Lipidomes, shotgun

X. L. Han and R. W. Gross, Shotgun lipidomics Electrospray ionization mass spectrometric analysis and quantitation of cellular lipidomes directly from crude extracts of biological samples, Mass Spectrom. Rev., 24 (2005) 367-412. 

X. L. Han and H. Cheng, Characterization and direct quantitation of cerebroside molecular species from lipid extracts by shotgun lipidomics, J. Lipid Res., 46 (2005) 163-175. 

In lipidomics, MS can be used either by direct infusion, that is, by the so-called shotgun MS, or in combination with chromatographic separation, typically LC and sometimes also with GC. Both approaches have their own advantages and limitations. Most targeted lipid analyses are performed with liquid chromatography coupled to mass spectrometry (LC-MS), while the use of gas chromatography-mass spectrometry (GC-MS) is utilized only for the analysis of fatty acids and some steroids. In addition, surface analysis by MS has been applied in lipid analysis of intact tissues. 

Han, X. 2011. Shotgun Lipidomics, from http //lipidlibrary.aocs.org/lipidomics/shot-gun-Han/index.htm. accessed April 2011. 

As mentioned above, two different mass spectrometric approaches to lipid analysis exist The first one is performed directly from lipid extracts without prior chromatographic separation and is referred to as shotgun lipidomics. Here, lipid classes are separated in the ion source according to their intrinsic electrical properties (24). Detailed and unambiguous structural and quantitative analysis of individual species is obtained by means of multiplexed mass spectrometry using NL, PIS, and... 

Han X, Yang J, Yang K, Zhao Z, Abendschein DR, Gross RW. 50. Alterations in myocardial cardiolipin content and composition occur at the very earliest stages of diabetes a shotgun lipidomics study. Biochemistry. 2007 46 6417-6428. 

By using the direct-infusion approach based on ESI-MS, multidimensional MS-based shotgun lipidomics (MDMS-SL) has also demonstrated to be a... 

Su X., Han X., Mancuso D.J., Abendschein D.R., Gross R.W. Accumulation of long-chain acylcarnitine and 3-hydroxy acylcarnitine molecular species in diabetic myocardium identification of alterations in mitochondrial fatty acid processing in diabetic myocardium by shotgun lipidomics. Biochemistry 44 (2005) 5234-5245. 

Shevchenko and colleagues have developed a somewhat different form of shotgun lipidomics which is particularly suitable to applications utilizing a hybrid linear ion trap (LIT) Fourier transform (FT) instrument, for example, LTQ-Orbitrap, called top-down lipidomics [18,24]. In a top-down lipidomics experiment, the survey scan is recorded at high resolution (100,000) (full width at half maximum height [FWMH]) in the FT analyzer. Mass accuracy on FT instruments is typically <5 ppm and often with internal calibration <2 ppm. This degree of mass accuracy... 

Quantification in shotgun lipidomics requires the addition of internal standards. Internal standards should be added during the extraction step and should consist of at least one standard for each lipid class. 

Figure 2.4 MDMS of a chloroform extract of mouse retina prepared by a modified Bligh and Dyer method [25]. Direct-infusion ESI spectra were acquired directly from the diluted lipid extract (total Upid 50 pmol/pL) using a TSQ Quantum Ultra tandem quadrupole instrument. The first (x) dimension is represented in the top panel (negative-ion ESI-MS). The second dimension (y) is represented by successive neutral-loss (NL) and precmsor-ion (PI) scans. All traces were displayed after normalization to the base peak in each spectrum. Internal standard (IS) m n, acyl chain containing m carbons and n double bonds. (Modified with permission from Han, X. et al., 2005, Shotgun Lipidomics of Phosphoethanolamine-Containing Lipids in Biological Samples after One-Step in Situ Derivatization, /. Upid Res. 46 1548-60.)...

Han, X. 2010. Multi-dimensional mass spectrometry-based shotgun lipidomics and the altered lipids at the mild cognitive impairment stage of Alzheimer s disease. Biochim. Biophys. Acta 1801 774-83. 

Han, X., Yang, K., Cheng, H., Pikes, K. N., and Gross, R. W. 2005. Shotgun lipidomics of phosphoethanolamine-containing lipids in biological samples after one-step in situ derivatization. /. Lipid Res. 46 1548-60. 

Figure 12.18. Shotgun lipidomics using ESI intrasource separation and multidimensional mass spectrometry of lipids from a complex extract. (From refs. 65 and 66.)...

Through global lipidomics, each distinct lipid species present in a cell s lip-idome can be identified. A shotgun lipidomics approach, which uses an ESI-intrasource separation of Upids from a complex extract, multidimensional mass spectrometry, and computer-assisted array analysis, is described. 

X. Han and R. W. Gross, New Developments in Multi-Dimensional Mass Spectrometry Based Shotgun Lipidomics , in Metabolomics, Metabonomics and Metabolite Profiling, ed. W. J. Griffiths, Royal Society of Chemistry, Cambridge, UK, 2008, p. 134. 

Yang, K., Jenkins, C.M., Dilthey, B. and Gross, R.W. (2015) Multidimensional mass spectrometry-based shotgun lipidomics analysis of vinyl ether diglyceiides. Anal. Bioanal. Chem. 407, 5199-5210. 

Yang, K., Zhao, Z., Gross, R.W. and Han, X. (2007) Shotgun lipidomics identifles a paired rule for the presence of isomeric ether phospholipid molecular species. PLoS ONE 2, el368. 

Cheng, H., Jiang, X. and Han, X. (2007) Alterations in lipid homeostasis of mouse dorsal root ganglia induced by apolipoprotein E deficiency A shotgun lipidomics study. J. Neurochem. 101, 57-76. 

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