A large scale multi-laboratory suspect screening of pesticide metabolites in human biomonitoring: From tentative annotations to verified occurrences

Huber, Carolin; Nijssen, Rosalie; Mol, Hans; Antignac, Jean‐Philippe; Krauß, Martin; Brack, Werner; Wagner, Kévin; Debrauwer, Laurent; Vitale, Chiara Maria; Price, Elliott J.; Klánová, Jana; Garlito, Borja; León, Núria; Pardo, Olga; Fernández, Sandra F.; Szigeti, Tamás; Középesy, Szilvia; Šulc, Libor; Čupr, Pavel; Mārtiņsone, Inese; Akūlova, Lāsma; Ottenbros, Ilse; Vermeulen, Roel; Vlaanderen, Jelle; Luijten, Mirjam; Lommen, Arjen

doi:10.1016/j.envint.2022.107452

Cited by 25 publications

(7 citation statements)

References 48 publications

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“…In a large majority of the samples (84%) two or more different pesticides were detected. Our findings confirm the presence of mixtures and the necessity of assessing co-occurrent exposures, which is a topic of high concern in risk assessment (European Commission, 2020; Socianu et al, 2022;Luijten et al, 2022). The number of co-occurring pesticides typically ranged from 2 to 5, with a maximum of 13 different pesticides (2 urine samples).…”

Section: Co-occurrencesupporting

confidence: 76%

Approaches to identify exposure to real-life chemical mixtures in the general population

Ottenbros

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Humans are exposed to large number of chemicals from various sources in their environment. Current risk assessment approaches often focus on single chemicals, sources or routes, not accounting for possible combinations of chemicals and overlooking potential additional risks associated with chemical mixtures. This thesis focusses on how to accurately measure and describe exposure patterns of chemical mixtures in the general population. Measuring exposure to chemical mixtures in real-life situations at a population level is a complex task. The preferably individual measurements can be obtained either externally (e.g. silicone wristbands) or internally (human biomonitoring). In my thesis, chemical mixtures are described as combinations of manufactured chemicals that co-occur within the same individual or sample. My thesis revolves around three different approaches to identify chemical mixtures in the general population. 1) The first approach focusses on describing co-occurrence patterns of chemicals in existing human biomonitoring datasets, combining a graphical correlation network model with a clustering algorithm. This method visualizes and summarizes these co-occurrence patterns by identifying highly correlated groups or clusters of chemicals. We demonstrated that presenting biomonitoring data in networks facilitates the identification of exposure patterns that contribute to the observed exposure levels in the samples. The application of community detection with a clustering algorithm was instrumental in identifying patterns within and between chemical families. 2) The second approach involves measuring chemical mixtures at individual level, employing external and internal measurements. 3) The third approach refers to the analytical measurement of chemical mixtures in urine samples, for which a suspect screening approach based on high resolution mass spectrometry was applied, enabling detection of a broad range of biomarkers in a single sample. The second and third approach were applied on pesticides, as an example of a mixture of chemicals. By utilization of wristbands we were able to detect multiple pesticides over a longer period of time, reflecting highly individual exposure profiles. It was demonstrated that a harmonized pan-European sample collection, combined with suspect screening provided valuable new insights into the presence of pesticide mixture exposure in the European population. Forty pesticide biomarkers corresponding to 29 different pesticides were confidently identified across six countries. Some variation but no consistent pattern in the probability of detection of pesticide biomarkers was observed based on residential location or season of urine sampling. Pesticide mixture patterns in the adult populations of the Netherlands and Switzerland were analyzed by their semi-quantitative levels. Urinary concentrations of the two most frequently detected pesticides (acetamiprid and chlorpropham) showed an inverse association with high organic vegetable and fruit consumption. In both countries, detection rates and co-occurrence of pesticides in the same urine sample were typically low. This thesis highlights the importance of understanding and measuring the mixture of chemicals we encounter. Knowledge of what these mixtures are helps us to figure out the risks to human health. I recommend to incorporate the approaches of this thesis in future studies to learn more about human exposure to chemical mixtures, and that research and sharing data is conducted in a harmonized way.

