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Molecular speciation and dynamics of oxidized triacylglycerols in lipid droplets : Mass spectrometry and coarse-grained simulations
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Mohammadyani, Dariush, Tyurin, Vladimir A., O׳Brien, Matthew, Sadovsky, Yoel, Gabrilovich, Dmitry I., Klein-Seetharaman, Judith and Kagan, Valerian E. (2014) Molecular speciation and dynamics of oxidized triacylglycerols in lipid droplets : Mass spectrometry and coarse-grained simulations. Free Radical Biology and Medicine, Volume 76 . pp. 53-60. doi:10.1016/j.freeradbiomed.2014.07.042 ISSN 0891-5849.
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Official URL: http://dx.doi.org/10.1016/j.freeradbiomed.2014.07....
Abstract
Lipid droplets (LDs) are ubiquitous and physiologically active organelles regulating storage and mobilization of lipids in response to metabolic demands. Among the constituent LD neutral lipids, such as triacylglycerols, cholesterol esters, and free fatty acids, oxidizable polyunsaturated molecular species may be quite abundant, yet the structural and functional roles of their oxidation products have not been studied. Our previous work documented the presence of these peroxidized species in LDs. Assuming that hydrophilic oxygen-containing functionalities may markedly change the hydrophobic/hydrophilic molecular balance, here we utilized computational modeling to test the hypothesis that lipid peroxidation causes redistribution of lipids between the highly hydrophobic core and the polar surface (phospho)lipid monolayer-the area enriched with integrated enzymatic machinery. Using quantitative liquid chromatography/mass spectrometry, we characterized molecular speciation of oxTAGs in LDs of dendritic cells in cancer and hypoxic trophoblasts cells as two cellular models associated with dyslipidemia. Among the many types of oxidized lipids identified, we found that oxidatively truncated forms and hydroxyl derivatives of TAGs were the prevailing oxidized lipid species in LDs in both cell types. Using coarse-grained molecular dynamics (CG-MD) simulations we established that lipid oxidation changed their partitioning whereby oxidized lipids migrated into the outer monolayer of the LD, where they can affect essential metabolic pathways and undergo conversions, possibly leading to the formation of oxygenated lipid mediators.
Item Type: | Journal Article | ||||||
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Divisions: | Faculty of Science, Engineering and Medicine > Medicine > Warwick Medical School > Biomedical Sciences > Translational & Experimental Medicine > Metabolic and Vascular Health (- until July 2016) Faculty of Science, Engineering and Medicine > Medicine > Warwick Medical School |
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Journal or Publication Title: | Free Radical Biology and Medicine | ||||||
Publisher: | Elsevier Science Inc. | ||||||
ISSN: | 0891-5849 | ||||||
Official Date: | November 2014 | ||||||
Dates: |
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Volume: | Volume 76 | ||||||
Page Range: | pp. 53-60 | ||||||
DOI: | 10.1016/j.freeradbiomed.2014.07.042 | ||||||
Status: | Peer Reviewed | ||||||
Publication Status: | Published | ||||||
Access rights to Published version: | Restricted or Subscription Access |
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