Skip to main content
SpringerLink
Log in

Multiplex Mass Spectrometric Imaging with Polarity Switching for Concurrent Acquisition of Positive and Negative Ion Images

  • Research Article
  • Published:
Journal of The American Society for Mass Spectrometry

Abstract

We have recently developed a multiplex mass spectrometry imaging (MSI) method which incorporates high mass resolution imaging and MS/MS and MS3 imaging of several compounds in a single data acquisition utilizing a hybrid linear ion trap-Orbitrap mass spectrometer (Perdian and Lee, Anal. Chem. 82, 9393–9400, 2010). Here we extend this capability to obtain positive and negative ion MS and MS/MS spectra in a single MS imaging experiment through polarity switching within spiral steps of each raster step. This methodology was demonstrated for the analysis of various lipid class compounds in a section of mouse brain. This allows for simultaneous imaging of compounds that are readily ionized in positive mode (e.g., phosphatidylcholines and sphingomyelins) and those that are readily ionized in negative mode (e.g., sulfatides, phosphatidylinositols and phosphatidylserines). MS/MS imaging was also performed for a few compounds in both positive and negative ion mode within the same experimental set-up. Insufficient stabilization time for the Orbitrap high voltage leads to slight deviations in observed masses, but these deviations are systematic and were easily corrected with a two-point calibration to background ions.

ᅟ

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Figure 1
Figure 2
Figure 3
Figure 4

Similar content being viewed by others

References

  1. Svatos, A.: Mass spectrometric imaging of small molecules. Trends Biotechnol. 28, 425–434 (2010)

    Article  CAS  Google Scholar 

  2. Burnum, K.E., Frappier, S.L., Caprioli, R.M.: Matrix-assisted laser desorption/ionization imaging mass spectrometry for the investigation of proteins and peptides. Annu. Rev. Anal. Chem. 1, 689–705 (2008)

    Article  CAS  Google Scholar 

  3. Goto-Inoue, N., Hayasaka, T., Zaima, N., Setou, M.: Imaging mass spectrometry for lipidomics. Biochim. Biophys. Acta 1811, 961–969 (2011)

    Article  CAS  Google Scholar 

  4. Smith, D.F., Aizikov, K., Duursma, M.C., Giskes, F., Spaanderman, D.-J., McDonnell, L.A., O’Conner, P.B., Heeren, R.M.A.: An external matrix-assisted laser desorption ionization source for flexible FT-ICR mass spectrometry imaging with internal calibration on adjacent samples. J. Am. Soc. Mass Spectrom. 22, 130–137 (2011)

    Article  CAS  Google Scholar 

  5. Schober, Y., Schramm, T., Spengler, B., Römpp, A.: Protein identification by accurate mass matrix-assisted laser desorption/ionization imaging of tryptic peptides. Rapid Commun. Mass Spectrom. 25, 2475–2483 (2011)

    Article  CAS  Google Scholar 

  6. Perdian, D.C., Lee, Y.J.: Imaging MS methodology for more chemical information in less data acquisition time utilizing a hybrid linear ion trap-Orbitrap mass spectrometer. Anal. Chem. 82, 9393–9400 (2010)

    Article  CAS  Google Scholar 

  7. Lunsford, K.A., Peter, G.F., Yost, R.A.: Direct matrix-assisted laser desorption/ionization mass spectrometric imaging of cellulose and hemicellulose in populus tissue. Anal. Chem. 83, 6722–6730 (2011)

    Article  CAS  Google Scholar 

  8. Cerruti, C.D., Benabdellah, F., Laprevote, O., Touboul, D., Brunelle, A.: MALDI imaging and structural analysis of rat brain lipid negative ions with 9-aminoacridine matrix. Anal. Chem. 84, 2164–2171 (2012)

    Article  CAS  Google Scholar 

  9. Gode, D., Volmer, D.A.: Lipid imaging by mass spectrometry: a review. Analyst 138, 1289–1315 (2013)

    Article  CAS  Google Scholar 

  10. Berry, K.A., Hankin, J.A., Barkley, R.M., Spraggins, J.M., Caprioli, R.M., Murphy, R.C.: MALDI imaging of lipid biochemistry in tissues by mass spectrometry. Chem. Rev. 111, 6491–6512 (2011)

    Article  Google Scholar 

  11. Eberlin, L.S., Ferreira, C.R., Dill, A.L., Ifa, D.R., Cooks, R.G.: Desorption electrospray ionization mass spectrometry for lipid characterization and biological tissue imaging. Biochim. Biophys. Acta 1811, 946–950 (2011)

    Article  CAS  Google Scholar 

  12. Passarelli, M.K., Winograd, N.: Lipid imaging with time-of-flight secondary ion mass spectrometry (TOF-SIMS). Biochim. Biophys. Acta 1811, 976–990 (2011)

    Article  CAS  Google Scholar 

  13. Fletcher, J.S., Vickerman, J.C., Winograd, N.: Label free biochemical 2D and 3D imaging using secondary ion mass spectrometry. Curr. Opin. Chem. Biol. 15, 733–740 (2011)

