Abstract
We reported the use of ion mobility (IM) combined with mass spectrometry (MS) as an analytical tool to investigate low generation polyamidoanine (PAMAM) dendrimers. This analytical approach has been employed to separate ions of defective structures with different charge state but exactly the same m/z value. Tandem mass spectrometry (MS/MS) after IM separation allowed a comprehensive structural characterization of defective dendrimers. In addition, IM was used to evaluate the collision cross-sections of ions of perfect dendrimers. They showed a good correlation with calculated collision cross-sections obtained by the trajectory method (TM) and were also consistent with dimensions reported by other established analytical methods.
Similar content being viewed by others
References
Swanson, S., Kukowska-Latallo, J., Patri, A., Chen, C., Ge, S., Cao, Z., Kotlyar, A., East, A., Baker, J.: Targeted gadolinium-loaded dendrimer nanoparticles for tumor-specific magnetic resonance contrast enhancement. Int. J. Nanomed. 3, 201–210 (2008)
de Jong, P.: Drug delivery and nanoparticles: applications and hazards. Int. J. Nanomed. 3, 133–149 (2008)
Dufès, C., Uchegbu, I., Schätzlein, A.: Dendrimers in gene delivery. Adv. Drug Delivery Rev. 57, 2177–2202 (2005)
Tomalia, D., Baker, H., Dewald, J., Hall, M., Kallos, G., Martin, S., Roeck, J., Ryder, J., Smith, P.: A new class of polymers: starburst-dendritic macromolecules. Polym. J. 17, 117–132 (1985)
Vögtle, F., Richardt, G., Werner, N.: Dendrimer chemistry. pp 253–288. WILEY-VCH Verlag, Weinheim, (2009)
Caminade, A.-M., Laurent, R., Majoral, J.-P.: Characterization of dendrimers. Adv. Drug Delivery Rev. 57, 2130–2146 (2005)
Peterson, J., Allikmaa, V., Subbi, J., Pehk, T., Lopp, M.: Structural deviations in poly(amidoamine) dendrimers: a MALDI-TOF MS analysis. Eur. Polym. J. 39, 33–42 (2003)
Fischer-Durand, N., Salmain, M., Rudolf, B., Jugé, L., Guérineau, V., Laprévote, O., Vessières, A., Jaouen, G.: Design of a new multifunctionalized PAMAM dendrimer with hydrazide-terminated spacer arm suitable for metal-carbonyl multilabeling of aldehyde-containing molecules. Macromolecules 40, 8568–8575 (2007)
Hummelen, J.C., Joost, J.L., Meijer, E.W.: Electrospray mass spectrometry of poly(propylene imine) dendrimers: the issue of dendritic purity or polydispersity. Chem. Eur. J. 3, 1489–1493 (1997)
Krupkova, A., Cermak, J., Walterova, Z., Horsky, J.: Quantitative interpretation of MALDI-TOF mass spectra of imperfect carbosilane dendrimers. Anal. Chem. 79, 1639–1645 (2007)
Giordanengo, R., Mazarin, M., Wu, J., Peng, L., Charles, L.: Propagation of structural deviations of poly(amidoamine) fan-shape dendrimers (generations 0–3) characterized by MALDI and electrospray mass spectrometry. Int. J. Mass Spectrom. 266, 62–75 (2007)
Tintaru, A., Monnier, V., Bouillon, C., Giordanengo, R., Quéléver, G., Peng, L., Charles, L.: Structural characterization of poly(amino)ester dendrimers and related impurities by electrospray tandem mass spectrometry. Rapid Commun. Mass Spectrom. 24, 2207–2216 (2010)
Tintaru, A., Chendo, C., Monnier, V., Bouillon, C., Quelever, G., Peng, L., Charles, L.: Electrospray tandem mass spectrometry of poly(amino)ester dendrimers: dissociation rules and structural characterization of defective molecules. Int. J. Mass Spectrom. 308, 56–64 (2011)
