Abstract
Triply deprotonated DGAILDGAILD was reacted in the gas-phase with doubly charged copper, cobalt, and iron metal complexes containing either two or three phenanthroline ligands. Reaction products result from two major pathways. The first pathway involves the transfer of an electron from the negatively charged peptide to the transition-metal complex. The other major pathway consists of the displacement of the phenanthroline ligands by the peptide resulting in the incorporation of the transition-metal into the peptide to form [M − 3H + XII]− ions, where X is Cu, Co, or Fe, respectively. The extent to which each pathway contributes is dependent on the nature of transition-metal complex. In general, bis-phen complexes result in more electron-transfer than the tris—phen complexes, while the tris—phen complexes result in more metal insertion. The metal in the complex plays a large role as well, with the Cu containing complexes giving rise to more electron transfer than the corresponding complexes of Co and Fe. The results show that a single reagent solution can be used to achieve two distinct sets of products (i.e., electron-transfer products and metal insertion products). These results constitute the demonstration of novel means for the gas-phase transformation of peptide anions from one ion type to another via ion/ion reactions using reagents formed via electrospray ionization.
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References
Aebersold, R.; Goodlett, D. R. Mass Spectrometry in Proteomics. Chem. Rev 2001, 101, 269–296.
Wells, J. M.; McLuckey, S. A. Collision-Induced Dissociation (CID) of Peptides and Proteins. Methods Enzymol 2005, 402, 148–185.
Zubarev, R. A.; Kelleher, N. L.; McLafferty, F. W. Electron Capture Dissociation of Multiply Charged Protein Cations: A Nonergodic Process. J. Am. Chem. Soc 1998, 120, 3265–3266.
Syka, J. E. P.; Coon, J. J.; Schroeder, M. J.; Shabanowitz, J.; Hunt, D. F. Peptide and Protein Sequence Analysis by Electron Transfer Dissociation Mass Spectrometry. Proc. Natl. Acad. Sci. U.S.A. 2004, 101, 9528–9533.
Bowie, J. H.; Brinkworth, C. S.; Dua, S. Collision-Induced Fragmentations of the (M − H)− Parent Anions of Underivatized Peptides: An Aid to Structure Determination and Some Unusual Negative Ion Cleavages. Mass Spectrom. Rev 2002, 21, 87–107.
Bilusich, D.; Bowie, J. H. Fragmentations of (M − H)− Anions of Underivatized Peptides: Part 2: Characteristic Cleavages of Ser and Cys and of Disulfides and Other Post-Translational Modifications, Together with Some Unusual Internal Processes. Mass Spectrom. Rev 2009, 28, 20–34.
Budnik, B. A.; Haselmann, K. F.; Zubarev, R. A. Electron Detachment Dissociation of Peptide Dianions: An Electron-Hole Recombination Phenomenon. Chem. Phys. Lett 2001, 342, 299–302.
Wolff, J. J.; Laremore, A. M.; Busch, A. M.; Linhardt, R. J.; Amster, I. J. Electron Detachment Dissociation of Dermatan Sulfate Oligosaccharides. J. Am. Soc. Mass Spectrom 2008, 19, 294–304.
Yang, J.; Mo, J.; Adamson, J. T.; Håkansson, K. Characterization of Oligodeoxynucleotides by Electron Detachment Dissociation Fourier Transform Ion Cyclotron Resonance Mass Spectrometry. Anal. Chem 2005, 77, 1876–1882.
Herron, W. J.; Goeringer, D. E.; McLuckey, S. A. Gas-Phase Electron Transfer Reactions from Multiply Charged Anions to Rare Gas Cations. J. Am. Chem. Soc 1995, 117, 11555–11562.
Coon, J. J.; Shabanowitz, J.; Hunt, D. F.; Syka, J. E. P. Electron Transfer Dissociation of Peptide Anions. J. Am. Soc. Mass Spectrom 2005, 16, 880–882.
Lam, C. N. W.; Chu, I. K. Formation of Anionic Peptide Radicals in Vacuo. J. Am. Soc. Mass Spectrom 2006, 17, 1249–1257.
Hu, P. F.; Gross, M. L. Gas Phase Interactions of Transition Metal Ions and Dipeptides and Tripeptides: A Comparison with Alkaline Earth Metal Ion Interactions. J. Am. Chem. Soc 1993, 115, 8821–8828.
Lee, S. W.; Kim, H. S.; Beauchamp, J. L. Salt Bridge Chemistry Applied to Gas-Phase Peptide Sequencing: Selective Fragmentation of Sodiated Gas-Phase Peptide Ions Adjacent to Aspartic Acid Residues. J. Am. Chem. Soc 1998, 120, 3188–3195.
Pingitore, F.; Wesdemiotis, C. Characterization of Dipeptide Isomers by Tandem Mass Spectrometry of Their Mono- versus Di-Lithiated Complexes. Anal. Chem 2005, 77, 1796–1806.
Barlow, C. K.; Hodges, B. D. M.; Xia, Y.; O’Hair, R. A. J.; McLuckey, S. A. Gas-Phase Ion/Ion Reactions of Transition Metal Complex Cations with Multiply Charged Oligodeoxynucleotide Anions. J. Am. Soc. Mass Spectrom 2008, 19, 281–293.
Van Berkel, G. J.; Asano, K. G.; Schnier, P. D. Electrochemical Processes in a Wire-in-a-Capillary Bulk-Loaded, Nano-Electrospray Emitter. J. Am. Soc. Mass Spectrom 2001, 12, 853–862.
Xia, Y.; Liang, X.; McLuckey, S. A. Pulsed Dual Electrospray ionization for ion/ion reactions. J. Am. Soc. Mass Spectrom 2005, 16, 1750–1756.
Xia, Y.; Chrisman, P. A.; Erickson, D. E.; Liu, J.; Liang, X. R.; Londry, F. A.; Yang, M. J.; McLuckey, S. A. Implementation of Ion/Ion Reactions in a Quadrupole/Time-of-Flight Tandem Mass Spectrometer. Anal. Chem 2006, 78, 4146–4154.
Xia, Y.; Chrisman, P. A.; Pitteri, S. J.; Erickson, D. E.; McLuckey, S. A. Ion/Molecule Reactions of Cation Radicals Formed from Protonated Polypeptides via Gas-Phase Ion/Ion Electron Transfer. J. Am. Chem. Soc 2006, 128, 11792–11798.
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Published online May 20, 2009
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Crizer, D.M., Xia, Y. & McLuckey, S.A. Transition metal complex cations as reagents for gas-phase transformation of multiply deprotonated polypeptides. J Am Soc Mass Spectrom 20, 1718–1722 (2009). https://doi.org/10.1016/j.jasms.2009.05.008
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DOI: https://doi.org/10.1016/j.jasms.2009.05.008