    Article  CAS  Google Scholar 

  14. Thomas, A., Charbonneau, J.L., Fournaise, E., Chaurand, P.: Sublimation of new matrix candidates for high spatial resolution imaging mass spectrometry of lipids: enhanced information in both positive and negative polarities after 1,5-diaminonaphthalene deposition. Anal. Chem. 84, 2048–2054 (2012)

    Article  CAS  Google Scholar 

  15. Benabdellah, F., Seyer, A., Quinton, L., Touboul, D., Brunelle, A., Laprevote, O.: Mass spectrometry imaging of rat brain sections: nanomolar sensitivity with MALDI versus nanometer resolution by TOF-SIMS. Anal. Bioanal. Chem. 396, 151–162 (2010)

    Article  CAS  Google Scholar 

  16. Leefmann, T., Heim, C., Siljeström, S., Blumenberg, M., Sjövall, P., Thiel, V.: Spectral characterization of 10 cyclic lipids using time-of-flight secondary ion mass spectrometry. Rapid Commun. Mass Spectrom. 27, 565–581 (2013)

    Article  CAS  Google Scholar 

  17. Solé-Domènech, S., Sjövall, P., Vukojević, V., Fernando, R., Codita, A., Salve, S., Bogdanović, N., Mohammed, A.H., Hammarström, P., Nilsson, K.P., LaFerla, F.M., Jacob, S., Berggren, P.O., Giménez-Llort, L., Schalling, M., Terenius, L., Johansson, B.: Localization of cholesterol, amyloid and glia in Alzheimer’s disease transgenic mouse brain tissue using time-of-flight secondary ion mass spectrometry (TOF-SIMS) and immunofluorescence imaging. Acta Neuropathol. 125, 145–157 (2013)

    Article  Google Scholar 

  18. Schuhmann, K., Almeida, R., Baumert, M., Herzog, R., Bornstein, S.R., Shevchenko, A.: Shotgun lipidomics on a LTQ Orbitrap mass spectrometer by successive switching between acquisition polarity modes. J. Mass Spectrom. 47, 96–104 (2012)

    Article  CAS  Google Scholar 

  19. Hankin, J.A., Barkley, R.M., Murphy, R.C.: Sublimation as a method of matrix application for mass spectrometric imaging. J. Am. Soc. Mass Spectrom. 18, 1646–1652 (2007)

    Article  CAS  Google Scholar 

  20. Sjovall, P., Lausmaa, J., Johannson, B.: Mass spectrometric imaging of lipids in brain tissue. Anal. Chem. 76, 4271–4278 (2004)

    Article  Google Scholar 

  21. Hankin, J.A., Farias, S.E., Barkley, R.M., Heidenreich, K., Frey, L.C., Hamazaki, K., Kim, H.-Y., Murphy, R.C.: MALDI mass spectrometric imaging of lipids in rat brain injury models. J. Am. Soc. Mass Spectrom. 22, 1014–1021 (2011)

    Article  CAS  Google Scholar 

  22. Martha, D.S., Douglas, F.B.: Complementary use of MALDI and ESI for the HPLC-MS/MS analysis of DNA-binding proteins. Anal. Chem. 76, 5423–5430 (2004)

    Article  Google Scholar 

Download references

Acknowledgments

The authors thank Emile de Leeuw at Thermo Fisher Scientific for providing them a software patch and for helpful conversations. This work was supported by the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. The Ames Laboratory is operated by Iowa State University under DOE Contract DE-AC02-07CH11358.

Author information

Authors and Affiliations

  1. Ames Laboratory, US Department of Energy, Ames, IA, 50011, USA

    Andrew R. Korte & Young Jin Lee

  2. Department of Chemistry, Iowa State University of Science and Technology, Ames, IA, 50011, USA

    Andrew R. Korte & Young Jin Lee

Authors
  1. Andrew R. Korte
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Young Jin Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Young Jin Lee.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Figure S1

MS/MS spectra used to generate MS/MS images in Figure 3. MS/MS of [PC (32:0) + K]+ (a), MS/MS of [PC (36:1) + K]+ (b), MS/MS of [PI (18:0/20:4) – H]− (c) and MS/MS of [ST (d18:1/h24:0) – H]− (d). Transitions used to generate images are labeled. m/z 886.7 in (c) is an isotope of precursor (m/z 885.5) that was included as a result of incomplete isolation but did not completely fragment because its secular frequency is slightly off from the activation frequency (PDF 129 kb) (PDF 129 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Korte, A.R., Lee, Y.J. Multiplex Mass Spectrometric Imaging with Polarity Switching for Concurrent Acquisition of Positive and Negative Ion Images. J. Am. Soc. Mass Spectrom. 24, 949–955 (2013). https://doi.org/10.1007/s13361-013-0613-1

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s13361-013-0613-1

Key words

Search

Navigation