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Trapped ion mobility spectrometry and PASEF enable in-depth lipidomics from minimal sample amounts.
Nature Communications ( IF 14.7 ) Pub Date : 2020-01-16 , DOI: 10.1038/s41467-019-14044-x
Catherine G Vasilopoulou 1 , Karolina Sulek 2 , Andreas-David Brunner 1 , Ningombam Sanjib Meitei 3 , Ulrike Schweiger-Hufnagel 4 , Sven W Meyer 4 , Aiko Barsch 4 , Matthias Mann 1, 2 , Florian Meier 1
Affiliation  

A comprehensive characterization of the lipidome from limited starting material remains very challenging. Here we report a high-sensitivity lipidomics workflow based on nanoflow liquid chromatography and trapped ion mobility spectrometry (TIMS). Taking advantage of parallel accumulation-serial fragmentation (PASEF), we fragment on average 15 precursors in each of 100 ms TIMS scans, while maintaining the full mobility resolution of co-eluting isomers. The acquisition speed of over 100 Hz allows us to obtain MS/MS spectra of the vast majority of isotope patterns. Analyzing 1 µL of human plasma, PASEF increases the number of identified lipids more than three times over standard TIMS-MS/MS, achieving attomole sensitivity. Building on high intra- and inter-laboratory precision and accuracy of TIMS collisional cross sections (CCS), we compile 1856 lipid CCS values from plasma, liver and cancer cells. Our study establishes PASEF in lipid analysis and paves the way for sensitive, ion mobility-enhanced lipidomics in four dimensions.

中文翻译:

俘获离子迁移谱和 PASEF 能够从最少的样品量中进行深入的脂质组学。

从有限的起始材料中全面表征脂质组仍然非常具有挑战性。在这里,我们报告了基于纳流液相色谱和捕获离子迁移谱 (TIMS) 的高灵敏度脂质组学工作流程。利用并行累积-串行碎裂 (PASEF),我们在每次 100 ms TIMS 扫描中平均裂解 15 个前体,同时保持共流出异构体的完整迁移率分辨率。超过 100 Hz 的采集速度使我们能够获得绝大多数同位素模式的 MS/MS 谱。与标准 TIMS-MS/MS 相比,PASEF 分析 1 µL 人血浆时可将识别出的脂质数量增加三倍以上,从而实现阿托摩尔灵敏度。基于 TIMS 碰撞截面 (CCS) 的高实验室内和实验室间精度和准确度,我们编译了来自血浆、肝脏和癌细胞的 1856 个脂质 CCS 值。我们的研究在脂质分析中建立了 PASEF,并为四个维度的灵敏、离子迁移率增强的脂质组学铺平了道路。
更新日期:2020-01-16
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