Collision induced unfolding; CIU; Collision induced dissociation; CID; Electron transfer dissociation; ETD; Synthetic polymers; Ion mobility calibration
Abstract :
[en] Polymer characterizations are often performed using mass spectrometry (MS). Aside from MS and different tandem MS (MS/MS) tech- niques, ion mobility–mass spectrometry (IM-MS) has been recently added to the inventory of char- acterization technique. However, only few studies have focused on the reproducibility and robust- ness of polymer IM-MS analyses. Here, we per- form collisional and electron-mediated activation of polymer ions before measuring IM drift times, collision cross-sections (CCS), or reduced ion mobilities (K0). The resulting IM behavior of different activated product ions is then compared to non-activated native intact polymer ions. First, we analyzed collision induced unfolding (CIU) of precursor ions to test the robustness of polymer ion shapes. Then, we focused on fragmen- tation product ions to test for shape retentions from the precursor ions: cation ejection species (CES) and product ions with m/z and charge state values identical to native intact polymer ions. The CES species are formed using both collision induced dissociation (CID) and electron transfer dissociation (ETD, formally ETnoD) experiments. Only small drift time, CCS, or K0 deviations between the activated/formed ions are observed compared to the native intact polymer ions. The polymer ion shapes seem to depend solely on their mass and charge state. The experiments were performed on three synthetic homopolymers: poly(ethoxy phosphate) (PEtP), poly(2-n-propyl- 2-oxazoline) (Pn-PrOx), and poly(ethylene oxide) (PEO). These results confirm the robustness of polymer ion CCSs for IM calibration, especially singly charged polymer ions. The results are also discussed in the context of polymer analyses, CCS predictions, and probing ion–drift gas interaction potentials.
Research Center/Unit :
MolSys - Molecular Systems - ULiège CESAM - Complex and Entangled Systems from Atoms to Materials - ULiège Supramolecular Chemistry Group
Disciplines :
Chemistry
Author, co-author :
Haler, Jean ; Université de Liège - ULiège > Département de chimie (sciences) > Chimie analytique inorganique
Massonnet, Philippe ; Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de spectrométrie de masse (L.S.M.)
Far, Johann ; Université de Liège - ULiège > Département de chimie (sciences) > Center for Analytical Research and Technology (CART)
de la Rosa, Victor; Ghent University > Supramolecular Chemistry Group
Lecomte, Philippe ; Université de Liège - ULiège > Département de chimie (sciences) > Centre d'études et de rech. sur les macromolécules (CERM)
Hoogenboom, Richard; Ghent University > Supramolecular Chemistry Group
Jérôme, Christine ; Université de Liège - ULiège > Département de chimie (sciences) > Centre d'études et de rech. sur les macromolécules (CERM)
De Pauw, Edwin ; Université de Liège - ULiège > Département de chimie (sciences) > Chimie analytique inorganique
Language :
English
Title :
Gas-Phase Dynamics of Collision Induced Unfolding, Collision Induced Dissociation, and Electron Transfer Dissociation-Activated Polymer Ions
Publication date :
April 2019
Journal title :
Journal of the American Society for Mass Spectrometry
FRIA - Fonds pour la Formation à la Recherche dans l'Industrie et dans l'Agriculture FWO - Fonds Wetenschappelijk Onderzoek Vlaanderen UGent - Universiteit Gent
