Analysis of the lipid composition of bull spermatozoa by MALDI-TOF mass spectrometry—a cautionary note

Schiller, Jürgen; Müller, Karin; Süß, Rosemarie; Arnhold, Jürgen; Gey, Claudia; Herrmann, Andreas; Lessig, Jacqueline; Arnold, Klaus; Müller, Peter

doi:10.1016/s0009-3084(03)00097-5

Cited by 71 publications

(36 citation statements)

References 18 publications

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“…Although a MALDI-TOF mass spectrometric characterization of bull spermatozoa lipid extracts was already performed [21], corresponding data on the lipid composition of roe deer spermatozoa are not yet available. Therefore, the method how the PL analysis may be performed by MALDI-TOF MS in combination with chemical modifications of the organic spermatozoa extracts shall be shortly introduced.…”

Section: Resultsmentioning

confidence: 99%

Characteristic Oxidation Products of Choline Plasmalogens are Detectable in Cattle and Roe Deer Spermatozoa by MALDI‐TOF Mass Spectrometry

Fuchs

Müller

Göritz

et al. 2007

Lipids

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Plasmalogens (1-O-alk-1'-enyl-2-acyl-sn-glycero-3-phosphocholines and -phosphoethanolamines) are important constituents of spermatozoa membranes and possess significant antioxidative properties. This particularly holds as plasmalogens from spermatozoa also possess a very high content of highly unsaturated fatty acyl residues (especially 22:6). The organic spermatozoa extracts of two different ruminants (cattle and roe deer) were analyzed for their contents of characteristic choline plasmalogen oxidation products by matrix-assisted laser desorption and ionization time-of-flight (MALDI-TOF) mass spectrometry. It will be shown that 1-hydroxy-2-docosahexaenoyl-sn-glycero-3-phosphocholine (LPC 22:6) and formyl-LPC 22:6 are reliable measures of lipid oxidation of spermatozoa and allow, accordingly, conclusions about the storage conditions. All data on spermatozoa were also confirmed by the investigation of the oxidation behavior of selected reference compounds. It will be shown that, equally if plasmalogens or diacyl PC species are used, oxidation takes place primarily at the double bond next to the glycerol backbone. These data were additionally confirmed by recording the corresponding post source decay (PSD) fragment ion spectra.

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Section: Resultsmentioning

confidence: 99%

Characteristic Oxidation Products of Choline Plasmalogens are Detectable in Cattle and Roe Deer Spermatozoa by MALDI‐TOF Mass Spectrometry

Fuchs

Müller

Göritz

et al. 2007

Lipids

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“…By separating lipid classes prior to analysis the suppression effects of PC/SM are eliminated and low abundance lipid classes (such as PI) can be observed even from complex samples [81]. TLC/MALDI has shown much promise for the analysis of both phospholipids (PLs) and glycosphingolipids (GSLs) from extracts obtained from a diverse range of sources [79,[81][82][83][84][85]. Nevertheless it may be affected by: (i) incomplete desorption of lipids from the plate due to the high affinity of some lipids for 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 13 silica; (ii) poor penetration of the UV-laser beam into the silica layer such that only lipids close to the surface are removed; and (iii) the possibility of ablating and contaminating the instrument with silica.…”

Section: Matrix-assisted Laser Desorption Ionization (Maldi)mentioning

confidence: 99%

Surface analysis of lipids by mass spectrometry: More than just imaging

Ellis

Brown

Panhuis

et al. 2013

Progress in Lipid Research

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Mass spectrometry is now an indispensable tool for lipid analysis and is arguably the driving force in the renaissance of lipid research. In its various forms, mass spectrometry is uniquely capable of resolving the extensive compositional and structural diversity of lipids in biological systems. Furthermore, it provides the ability to accurately quantify molecular-level changes in lipid populations associated with changes in metabolism and environment; bringing lipid science to the "omics" age. The recent explosion of mass spectrometry-based surface analysis techniques is fuelling further expansion of the lipidomics field. This is evidenced by the numerous papers published on the subject of mass spectrometric imaging of lipids in recent years. While imaging mass spectrometry provides new and exciting possibilities, it is but one of the many opportunities direct surface analysis offers the lipid researcher. In this review we describe the current state-ofthe-art in the direct surface analysis of lipids with a focus on tissue sections, intact cells and thin-layer chromatography substrates. The suitability of these different approaches towards analysis of the major lipid classes along with their current and potential applications in the field of lipid analysis are evaluated. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 2 AbstractMass spectrometry is now an indispensable tool for lipid analysis and is arguably the driving force in the renaissance of lipid research. In its various forms, mass spectrometry is uniquely capable of resolving the extensive compositional and structural diversity of lipids in biological systems. Furthermore, it provides the ability to accurately quantify molecular-level changes in lipid populations associated with changes in metabolism and environment;bringing lipid science to the "omics" age. The recent explosion of mass spectrometry-based surface analysis techniques is fuelling further expansion of the lipidomics field. This is evidenced by the numerous papers published on the subject of mass spectrometric imaging of lipids in recent years. While imaging mass spectrometry provides new and exciting possibilities, it is but one of the many opportunities direct surface analysis offers the lipid researcher. In this review we describe the current state-of-the-art in the direct surface analysis of lipids with a focus on tissue sections, intact cells and thin-layer chromatography substrates.The suitability of these different approaches towards analysis of the major lipid classes along with their current and potential applications in the field of lip...

