Electron capture dissociation of gaseous multiply charged ions by Fourier-transform ion cyclotron resonance

  • Fred W. McLafferty
  • David M. Horn
  • Kathrin Breuker
  • Ying Ge
  • Mark A. Lewis
  • Blas Cerda
  • Roman A. Zubarev
  • Barry K. Carpenter
Focus: FT-ICR-MS

Abstract

Fourier-transform ion cyclotron resonance instrumentation is uniquely applicable to an unusual new ion chemistry, electron capture dissociation (ECD). This causes nonergodic dissociation of far larger molecules (42 kDa) than previously observed (<1 kDa), with the resulting unimolecular ion chemistry also unique because it involves radical site reactions for similarly larger ions. ECD is highly complementary to the well known energetic methods for multiply charged ion dissociation, providing much more extensive protein sequence information, including the direct identification of N- versus C-terminal fragment ions. Because ECD only excites the molecule near the cleavage site, accompanying rearrangements are minimized. Counterintuitively, cleavage of backbone covalent bonds of protein ions is favored over that of noncovalent bonds; larger (>10 kDa) ions give far more extensive ECD if they are first thermally activated. This high specificity for covalent bond cleavage also makes ECD promising for studying the secondary and tertiary structure of gaseous protein ions caused by noncovalent bonding.