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Section: Co-occurrencesupporting

confidence: 76%

Approaches to identify exposure to real-life chemical mixtures in the general population

Ottenbros

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“…Another possible contaminant entering through the diet was quinmerac, an herbicide which has recently attracted the attention of the scientific community, as it has been determined in urine samples under the HBM4EU project [ 52 ]. Similarly, methylparaben (MeP) and propylparaben (PrP), chemicals, which are known as endocrine-disrupting chemicals [ 53 ] and commonly used as preservatives in personal care products, have been determined in 70% of the samples, ranging between nd–1.48 ng·mL −1 (MeP), and between nd–40.7 ng·mL −1 (PrP).…”

Section: Resultsmentioning

confidence: 99%

Comprehensive profiling and semi-quantification of exogenous chemicals in human urine using HRMS-based strategies

Gutiérrez-Martín,

Restrepo-Montes,

Golovko

et al. 2023

Anal Bioanal Chem

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Chemicals infiltrate our daily experiences through multiple exposure pathways. Human biomonitoring (HBM) is routinely used to comprehensively understand these chemical interactions. Historically, HBM depended on targeted screening methods limited to a relatively small set of chemicals with triple quadrupole instruments typically. However, recent advances in high-resolution mass spectrometry (HRMS) have facilitated the use of broad-scope target, suspect, and non-target strategies, enhancing chemical exposome characterization within acceptable detection limits. Despite these advancements, establishing robust and efficient sample treatment protocols is still essential for trustworthy broad-range chemical analysis. This study sought to validate a methodology leveraging HRMS-based strategies for accurate profiling of exogenous chemicals and related metabolites in urine samples. We evaluated five extraction protocols, each encompassing various chemical classes, such as pharmaceuticals, plastic additives, personal care products, and pesticides, in terms of their extraction recoveries, linearity, matrix effect, sensitivity, and reproducibility. The most effective protocol was extensively validated and subsequently applied to 10 real human urine samples using wide-scope target analysis encompassing over 2000 chemicals. We successfully identified and semi-quantified a total of 36 chemicals using an ionization efficiency-based model, affirming the methodology’s robust performance. Notably, our results dismissed the need for a deconjugation step, a typically labor-intensive and time-consuming process. Graphical Abstract

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“…A large‐scale human biomonitoring survey conducted in Europe between 2014 and 2021 identified at least 46 pesticides and their metabolites in adults and children across five European countries, with at least two pesticides detected in 84% of the samples collected. The ISA study has provided critical insight into health‐related effects of pesticides on the respiratory system, nervous system and reproductive system in mothers and infants 103–106 …”

Section: Key Guidance and Recommendationsmentioning

confidence: 99%

EAACI guidelines on environmental science for allergy and asthma: The impact of short‐term exposure to outdoor air pollutants on asthma‐related outcomes and recommendations for mitigation measures

Agache,

Annesi‐Maesano,

Cecchi

et al. 2024

Allergy

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The EAACI Guidelines on the impact of short‐term exposure to outdoor pollutants on asthma‐related outcomes provide recommendations for prevention, patient care and mitigation in a framework supporting rational decisions for healthcare professionals and patients to individualize and improve asthma management and for policymakers and regulators as an evidence‐informed reference to help setting legally binding standards and goals for outdoor air quality at international, national and local levels. The Guideline was developed using the GRADE approach and evaluated outdoor pollutants referenced in the current Air Quality Guideline of the World Health Organization as single or mixed pollutants and outdoor pesticides. Short‐term exposure to all pollutants evaluated increases the risk of asthma‐related adverse outcomes, especially hospital admissions and emergency department visits (moderate certainty of evidence at specific lag days). There is limited evidence for the impact of traffic‐related air pollution and outdoor pesticides exposure as well as for the interventions to reduce emissions. Due to the quality of evidence, conditional recommendations were formulated for all pollutants and for the interventions reducing outdoor air pollution. Asthma management counselled by the current EAACI guidelines can improve asthma‐related outcomes but global measures for clean air are needed to achieve significant impact.

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A large scale multi-laboratory suspect screening of pesticide metabolites in human biomonitoring: From tentative annotations to verified occurrences

Cited by 25 publications

References 48 publications

Approaches to identify exposure to real-life chemical mixtures in the general population

Approaches to identify exposure to real-life chemical mixtures in the general population

Comprehensive profiling and semi-quantification of exogenous chemicals in human urine using HRMS-based strategies

EAACI guidelines on environmental science for allergy and asthma: The impact of short‐term exposure to outdoor air pollutants on asthma‐related outcomes and recommendations for mitigation measures

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