I urval från Stockholms universitets publikationsdatabas

• Phospholipid Removal for Enhanced Chemical Exposomics in Human Plasma

  2023. Kalliroi Sdougkou (et al.). Environmental Science and Technology 57, 10173-10184

  Artikel

  Chemical exposomics in human plasma wasenhanced by an optimizedphospholipid removal step that increased targeted method sensitivitywhile also revealing >13,000 new molecular features by LC-HRMSnon-targetedacquisition. The challenge of chemical exposomics in human plasmais the 1000-foldconcentration gap between endogenous substances and environmentalpollutants. Phospholipids are the major endogenous small moleculesin plasma, thus we validated a chemical exposomics protocol with anoptimized phospholipid-removal step prior to targeted and non-targetedliquid chromatography high-resolution mass spectrometry. Increasedinjection volume with negligible matrix effect permitted sensitivemulticlass targeted analysis of 77 priority analytes; median MLOQ= 0.05 ng/mL for 200 & mu;L plasma.In non-targeted acquisition, mean total signal intensities of non-phospholipidswere enhanced 6-fold in positive (max 28-fold) and 4-fold in negativemode (max 58-fold) compared to a control method without phospholipidremoval. Moreover, 109 and 28% more non-phospholipid molecular featureswere detected by exposomics in positive and negative mode, respectively,allowing new substances to be annotated that were non-detectable withoutphospholipid removal. In individual adult plasma (100 & mu;L, n = 34), 28 analytes were detected and quantified among10 chemical classes, and quantitation of per- and polyfluoroalkylsubstances (PFAS) was externally validated by independent targetedanalysis. Retrospective discovery and semi-quantification of PFAS-precursorswas demonstrated, and widespread fenuron exposure is reported in plasmafor the first time. The new exposomics method is complementary tometabolomics protocols, relies on open science resources, and canbe scaled to support large studies of the exposome.

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• Nontarget mass spectrometry and in silico molecular characterization of air pollution from the Indian subcontinent

  2022. Stefano Papazian (et al.). Communications Earth & Environment 3 (1)

  Artikel

  A combination of high-resolution mass spectrometry and computational molecular characterization techniques can structurally annotate up to 17% of organic compounds in fine particulate matter in highly polluted air sampled in the Maldives. 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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• Defining the Scope of Exposome Studies and Research Needs from a Multidisciplinary Perspective

  2021. Pei Zhang (et al.). Environmental Science and Technology Letters 8 (10), 839-852

  Artikel

  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.

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• Silicone Foam for Passive Sampling and Nontarget Analysis of Air

  2023. Stefano Papazian (et al.). Environmental Science and Technology Letters 10 (11), 989-997

  Artikel

  The airborne chemical exposome is a dynamic complex mixture of gases and particles, and despite clear links to chronic disease and premature death, its molecular composition and variability remains largely uncharacterized. To overcome this, we aimed to pair nontarget analysis by high-resolution mass spectrometry (HRMS) with an inexpensive and stable passive sampling media for airborne gases and particles. To this end, we synthesized silicone (polydimethylsiloxane; PDMS) foam disks resulting in a low cost (0.02$/disk) and ultraclean material suitable for analysis by gas or liquid chromatography (GC/LC)HRMS. When tested for indoor passive sampling over 1-3 months, alongside a PDMS sheet, PDMS foam accumulated many nonpolar gas phase environmental contaminants (e.g., polychlorinated biphenyls), and a surprisingly complex mixture of larger polar substances (e.g., oxygen, nitrogen and sulfur-containing) that were absent from the PDMS sheet, suggesting sampling of the particulate phase. The airborne molecular discovery potential was further demonstrated using an open-science LC-HRMS workflow integrating molecular networks and in silico structural predictions tailored on PubChemLite for Exposomics, which revealed series of known and unknown substances, including aromatic nitrophenols and sulfonyls. Future studies may benefit from implementing PDMS foam as wearable or stationary passive samplers to support advances in understanding exposure and contaminant sources in the indoor, outdoor, and personal airborne exposomes.

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