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“…The lipid extract of mouse serum was performed using the method of Schiller et al [14], modified from Bligh and Dyer [15]. Twenty microliters of serum were vortexed with 75 l methanol/CHCl 3 2:1 for 1 min.…”

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confidence: 99%

Enhanced MALDI ionization efficiency at the metal-matrix interface: Practical and mechanistic consequences of sample thickness and preparation method

McCombie

Knochenmuss

2006

J. Am. Soc. Mass Spectrom.

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Electrosprayed spots of varying thickness were evaluated for use as reproducible, homogenous, high efficiency MALDI samples. Thin samples on stainless steel plates were found to give exceptionally strong signals, as did the last layers of thick samples, when ablated down to the steel substrate. A small enhancement was also observed for thin samples on a gold substrate, and with a few-nanometer gold coating on top of a thick sample. Ion yields and intensity ratios can be understood in the context of the previously described quantitative MALDI model including the matrix-metal interfacial ionization potential reduction effect (Knochenmuss, R.; Anal. Chem. 2004, 76, 3179 -3184). The absolute and relative stabilities of ion signals were found to be at least a factor of two better for the thin electrosprayed spots, , both the underlying ionization mechanisms and sample preparation methods remain objects of active study. These are coupled topics since mechanistic understanding can allow rational, rather than undirected, method development. Here, we make use of a recently developed quantitative model for UV-MALDI based on a two-step ionization process [2,3]. Primary laser-created matrix ions and analyte neutrals undergo ion-molecule reactions in the expanding ablation plume to yield secondary analyte ions. The observed mass spectrum is determined by the thermodynamics of these reactions. Because matrix and analyte are explicitly coupled, the model proved particularly suitable for understanding of practically relevant phenomena such as ion suppression effects [4 -6], which have been shown to be very common phenomena [7].A variant of this model has recently been developed for thin samples on metal substrates [8]. This was motivated by measurements of electron emission yields from MALDI samples on metallic versus insulating substrates [9], and suggestions that such electrons might neutralize (positive) analyte ions during the desorption process [10]. The model gave excellent agreement with the electron yield data, but this was not consistent with claims of higher analyte ion yields for samples on nonconductive versus conductive substrates [9]. The major difference between thick and thin samples is the interaction of matrix molecules with the substrate, which can lower the ionization potential of the combined system if the substrate is metal. It was, therefore, theoretically expected that thin samples on metal would yield higher, not lower, signals. The present study was undertaken to investigate this discrepancy and restore consistency to sample preparation strategy.The method selected here to prepare homogenous samples of variable thickness is electrospray (ES) deposition of analyte/matrix solution [11,12]. Electrospray produces more uniform, fine-grained sample spots than the more convenient and widespread dried droplet technique, which tends to form large matrix crystals in random locations. By varying the electrospray time, it is also possible to make samples as thin as a few hundred nanometers, but a few mm in diamete...

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Analysis of the lipid composition of bull spermatozoa by MALDI-TOF mass spectrometry—a cautionary note

Cited by 71 publications

References 18 publications

Characteristic Oxidation Products of Choline Plasmalogens are Detectable in Cattle and Roe Deer Spermatozoa by MALDI‐TOF Mass Spectrometry

Characteristic Oxidation Products of Choline Plasmalogens are Detectable in Cattle and Roe Deer Spermatozoa by MALDI‐TOF Mass Spectrometry

Surface analysis of lipids by mass spectrometry: More than just imaging

Enhanced MALDI ionization efficiency at the metal-matrix interface: Practical and mechanistic consequences of sample thickness and preparation method

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