoxyethyl terephthalate (IOPhET) and bis 3,5,5-trimethylhexyl phosphate (TMHPh), in handwipes based on pulverization was developed and in-house validated. In total, 164 handwipe samples (paired with house dust and human urine) were collected during winter (n = 82) and summer (n = 82) 2019 from adults and toddlers living in Flanders, Belgium. Method LOQs ranged from 1 to 200 ng/g. The ranges of Σplasticizers were 70-5400 ng/g for winter and 70-3720 ng/g for summer. The detection frequencies were 39% for DiPGDB, 27% for TBTM and <5% for IOPhET and TMHPh in winter samples and 33% for DiPGDB, 21% for TBTM and <10% for IOPhET and TMHPh in summer ones. The dominant compound in handwipes was DiPGDB, with mean contributions of 74% and 83% for winter and summer, followed by TBTM (24% and 9.2%), TMHPh (1.8% and 8.1%) and IOPhET (<1% and <1%). Σplasticizers concentrations were positively correlated in summer with the use of sanitizer (r = 0.375, p < 0.05) and negatively correlated in winter with the use of personal care products (r = -0.349, p < 0.05). DiPGDB was found positively correlated with the age of the participants (r = 0.363, p < 0.05) and the time spent indoors (r = 0.359, p < 0.05), indicating indoor environment as a potential source. Levels of TBTM in handwipes were positively correlated with dust samples collected from the same households (r = 0.597, p < 0.05), and those detected in toddler handwipes were significantly higher compared to adults (p < 0.05). Human daily exposure via dermal absorption was evaluated using the dermal derived no effects level values (DNEL), available in the database of the European Chemicals Agency (ECHA) and estimated using the theoretical bio-accessible fractions per compound. Toddler exposure to TBTM was significantly higher compared to adults (T-test, p < 0.05). No risk for adverse human health effects was derived from the comparison with DNELs for all compounds.

Suspect and non-targeted screening of chemicals of emerging concern for human biomonitoring, environmental health studies and support to risk assessment: From promises to challenges and harmonisation issues.

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.