Floris, F., Vallotto, C., Chiron, L., Lynch, A.M., Barrow, M.P., Delsuc, M.A., O’Connor, P.B.: Polymer analysis in the second dimension: preliminary studies for the characterization of polymers with 2D MS. Anal. Chem. 89, 9892–9899 (2017)
Wesdemiotis, C., Solak, N., Polce, M.J., Dabney, D.E., Chaicharoen, K., Katzenmeyer, B.C.: Fragmentation pathways of polymer ions. Mass Spectrom. Rev. 30, 523–529 (2011)
Baumgaertel, A., Altuntaş, E., Kempe, K., Crecelius, A., Schubert, U.S.: Characterization of different poly(2-oxazoline) block copolymers by MALDI-TOF MS/MS and ESI-Q-TOF MS/MS. J. Polym. Sci. A Polym. Chem. 48, 5533–5540 (2010)
Crotty, S., Gerişlioğlu, S., Endres, K.J., Wesdemiotis, C., Schubert, U.S.: Polymer architectures via mass spectrometry and hyphenated techniques: a review. Anal. Chim. Acta. 932, 1–21 (2016)
Yol, A.M., Dabney, D.E., Wang, S.F., Laurent, B.A., Foster, M.D., Quirk, R.P., Grayson, S.M., Wesdemiotis, C.: Differentiation of linear and cyclic polymer architectures by MALDI tandem mass spectrometry (MALDI-MS2). J. Am. Soc. Mass Spectrom. 24, 74–82 (2013)
Knop, K., Jahn, B.O., Hager, M.D., Crecelius, A., Gottschaldt, M., Schubert, U.S.: Systematic MALDI-TOF CID investigation on different substituted mPEG 2000. Macromol. Chem. Phys. 211, 677–684 (2010)
Girod, M., Phan, T.N.T., Charles, L.: Microstructural study of a nitroxide-mediated poly(ethylene oxide)/polystyrene block copolymer (PEO-b-PS) by electrospray tandem mass spectrometry. J. Am. Soc. Mass Spectrom. 19, 1163–1175 (2008)
Jeanne Dit Fouque, D., Maroto, A., Memboeuf, A.: Purification and quantification of an isomeric compound in a mixture by collisional excitation in multistage mass spectrometry experiments. Anal. Chem. 88, 10821–10825 (2016)
Memboeuf, A., Nasioudis, A., Indelicato, S., Pollreisz, F., Kuki, Á., Kéki, S., Van Den Brink, O.F., Vékey, K., Drahos, L.: Size effect on fragmentation in tandem mass spectrometry. Anal. Chem. 82, 2294–2302 (2010)
Josse, T., De Winter, J., Dubois, P., Coulembier, O., Gerbaux, P., Memboeuf, A.: A tandem mass spectrometry-based method to assess the architectural purity of synthetic polymers: a case of a cyclic polylactide obtained by click chemistry. Polym. Chem. 6, 64–69 (2015)
Memboeuf, A., Jullien, L., Lartia, R., Brasme, B., Gimbert, Y.: Tandem mass spectrometric analysis of a mixture of isobars using the survival yield technique. J. Am. Soc. Mass Spectrom. 22, 1744–1752 (2011)
Nasioudis, A., Memboeuf, A., Heeren, R.M.A., Smith, D.F., Vékey, K., Drahos, L., Van Den Brink, O.F.: Discrimination of polymers by using their characteristic collision energy in tandem mass spectrometry. Anal. Chem. 82, 9350–9356 (2010)
Katzenmeyer, B.C., Cool, L.R., Williams, J.P., Craven, K., Brown, J.M., Wesdemiotis, C.: Electron transfer dissociation of sodium cationized polyesters: reaction time effects and combination with collisional activation and ion mobility separation. Int. J. Mass Spectrom. 378, 303–311 (2015)
Burel, A., Carapito, C., Lutz, J.-F., Charles, L.: MS-DECODER: milliseconds sequencing of coded polymers. Macromolecules. 50, 8290–8296 (2017)
Chendo, C., Phan, T.N.T., Rollet, M., Gigmes, D., Charles, L.: Adduction of ammonium to polylactides to modify their dissociation behavior in collision-induced dissociation. Rapid Commun. Mass Spectrom. 32, 423–430 (2018)
Amalian, J.-A., Trinh, T.T., Lutz, J.-F., Charles, L.: MS/MS digital readout: analysis of binary information encoded in the monomer sequences of poly(triazole amide)s. Anal. Chem. 88, 3715–3722 (2016)
Amalian, J.-A., Poyer, S., Petit, B.E., Telitel, S., Monnier, V., Karamessini, D., Gigmes, D., Lutz, J.-F., Charles, L.: Negative mode MS/MS to read digital information encoded in sequence-defined oligo(urethane)s: a mechanistic study. Int. J. Mass Spectrom. 421, 271–278 (2017)
