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High-Resolution Mass Spectrometry for Human Exposomics: Expanding Chemical Space Coverage
In the modern “omics” era, measurement of the human exposome is a critical missing link between genetic drivers and disease outcomes. High-resolution mass spectrometry (HRMS), routinely used in proteomics and metabolomics, has emerged as a leading technology to broadly profile chemical exposure agents and related biomolecules for accurate mass measurement, high sensitivity, rapid data acquisition, and increased resolution of chemical space. Non-targeted approaches are increasingly accessible, supporting a shift from conventional hypothesis-driven, quantitation-centric targeted analyses toward data-driven, hypothesis-generating chemical exposome-wide profiling. However, HRMS-based exposomics encounters unique challenges. New analytical and computational infrastructures are needed to expand the analysis coverage through streamlined, scalable, and harmonized workflows and data pipelines that permit longitudinal chemical exposome tracking, retrospective validation, and multi-omics integration for meaningful health-oriented inferences. In this article, we survey the literature on state-of-the-art HRMS-based technologies, review current analytical workflows and informatic pipelines, and provide an up-to-date reference on exposomic approaches for chemists, toxicologists, epidemiologists, care providers, and stakeholders in health sciences and medicine. We propose efforts to benchmark fit-for-purpose platforms for expanding coverage of chemical space, including gas/liquid chromatography–HRMS (GC-HRMS and LC-HRMS), and discuss opportunities, challenges, and strategies to advance the burgeoning field of the exposome.
2024
2018
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The historical (1835–2020) dry deposition of major air pollutants (SO2, NOx, O3 and PM2.5) in the urban background in Oslo, Norway, in a situation that could represent the building facades, was approximated from reported fuel combustion, emission factors, air concentrations since 1960, and dry deposition velocities. The annual accumulated dry deposition (and thus not considering the removal processes) of the pollutants, together, was found to have varied from about 2.3 to 27 g m−2, with the maximum in the 1960s caused by high SO2 emissions from the combustion of fuel oils, and with 1.6 kg m−2 having deposited over all the years. The deposition of PM2.5 was found to have dominated from 1835, have increased to a maximum in 1875 and then slowly decreased. The SO2 deposition decreased to a low value around 1990. The NOx deposition was also at its highest in the 1960s to about 1970, it became the largest from the 1980s, and then showed a clear decrease from about 2010. The O3 deposition was lower in the years of the maximum total and NOx deposition. The dry deposition of O3 and NOx were found to be about similar in 2020, more than two times that of PM2.5 and more than four times that of SO2. The trends of the NOx emissions were found to reflect the relative (1975) and absolute (∼2000) turning points of the environmental Kuznets curves (EKC) that has been suggested for Norway, whereas the trend of the SO2 emissions seems to have “shortcut” this development by the strong regulations in the emissions from 1970 that lead to near simultaneous relative and absolute reductions. The gradual decrease of the PM2.5 emissions from about 1945 seems to correspond with the decrease in combustion energy intensity in the economy as wood was substituted with more energy efficient fuels and then with the continued reduction in the wood burning.
Elsevier
2021
2017
2007
We present the organization, instrumentation, datasets, data interpretation, modeling, and accomplishments of the multinational global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). AGAGE is distinguished by its capability to measure globally, at high frequency, and at multiple sites all the important species in the Montreal Protocol and all the important non-carbon-dioxide (non-CO2) gases assessed by the Intergovernmental Panel on Climate Change (CO2 is also measured at several sites). The scientific objectives of AGAGE are important in furthering our understanding of global chemical and climatic phenomena. They are the following: (1) to accurately measure the temporal and spatial distributions of anthropogenic gases that contribute the majority of reactive halogen to the stratosphere and/or are strong infrared absorbers (chlorocarbons, chlorofluorocarbons – CFCs, bromocarbons, hydrochlorofluorocarbons – HCFCs, hydrofluorocarbons – HFCs and polyfluorinated compounds (perfluorocarbons – PFCs), nitrogen trifluoride – NF3, sulfuryl fluoride – SO2F2, and sulfur hexafluoride – SF6) and use these measurements to determine the global rates of their emission and/or destruction (i.e., lifetimes); (2) to accurately measure the global distributions and temporal behaviors and determine the sources and sinks of non-CO2 biogenic–anthropogenic gases important to climate change and/or ozone depletion (methane – CH4, nitrous oxide – N2O, carbon monoxide – CO, molecular hydrogen – H2, methyl chloride – CH3Cl, and methyl bromide – CH3Br); (3) to identify new long-lived greenhouse and ozone-depleting gases (e.g., SO2F2, NF3, heavy PFCs (C4F10, C5F12, C6F14, C7F16, and C8F18) and hydrofluoroolefins (HFOs; e.g., CH2 = CFCF3) have been identified in AGAGE), initiate the real-time monitoring of these new gases, and reconstruct their past histories from AGAGE, air archive, and firn air measurements; (4) to determine the average concentrations and trends of tropospheric hydroxyl radicals (OH) from the rates of destruction of atmospheric trichloroethane (CH3CCl3), HFCs, and HCFCs and estimates of their emissions; (5) to determine from atmospheric observations and estimates of their destruction rates the magnitudes and distributions by region of surface sources and sinks of all measured gases; (6) to provide accurate data on the global accumulation of many of these trace gases that are used to test the synoptic-, regional-, and global-scale circulations predicted by three-dimensional models; and (7) to provide global and regional measurements of methane, carbon monoxide, and molecular hydrogen and estimates of hydroxyl levels to test primary atmospheric oxidation pathways at midlatitudes and the tropics. Network Information and Data Repository: http://agage.mit.edu/data or http://cdiac.ess-dive.lbl.gov/ndps/alegage.html (https://doi.org/10.3334/CDIAC/atg.db1001).
2018
Electrification of residential heating and investment in building energy efficiency are central pillars of many national strategies to reduce carbon emissions from the built environment sector. Ireland has a strong dependence on oil use for central heating and a substantial share of homes still using solid fuels. The current national strategy calls for the retrofitting of 400,000 home heating systems with heat pumps by 2030, principally replacing oil fired heating systems. Displacing natural gas, oil and solid fuel boilers with heat pumps will have a favourable impact on climate outcomes. However, the impact on air pollutant outcomes is far more favourable when solid fuels are replaced, and the positive impact on ambient air quality is much enhanced where concentrated clusters of solid-fuel use are targeted. This research spatially analyses emissions and air pollutant concentration outcomes for both targeted and non-targeted deployments of heat pumps and shows that a focused deployment of just 3% of the national heat pump target on solid-fuel homes could offer similar progress on climate goals but with a substantial impact in terms of reducing air pollution hot spots. For the Irish residential heating season (October–March), the targeted solid fuel scenario delivers average PM2.5 concentration decreases of 20–34%. This paper shows that these targeted communities are often in areas of relative deprivation, and as such, direct support for fabric retrofitting and heat pump technology installation offers the potential to simultaneously advance climate, air and just transition policy ambitions.
Elsevier
2022
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