Felder, T., Schalley, C., Fakhrnabavi, H., Lukin, O.: A combined ESI- and MALDI-MS(/MS) study of peripherally persulfonylated dendrimers: false negative results by MALDI-MS and analysis of defects. Chem. Eur. J. 11, 5625–5636 (2005)
Baytekin, B., Werner, N., Luppertz, F., Engeser, M., Brüggemann, J., Bitter, S., Henkel, R., Felder, T., Schalley, C.A.: How useful is mass spectrometry for the characterization of dendrimers?: fake defects in the ESI and MALDI mass spectra of dendritic compounds. Int. J. Mass Spectrom. 249, 138–148 (2006)
Maire, F., Lange, C.M.: Formation of unexpected ions from a first-generation polyamidoamine dendrimer by use of methanol: an artefact due to electrospray emitter corrosion? Rapid Commun. Mass Spectrom. 24, 995–1000 (2010)
Giles, K., Pringle, S., Worthington, K., Little, D., Wildgoose, J., Bateman, R.: Applications of a traveling wave-based radio-frequency-only stacked ring ion guide. Rapid Commun Mass Spectrom. 18, 2401–2414 (2004)
Giles, K., Williams, J.P., Campuzano, I.: Enhancements in traveling wave ion mobility resolution. Rapid Commun. Mass Spectrom. 25, 1559–1566 (2011)
Hilton, G., Jackson, A., Thalassinos, K., Scrivens, J.: Structural analysis of synthetic polymer mixtures using ion mobility and tandem mass spectrometry. Anal. Chem. 80, 9720–9725 (2008)
Song, J., Grün, C.H., Heeren, R.M.A., Janssen, H.-G., van den Brink, O.F.: High-resolution ion mobility spectrometry-mass spectrometry on poly(methyl methacrylate). Angew. Chem. Int. Ed. 49, 10168–10171 (2010)
Hoskins, J.N., Trimpin, S., Grayson, S.M.: Architectural differentiation of linear and cyclic polymeric isomers by ion mobility spectrometry-mass spectrometry. Macromolecules 44, 6915–6918 (2011)
Li, X., Chan, Y.-T., Casiano-Maldonado, M., Yu, J., Carri, G.A., Newkome, G.R., Wesdemiotis, C.: Separation and characterization of metallosupramolecular libraries by ion mobility mass spectrometry. Anal. Chem. 83, 6667–6674 (2011)
Li, X., Chan, Y.-T., Newkome, G.R., Wesdemiotis, C.: Gradient tandem mass spectrometry interfaced with ion mobility separation for the characterization of supramolecular architectures. Anal. Chem. 83, 1284–1290 (2011)
Angel, L., Majors, L., Dharmaratne, A., Dass, A.: Ion mobility mass spectrometry of Au25(SCH2CH2Ph)18 nanoclusters. ACS Nano 4, 4691–4700 (2010)
Smith, D., Knapman, T., Campuzano, I., Malham, R., Berryman, J., Radford, S., Ashcroft, A.: Deciphering drift time measurements from traveling wave ion mobility spectrometry-mass spectrometry studies. Eur. J. Mass Spectrom. 15, 113–130 (2009)
Valentine, S., Counterman, A., Clemmer, D.: Conformer-dependent proton-transfer reactions of ubiquitin ions. J. Am. Soc. Mass Spectrom. 8, 954–961 (1997)
Shelimov, K.B., Clemmer, D.E., Hudgins, R.R., Jarrold, M.F.: Protein Structure in Vacuo: Gas-Phase Conformations of BPTI and Cytochrome c. J. Am. Chem. Soc. 119, 92240–2248 (1997)
Henderson, S., Li, J., Counterman, A., Clemmer, D.: Intrinsic size parameters for val, ile, leu, gln, thr, phe, and trp residues from ion mobility measurements of polyamino acid ions. J. Phys. Chem. B 103, 8780–8785 (1999)
Hagler, A.: Theoretical simulation of conformation, energetics, and dynamics of peptides. Peptides 213–299 (1985)