Kaczorowska, M.A., Cooper, H.J.: Electron capture dissociation, electron detachment dissociation, and collision-induced dissociation of polyamidoamine (PAMAM) dendrimer ions with amino, amidoethanol, and sodium carboxylate surface groups. J. Am. Soc. Mass Spectrom. 19, 1312–1319 (2008)
Kaczorowska, M.A., Cooper, H.J.: Characterization of polyphosphoesters by Fourier transform ion cyclotron resonance mass spectrometry. J. Am. Soc. Mass Spectrom. 20, 2238–2247 (2009)
Cerda, B., Horn, D., Breuker, K., Carpenter, B., McLafferty, F.: Electron capture dissociation of multiply-charged oxygenated cations. A nonergodic process. Eur. J. Mass Spectrom. 5, 335 (1999)
Cerda, B.A., Breuker, K., Horn, D.M., McLafferty, F.W.: Charge/radical site initiation versus coulombic repulsion for cleavage of multiply charged ions. Charge solvation in poly(alkene glycol) ions. J. Am. Soc. Mass Spectrom. 12, 565–570 (2001)
Cerda, B.A., Horn, D.M., Breuker, K., McLafferty, F.W.: Sequencing of specific copolymer oligomers by electron-capture-dissociation mass spectrometry. J. Am. Chem. Soc. 124, 9287–9291 (2002)
Altuntaş, E., Knop, K., Tauhardt, L., Kempe, K., Crecelius, A.C., Jäger, M., Hager, M.D., Schubert, U.S.: Tandem mass spectrometry of poly(ethylene imine)s by electrospray ionization (ESI) and matrix-assisted laser desorption/ionization (MALDI). J. Mass Spectrom. 47, 105–114 (2012)
Altuntas, E., Weber, C., Schubert, U.S.: Detailed characterization of poly(2-ethyl-2oxazoline)s by energy variable collision-induced dissociation study. Rapid Commun. Mass Spectrom. 27, 1095–1100 (2013)
Trimpin, S., Clemmer, D.E.: Ion mobility spectrometry/mass spectrometry snapshots for assessing the molecular compositions of complex polymeric systems. Anal. Chem. 80, 9073–9083 (2008)
Trimpin, S., Plasencia, M., Isailovic, D., Clemmer, D.E.: Resolving oligomers from fully grown polymers with IMS-MS. Anal. Chem. 79, 7965–7974 (2007)
Larriba, C., Fernandez De La Mora, J.: The gas phase structure of coulombically stretched polyethylene glycol ions. J. Phys. Chem. B. 116, 593–598 (2012)
Haler, J.R.N., Massonnet, P., Chirot, F., Kune, C., Comby-Zerbino, C., Jordens, J., Honing, M., Mengerink, Y., Far, J., Dugourd, P., De Pauw, E.: Comparison of different ion mobility setups using poly (ethylene oxide) PEO polymers: drift tube, TIMS, and T-wave. J. Am. Soc. Mass Spectrom. 29, 114–120 (2018)
Haler, J.R.N., Far, J., Aqil, A., Claereboudt, J., Tomczyk, N., Giles, K., Jérôme, C., De Pauw, E.: Multiple gas-phase conformations of a synthetic linear poly(acrylamide) polymer observed using ion mobility–mass spectrometry. J. Am. Soc. Mass Spectrom. 28, 2492–2499 (2017)
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)
Morsa, D., Defize, T., Dehareng, D., Jérôme, C., De Pauw, E.: Polymer topology revealed by ion mobility coupled with mass spectrometry. Anal. Chem. 86, 9693–9700 (2014)
Duez, Q., Josse, T., Lemaur, V., Chirot, F., Choi, C.M., Dubois, P., Dugourd, P., Cornil, J., Gerbaux, P., De Winter, J.: Correlation between the shape of the ion mobility signals and the stepwise folding process of polylactide ions. J. Mass Spectrom. 52, 133–138 (2017)
Haler, J.R.N., Morsa, D., Lecomte, P., Jérôme, C., Far, J., De Pauw, E.: Predicting ion mobility–mass spectrometry trends of polymers using the concept of apparent densities. Methods. 144, 125–133 (2018)
Wesdemiotis, C.: Multidimensional mass spectrometry of synthetic polymers and advanced materials. Angew. Chem. Int. Ed. 56, 1452–1464 (2017)
