Abstract
Complementing the genome with an understanding of the human exposome is an important challenge for contemporary science and technology. Tens of thousands of chemicals are used in commerce, yet cost for targeted environmental chemical analysis limits surveillance to a few hundred known hazards. To overcome limitations which prevent scaling to thousands of chemicals, we develop a single-step express liquid extraction and gas chromatography high-resolution mass spectrometry analysis to operationalize the human exposome. We show that the workflow supports quantification of environmental chemicals in human plasma (200 µL) and tissue (≤100 mg) samples. The method also provides high resolution, sensitivity and selectivity for exposome epidemiology of mass spectral features without a priori knowledge of chemical identity. The simplicity of the method can facilitate harmonization of environmental biomonitoring between laboratories and enable population level human exposome research with limited sample volume.
Highlights
Complementing the genome with an understanding of the human exposome is an important challenge for contemporary science and technology
Compared with using dispersive solid-phase extraction (SPE) based on the QuEChERS procedure, we found similar reproducibility using high-purity MgSO4 to prepare standard reference material (SRM) of human serum and human plasma samples for Gas chromatography (GC)–HRMS analysis and slightly higher recovery of targeted chemicals using MgSO4 (Supplementary Fig. 2)
The results of total ion intensity calculated by the sum of all Mass spectrometry (MS) peak intensities showed that the signals in saline extracted by XLE matched the baseline signals found in the directly injected isooctane solvent (Fig. 2b)
Summary
Complementing the genome with an understanding of the human exposome is an important challenge for contemporary science and technology. An analytical workflow to operationalize untargeted environmental biomonitoring is needed to gain information on known as well as unknown exposures for human exposome research. In contrast to targeted MS analysis, which is developed to measure specific chemicals, untargeted exposome analysis includes measures of known chemicals that are “identified” by MS criteria, and other MS signals that are unidentified because they have not been associated with known chemicals by MS criteria[6] These unidentified signals include chemical contaminants that are known and uncharacterized, as well as reaction products that are effectively unknown to science; the capability to measure these unidentified chemicals in biologic samples is essential to enable population health studies of the dark matter of the exposome. Collection of all spectral features enables measurement of known targets based on libraries of authentic standards, while reproducibly measuring and preserving information for unidentified MS features
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