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References

  1. 1.
    Comisarow, M. B.; Marshall, A. G. Chem. Phys. Lett. 1974, 25, 282–283. White, R. L.; Ledford, E. B.; Ghaderi, S.; Wilkins, S. L.; Gross, M. L. Anal. Chem. 1980, 52, 1525. Karlin, T. J.; Freiser, B. S. Anal. Chem. 1983, 55, 571–574. Castro, M. E.; Russell, D. H. Anal. Chem. 1984, 56, 578. Hunt, D. F.; Shabanowitz, J.; McIver, R. T., Jr.; Hunter, R. L.; Syka, J. E. P. Anal. Chem. 1985, 57, 765–768. Marshall, A. G.; Wang, T. C. L.; Chen. L.; Ricca, T. L. ACS Symp. Ser. 1987, 359, 21–33. Fourier-Transform Mass Spectrometry; Buchanan, M. V. Ed.; American Chemical Society: Washington, DC, 1987. Wilkins, C. L.; Chowdhury, A. K.; Nuwaysir, L. M.; Coates, M. L. Mass Spectrom Rev. 1989, 8, 67–92. Marshall, A. G.; Grosshans, P. B. Anal. Chem. 1991, 63, A215–A229. Beu, S. C.; Laude, D. A., Jr. Int. J. Mass Spectrom. Ion Processes 1992, 112, 215–230. Hofstadler, S. A.; Laude, D. A., Jr. J. Am. Soc. Mass Spectrom. 1992, 3, 615–623. Hofstadler, S. A.; Beu, S. C.; Laude, D. A., Jr. Anal Chem. 1993, 65, A245–A259. Winger, B. E.; Hofstadler, S. A.; Bruce, J. E.; Udseth, H. R.; Smith, R. D. J. Am. Soc. Mass Spectrom. 1993, 4, 566–577. Williams, E. R. Anal Chem. 1998, 70, 179A–185A. Marshall A. G.; Hendrickson, C. L; Jackson, G. S. Mass. Spectrom. Rev. 1998, 17, 1–36.CrossRefGoogle Scholar
  2. 2.
    Cody, R. B., Jr.; Amster, I. J.; McLafferty, F. W. Proc. Natl. Acad. Sci. U.S.A., 1985, 82, 6367–6370. McLafferty, F. W.; Amster, I. J; Furlong, J. J. P.; Loo, J. A.; Wang, B. H.; Williams, E. R. Tandem Fourier-Transform Mass Spectrometry; M. V. Buchanan, Ed.; American Chemical Society: Washington, DC, 1987. Henry, K. D.; Williams, E. R.; Wang, B. H.; McLafferty, F. W.; Shabanowitz, J.; Hunt, D. F. Proc. Natl. Acad. Sci. U.S.A., 1989, 86, 9075–9078. Beu, S. C.; Senko, M. W.; Quinn, J. P.; Wampler, F. M., III; McLafferty, F. W. J. Am. Soc. Mass Spectrom., 1993, 4, 557–565. Senko, M. W.; Beu, S. C.; McLafferty, F. W. Annu. Rev. Biophys. Biomol. Struct. 1994, 23, 763–785.CrossRefGoogle Scholar
  3. 3. (a)
    Loo, J. A.; Udseth, H. R.; Smith, R. D. Rapid Commun. Mass Spectrom. 1988, 2, 207–210.CrossRefGoogle Scholar
  4. 3. (b)
    Gauthier, J. W.; Trautman, T. R.; Jacobsen, D. B. Anal. Chim. Acta 1991, 246, 211–225.CrossRefGoogle Scholar
  5. 3. (c)
    Senko, M. W.; Speir, J. P.; McLafferty, F. W. Anal. Chem. 1994, 66, 2801–2808.CrossRefGoogle Scholar
  6. 4.
    Little, D. P.; Chorush, R. A.; Speir, J. P.; Senko, M. W.; Kelleher, N. L.; McLafferty, F. W. J. Am. Chem. Soc. 1994, 116, 4893–4897.CrossRefGoogle Scholar
  7. 5.
    Price, W. D.; Schnier, P. D.; Williams, E. R. Anal Chem. 1996, 68, 859–866.CrossRefGoogle Scholar
  8. 6. (a)
    McCormack, A. L.; Jones, J. L.; Wysocki, V. H. J. Am. Soc. Mass Spectrom. 1992, 3, 859–862.CrossRefGoogle Scholar
  9. 6. (b)
    Chorush, R. A.; Little, D. P.; Beu, S. C.; Wood, T. D.; McLafferty, F. W. Anal. Chem. 1995, 67, 1042–1046.CrossRefGoogle Scholar
  10. 7.
