期刊
ANALYTICAL CHEMISTRY
卷 89, 期 13, 页码 7046-7052出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.7b00794
关键词
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资金
- Max Planck Gesellschaft
- Deutsche Forschungsgemeinschaft (DFG) [TRR83]
- LiSyM program
- LIES Unit of the de.NBI Consortium
- Bundesministerium f. Bildung u. Forschung (BMBF)
Shotgun lipidomics relies on the direct infusion of total lipid extracts into a high resolution tandem mass spectrometer. A single shotgun analysis produces several hundred of densely. opulated FT MS and FT MS/MS spectra, each of which might comprise thousands of peaks although a very small percentage of those belong to lipids. Eliminating noise by adjusting a minimal peak intensity threshold is biased and inefficient since lipid species and classes vary in their natural abundance and ionization capacity. We developed a method of peak intensity-independent noise filtering in shotgun FT MS and FT MS/MS spectra that capitalizes on a stable composition of the infused analyte leading to consistent time-independent detection of its bona fide components. Repetition rate filtering relies on a single quantitative measure of peaks detection reproducibility irrespectively of their absolute intensities, masses, or assumed elemental compositions. In comparative experiments, it removed more than 95% of signals detectable in shotgun spectra without compromising the accuracy and scope of lipid identification and quantification. It also accelerated spectra processing by 15-fold and increased the number of simultaneously processed spectra by similar to 500-fold hence eliminating the major bottleneck in high-throughput bottom-up shotgun lipidomics.
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