title: High-speed tandem mass spectrometric in situ imaging by nanospray desorption electrospray ionization mass spectrometry.
abstract: Nanospray desorption electrospray ionization (nano-DESI) combined with tandem mass spectrometry (MS/MS), high-resolution mass analysis of the fragment ions (m/Δm = 17 500 at m/z 200), and rapid spectral acquisition enabled simultaneous imaging and identification of a large number of metabolites and lipids from 92 selected m/z windows (±1 Da) with a spatial resolution of better than 150 μm. Mouse uterine sections of implantation sites on day 6 of pregnancy were analyzed in the ambient environment without any sample pretreatment. MS/MS imaging was performed by scanning the sample under the nano-DESI probe at 10 μm/s, while higher-energy collision-induced dissociation (HCD) spectra were acquired for a targeted inclusion list of 92 m/z values at a rate of ∼6.3 spectra/s. Molecular ions and their corresponding fragments, separated by high-resolution mass analysis, were assigned on the basis of accurate mass measurement. Using this approach, we were able to identify and image both abundant and low-abundance isobaric and isomeric species within each m/z window. MS/MS analysis enabled efficient separation and identification of isomeric and isobaric phospholipids that are difficult to separate in full-scan mode. Furthermore, we identified several metabolites associated with early pregnancy and obtained the first 2D images of these molecules.
authors.affiliation: Physical Sciences Division and ‡Biological Sciences Division, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors.forename: Ingela
authors.initials: I
authors.lastname: Lanekoff
authors.forename: Kristin
authors.initials: K
authors.lastname: Burnum-Johnson
authors.forename: Mathew
authors.initials: M
authors.lastname: Thomas
authors.forename: Joshua
authors.initials: J
authors.lastname: Short
authors.forename: James P
authors.initials: JP
authors.lastname: Carson
authors.forename: Jeeyeon
authors.initials: J
authors.lastname: Cha
authors.forename: Sudhansu K
authors.initials: SK
authors.lastname: Dey
authors.forename: Pengxiang
authors.initials: P
authors.lastname: Yang
authors.forename: Maria C
authors.initials: MC
authors.lastname: Prieto Conaway
authors.forename: Julia
authors.initials: J
authors.lastname: Laskin
mesh_terms: D000818:Animals; D005260:Female; D050356:Lipid Metabolism; D008297:Male; D055432:Metabolomics; D051379:Mice; D057054:Molecular Imaging / Q000379:methods*; D036103:Nanotechnology / Q000379:methods*; D011247:Pregnancy; D012822:Silicon Dioxide / Q000737:chemistry; D021241:Spectrometry, Mass, Electrospray Ionization / Q000379:methods*; D053719:Tandem Mass Spectrometry / Q000379:methods*; D013997:Time Factors
chemical_list: D012822:Silicon Dioxide
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