    Guan, Z.; Kelleher, N. L.; O’Connor, P. B.; Aaserud, D. J.; Little, D. P.; McLafferty, F. W. Int. J. Mass Spectrom. Ion Processes 1996, 157, 357–364.CrossRefGoogle Scholar
  11. 8. (a)
    Mirgorodskaya, E.; Roepstorff, P.; Zubarev, R. Anal. Chem. 1999, 71, 4431–4436.CrossRefGoogle Scholar
  12. 8. (b)
    Kelleher, N. L.; Zubarev, R. A.; Bush, K.; Furie, B.; Furie, B. C.; McLafferty, F. W.; Walsh, C. T. Anal. Chem. 1999, 71, 4250–4253.CrossRefGoogle Scholar
  13. 8. (c)
    Fridriksson, E. K.; Beavil, A.; Holowka, D.; Gould, H. J.; Baird, B.; McLafferty, F. W. Biochemistry 2000, 39, 3369–3376.CrossRefGoogle Scholar
  14. 8. (d)
    Schey, K. L.; Finley, E. L. Acc Chem. Res. 2000, 33, 299–306.CrossRefGoogle Scholar
  15. 8. (e)
    Shi, S. D.-H.; Hemling, M. E.; Carr, S. A.; Horn, D. M.; Lindh, I.; McLafferty, F. W. Anal. Chem., submitted.Google Scholar
  16. 9. (a)
    Zubarev, R. A.; Kelleher, N. L.; McLafferty, F. W. J. Am. Chem. Soc. 1998, 120, 3265–3266.CrossRefGoogle Scholar
  17. 9. (b)
    Zubarev, R. A.; Kruger, N. A.; Fridriksson, E. K.; Lewis, M. A.; Horn, D. M.; Carpenter, B. K.; McLafferty, F. W. J. Am. Chem. Soc. 1999, 121, 2857–2862.CrossRefGoogle Scholar
  18. 9. (c)
    Zubarev, R. A.; Horn, D. M.; Fridriksson, E. K.; Kelleher, N. L.; Kruger, N. A.; Lewis, M. A.; Carpenter, B. K.; McLafferty, F. W. Anal. Chem. 2000, 72, 563–573.CrossRefGoogle Scholar
  19. 9. (d)
    Horn, D. M.; Ge, Y.; McLafferty, F. W. Anal. Chem., 2000, 72, 4778–4784.CrossRefGoogle Scholar
  20. 10.
    Turecek, F.; McLafferty, F. W. J. Am. Chem. Soc. 1984, 106, 2525–2528.CrossRefGoogle Scholar
  21. 11. (a)
    Biemann, K. In Methods in Enzymology; McCloskey, J. A., Ed., Academic: San Diego, 1990; Vol. 193, p 887.Google Scholar
  22. 11. (b)
    Andersen, J. S.; Svensson, B.; Roepstorff, P. Nature Biotechnol. 1996, 14, 449–457.CrossRefGoogle Scholar
  23. 11. (c)
    Qin, J.; Chait, B. T. Anal. Chem. 1997, 69, 4002–4009.CrossRefGoogle Scholar
  24. 11. (d)
    Kuster, B.; Mann, M. Curr. Opin. Chem. Biol. 1998, 8, 393–400.Google Scholar
  25. 11. (e)
    Jensen, K.; Pasa-Tolic, L.; Anderson, G. A.; Horner, J. A.; Lyston, M. S.; Bruce, J. E.; Smith, R. D. Anal. Chem. 1999, 71, 2076–2084.CrossRefGoogle Scholar
  26. 12. (a)
    McLafferty, F. W. Acc. Chem. Res. 1994, 27, 379–386.CrossRefGoogle Scholar
  27. 12. (b)
    McLafferty, F. W.; Kelleher, N. L.; Begley, T. P.; Fridriksson, E. K.; Zubarev, R. A.; Horn, D. M. Curr. Opin. Chem. Biol. 1998, 2, 571–578.CrossRefGoogle Scholar
  28. 12. (c)
    Kelleher, N. L.; Lin, H. Y.; Valaskovic, G. A.; Aaserud, D. J.; Fridriksson, E. K.; McLafferty, F. W. J. Am. Chem. Soc. 1999, 121, 806–812.CrossRefGoogle Scholar
  29. 12. (d)
    McLafferty, F. W.; Fridriksson, E. K.; Horn, D. M.; Lewis, M. A.; Zubarev, R. A. Science (Washington, D. C.) 1999, 284, 1289–1290.CrossRefGoogle Scholar
  30. 13.
    Green, M. K.; Lebrilla, C. B. Mass. Spectrom. Rev. 1997, 16, 53–72. Brodbelt, J. S. Mass Spectrom Rev. 1997, 16, 91–110. Ranatunga, T. D.; Kennady, J. M.; Kenttamaa, H. I. J. Am. Chem. Soc. 1997, 119, 5200–5207. McLuckey, S. A.; Stephenson, J. L. Mass Spectrom. Rev. 1998, 17, 369–407.CrossRefGoogle Scholar
