The concept of the
exposome was introduced over 15 years ago to
reflect the important role that the environment exerts on health and
disease. While originally viewed as a call-to-arms to develop more
comprehensive exposure assessment methods applicable at the individual
level and throughout the life course, the scope of the exposome has
now expanded to include the associated biological response. In order
to explore these concepts, a workshop was hosted by the Gunma University
Initiative for Advanced Research (GIAR, Japan) to discuss the scope
of exposomics from an international and multidisciplinary perspective.
This Global Perspective is a summary of the discussions with emphasis
on (1) top-down, bottom-up, and functional approaches to exposomics,
(2) the need for integration and standardization of LC- and GC-based
high-resolution mass spectrometry methods for untargeted exposome
analyses, (3) the design of an exposomics study, (4) the requirement
for open science workflows including mass spectral libraries and public
databases, (5) the necessity for large investments in mass spectrometry
infrastructure in order to sequence the exposome, and (6) the role
of the exposome in precision medicine and nutrition to create personalized
environmental exposure profiles. Recommendations are made on key issues
to encourage continued advancement and cooperation in exposomics.
Fine particulate-matter is an important component of air pollution that impacts health and climate, and which delivers anthropogenic contaminants to remote global regions. The complex composition of organic molecules in atmospheric particulates is poorly constrained, but has important implications for understanding pollutant sources, climate-aerosol interactions, and health risks of air pollution exposure. Here, comprehensive nontarget high-resolution mass spectrometry was combined with in silico structural prediction to achieve greater molecular-level insight for fine particulate samples (n = 40) collected at a remote receptor site in the Maldives during January to April 2018. Spectral database matching identified 0.5% of 60,030 molecular features observed, while a conservative computational workflow enabled structural annotation of 17% of organic structures among the remaining molecular dark matter. Compared to clean air from the southern Indian Ocean, molecular structures from highly-polluted regions were dominated by organic nitrogen compounds, many with computed physicochemical properties of high toxicological and climate relevance. We conclude that combining nontarget analysis with computational mass spectrometry can advance molecular-level understanding of the sources and impacts of polluted air.
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