Mesleh, M.F., Hunter, J.M., Shvartsburg, A.A., Schatz, G.C., Jarrold, M.F.: Structural information from ion mobility measurements: effects of the long-range potential. J. Phys. Chem. 100(40), 16082–16086 (1996)
Fréchet, J., Tomalia, D.: Dendrimers and other dendritic polymers. pp 587–604. John Wiley & Sons, Chichester (2001)
Bosman, A.W., Janssen, H.M., Meijer, E.W.: About dendrimers: structure, physical properties, and applications. Chem. Rev. 99, 1665–1688 (1999)
Leriche, E.-D., Maire, F., Grossel, M.C., Lange, C.M., Loutelier-Bourhis, C.: Off-line capillary electrophoresis/matrix-assisted laser desorption/ionization tandem time-of-flight mass spectrometry for analysis of synthesized poly(amido)amine dendrimers. Rapid Commun. Mass Spectrom. 26, 1718–1724 (2012)
Subbi, J., Aguraiuja, R., Tanner, R., Allikmaa, V., Lopp, M.: Fragmentation of poly(amidoamine) dendrimers in matrix-assisted laser desorption. Eur. Polym. J. 41, 2552–2558 (2005)
Vincent, T., Dolé, R., Lange, C.M.: Gas-phase fragmentation of half- and first-generation polyamidoamine dendrimers by electrospray mass spectrometry using a quadrupole ion trap. Rapid Commun. Mass Spectrom. 22, 363–372 (2008)
Ruotolo, B., Benesch, J., Sandercock, A., Hyung, S., Robinson, C.: Ion mobility-mass spectrometry analysis of large protein complexes. Nat. Protoc. 3, 1139–1152 (2008)
Shvartsburg, A.A., Smith, R.D.: Fundamentals of traveling wave ion mobility spectrometry. Anal. Chem. 80, 9689–9699 (2008)
Scarff, C., Thalassinos, K., Hilton, G., Scrivens, J.: Traveling wave ion mobility mass spectrometry studies of protein structure: biological significance and comparison with X-ray crystallography and nuclear magnetic resonance spectroscopy measurements. Rapid Commun. Mass Spectrom. 22, 3297–3304 (2008)
Knapman, T.W., Berryman, J.T., Campuzano, I., Harris, S.A., Ashcroft, A.E.: Considerations in experimental and theoretical collision cross-section measurements of small molecules using traveling wave ion mobility spectrometry-mass spectrometry. Int. J. Mass Spectrom. 298, 17–23 (2010)
Fritzinger, B., Scheler, U.: Scaling behavior of PAMAM dendrimers determined by diffusion NMR. Macromol. Chem. Phys. 206, 1288–1291 (2005)
Rathgeber, S., Monkenbusch, M., Kreitschmann, M., Urban, V., Brulet, A.: Dynamics of star-burst dendrimers in solution in relation to their structural properties. J. Chem. Phys. 117, 4047–4062 (2002)
Govorun, E.N., Zeldovich, K.B., Khokhlov, A.R.: Structure of Charged poly(propylene imine) dendrimers: theoretical investigation. Macromol. Theory Simul. 12, 705–713 (2003)
Acknowledgments
The authors thank the Région Haute-Normandie and the European Regional Development Fund (ERDF) for financial support.
Author information
Authors and Affiliations
Corresponding author
Electronic supplementary material
Below is the link to the electronic supplementary material.
ESM 1
(DOCX 5988 kb)
Rights and permissions
About this article
Cite this article
Maire, F., Coadou, G., Cravello, L. et al. Traveling Wave Ion Mobility Mass Spectrometry Study of Low Generation Polyamidoamine Dendrimers. J. Am. Soc. Mass Spectrom. 24, 238–248 (2013). https://doi.org/10.1007/s13361-012-0527-3
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s13361-012-0527-3