  31. 14.
    McLafferty, F. W. In Mass Spectrometry in the Analysis of Large Molecules; McNeal, C. J., Ed., Wiley: New York, 1986, pp 107–120.Google Scholar
  32. 15.
    McLafferty, F. W.; Turecek, F. In Interpretation of Mass Spectra, 4th ed. University Science Books: Mill Valley, CA, 1993.Google Scholar
  33. 16.
    McLafferty, F. W.; Stauffer, D. A.; Loh, S. Y.; Wesdemiotis, C. J. Am. Soc. Mass Spectrom. 1999, 10, 1229–1240.CrossRefGoogle Scholar
  34. 17. (a)
    Kruger, N. A.; Zubarev, R. A.; Carpenter, B. K.; Kelleher, N. L.; Horn, D. M.; McLafferty, F. W. Int. J. Mass Spectrom. 1999, 182, 1–5.CrossRefGoogle Scholar
  35. 17. (b)
    Kruger, N. A.; Zubarev, R. A.; Horn, D. M.; McLafferty, F. W. Int. J. Mass Spectrom. 1999, 185, 787–793.CrossRefGoogle Scholar
  36. 18.
    Horn, D. M.; Zubarev, R. A.; McLafferty, F. W. J. Am. Soc. Mass Spectrom. 2000, 11, 320–332.CrossRefGoogle Scholar
  37. 19.
    Horn, D. M.; Zubarev, R. A.; McLafferty, F. W. Proc. Natl. Acad. Sci. U.S.A., 2000, 97, 10313–10317.CrossRefGoogle Scholar
  38. 20.
    Cerda, B. A.; Horn, D. M.; Breuker, K.; Carpenter, B. K.; McLafferty, F. W. Eur. Mass Spectrom. 1999, 5, 335–338.CrossRefGoogle Scholar
  39. 21.
    Cerda, B. A.; Horn, D. M.; Breuker, K.; McLafferty, F. W. J. Am Chem. Soc., submitted.Google Scholar
  40. 22.
    McLafferty, F. W.; Guan, Z.; Haupts, U.; Wood, T. D.; Kelleher, N. L. J. Am. Chem. Soc. 1998, 120, 4732–4740.CrossRefGoogle Scholar
  41. 23.
    Speir, J. P.; Senko, M. W.; Little, D. P.; Loo, J. A.; McLafferty, F. W. J. Mass Spectrom. 1995, 30, 39–42. Little, D. P.; McLafferty, F. W. J. Am. Soc. Mass Spectrom. 1996, 7, 209–210. Fridriksson, E. K.; Baird, B.; McLafferty, F. W. J. Am. Soc. Mass Spectrom. 1999, 10, 453–455.CrossRefGoogle Scholar
  42. 24.
    Horn, D. M.; Breuker, K.; Cerda, B. A.; Ge, Y.; McLafferty, F. W., unpublished.Google Scholar
  43. 25.
    Horn, D. M.; Breuker, K.; Frank, A. J.; McLafferty, F. W. J. Am. Chem. Soc., submitted.Google Scholar
  44. 26.
    Ganem, B.; Li, Y. -T.; Henion, J. D. J. Am. Chem. Soc. 1991, 113, 6294–6296. Li, Y.-T.; Henion, J. D.; Senko, M. W.; McLafferty, F. W.; Ganem, B. J. Am. Chem. Soc. 1993, 115, 8409–8413. Loo, J. A. Mass Spectrom. Rev. 1997, 16, 1–23.CrossRefGoogle Scholar
  45. 27.
    Mann, M.; Wilm, M. Anal. Chem. 1994, 66, 4390–4399. Mortz, E.; O’Connor, P. B.; Roepstorff, P.; Kelleher, N. L.; Wood, T. D.; McLafferty, F. W.; Mann, M. Proc. Natl. Acad. Sci. U.S.A. 1996, 93, 8264–8267.CrossRefGoogle Scholar

Copyright information

© American Society for Mass Spectrometry 2001

Authors and Affiliations

  • Fred W. McLafferty
    • 1
  • David M. Horn
    • 1
  • Kathrin Breuker
    • 1
  • Ying Ge
    • 1
  • Mark A. Lewis
    • 1
    • 2
  • Blas Cerda
    • 1
  • Roman A. Zubarev
    • 1
    • 3
  • Barry K. Carpenter
    • 1
  1. 1.Baker Chemistry LaboratoryCornell UniversityIthacaUSA
  2. 2.Corning Inc.Corning
  3. 3.Chemistry DepartmentOdense UniversityOdenseDenmark

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