Journal
ANALYTICAL CHEMISTRY
Volume 85, Issue 20, Pages 9596-9603Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ac401760s
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Funding
- U.S. Department of Energy (DOE) [DE-AC05-76RL01830]
- DOE's Office of Biological and Environmental Research
- NIH [HD068524, DA06668]
- Ruth L. Kirschstein predoctoral NRSA fellowship [F30AG040858]
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Nanospray desorption electrospray ionization (nano-DESI) combined with tandem mass spectrometry (MS/MS), high-resolution mass analysis of the fragment ions (m/Delta m = 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 pm. 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 mu m/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 similar to 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.
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