Microfluidics-based electrospray ionization enhances the intrasource separation of lipid classes and extends identification of individual molecular species through multi-dimensional mass spectrometry: Development of an automated high-throughput platform for shotgun lipidomics

Xianlin Han, Kui Yang, Richard W. Gross

Research output: Contribution to journalArticlepeer-review

91 Scopus citations

Abstract

Herein, we exploit the use of microfluidics and optimized Taylor cones for improved intrasource separation/selective ionization of lipid classes during electrospray ionization. Increased differential ionization of multiple phospholipid classes was achieved through microfluidics with chip-based ionization resulting in substantial enhancement of intrasource separation/selective ionization of phospholipid classes in comparison to the conventional ion source. For example, using myocardial lipid extracts, 3-fold improvements in intrasource separation/selective ionization of myocardial phospholipid classes were routinely realized in the negative-ion mode in the absence of LiOH or other basic modifiers in the infused sample solutions. Importantly, the relative ratios of ions corresponding to individual molecular species in each lipid class to a selected internal standard from myocardial extracts were nearly identical between the chip-based interface and the syringe-pump-driven capillary interface. Therefore, quantitation of individual lipid molecular species directly from biological extracts through comparisons with internal standards in each lipid class was readily accomplished with an accuracy and dynamic range nearly identical to those documented using the well-established direct syringe-pump-driven capillary interface. Collectively, the use of microfluidics and robotic sample handling substantially enhances intrasource separation of lipids in comparison to routine capillary interfaces and greatly facilitates the use of multi-dimensional mass spectrometry using shotgun lipidomics, thereby providing an automated and high-throughput platform for global analyses of cellular lipidomes.

Original languageEnglish (US)
Pages (from-to)2115-2124
Number of pages10
JournalRapid Communications in Mass Spectrometry
Volume22
Issue number13
DOIs
StatePublished - Jul 2008
Externally publishedYes

ASJC Scopus subject areas

  • Analytical Chemistry
  • Spectroscopy
  • Organic Chemistry

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