Larriba, C., De La Mora, J.F., Clemmer, D.E.: Electrospray ionization mechanisms for large polyethylene glycol chains studied through tandem ion mobility spectrometry. J. Am. Soc. Mass Spectrom. 25, 1332–1345 (2014)
de la Rosa, V.R., Tempelaar, S., Dubois, P., Hoogenboom, R., Mespouille, L.: Poly(2-ethyl-2-oxazoline)-block-polycarbonate block copolymers: from improved end-group control in poly(2-oxazoline)s to chain extension with aliphatic polycarbonate through a fully metal-free ring-opening polymerisation process. Polym. Chem. 7, 1559–1568 (2016)
Haler, J.R.N., Kune, C., Massonnet, P., Comby-Zerbino, C., Jordens, J., Honing, M., Mengerink, Y., Far, J., De Pauw, E.: Comprehensive ion mobility calibration: poly(ethylene oxide) polymer calibrants and general strategies. Anal. Chem. 89, 12076–12086 (2017)
Ruotolo, B.T., Benesch, J.L.P., Sandercock, A.M., Hyung, S.-J., Robinson, C.V.: Ion mobility–mass spectrometry analysis of large protein complexes. Nat. Protoc. 3, 1139–1152 (2008)
Counterman, A.E., Valentine, S.J., Srebalus, C.A., Henderson, S.C., Hoaglund, C.S., Clemmer, D.E.: High-order structure and dissociation of gaseous peptide aggregates that are hidden in mass spectra. J. Am. Soc. Mass Spectrom. 9, 743–759 (1998)
Bush, M.F., Campuzano, I.D.G., Robinson, C.V.: Ion mobility mass spectrometry of peptide ions: effects of drift gas and calibration strategies. Anal. Chem. 84, 7124–7130 (2012)
Valentine, S.J., Counterman, A.E., Clemmer, D.E.: Conformer-dependent proton-transfer reactions of ubiquitin ions. J. Am. Soc. Mass Spectrom. 8, 954–961 (1997)
Shelimov, K.B., Jarrold, M.F.: Vacuum: an activation barrier for gas-phase protein folding. J. Am. Chem. Soc. 119, 2987–2994 (1997)
Chen, Y.L., Collings, B.A., Douglas, D.J.: Collision cross sections of myoglobin and cytochrome c ions with Ne, Ar, and Kr. J. Am. Soc. Mass Spectrom. 8, 681–687 (1997)
Valentine, S.J., Anderson, J.G., Ellington, A.D., Clemmer, D.E.: Disulfide-intact and -reduced lysozyme in the gas phase: conformations and pathways of folding and unfolding. J. Phys. Chem. B. 101, 3891–3900 (1997)
Flanagan, J.M.: Mass spectrometry calibration using homogeneously substituted fluorinated triazatriphosphorines. US 5872357 A (1999)
Zhong, Y., Han, L., Ruotolo, B.T.: Collisional and coulombic unfolding of gas-phase proteins: high correlation to their domain structures in solution. Angew. Chem. Int. Ed. 53, 9209–9212 (2014)
Tian, Y., Han, L., Buckner, A.C., Ruotolo, B.T.: Collision induced unfolding of intact antibodies: rapid characterization of disulfide bonding patterns, glycosylation, and structures. Anal. Chem. 87, 11509–11515 (2015)
Duez, Q., Chirot, F., Liénard, R., Josse, T., Choi, C.M., Coulembier, O., Dugourd, P., Cornil, J., Gerbaux, P., De Winter, J.: Polymers for traveling wave ion mobility spectrometry calibration. J. Am. Soc. Mass Spectrom. 28, 2483–2491 (2017)
Lermyte, F., Łącki, M.K., Valkenborg, D., Gambin, A., Sobott, F.: Conformational space and stability of ETD charge reduction products of ubiquitin. J. Am. Soc. Mass Spectrom. 28, 69–76 (2017)
Morsa, D., Gabelica, V., De Pauw, E.: Fragmentation and isomerization due to field heating in traveling wave ion mobility spectrometry. J. Am. Soc. Mass Spectrom. 25, 1384–1393 (2014)
Counterman, A.E., Clemmer, D.E.: Anhydrous polyproline helices and globules. J. Phys. Chem. B. 108, 4885–4898 (2004)
Counterman, A.E., Clemmer, D.E.: Gas phase polyalanine: assessment of i → i + 3 and i → i + 4 helical turns in [Alan + 4H]4+ (n = 29–49) ion. J. Phys. Chem. B. 106, 12045–12051 (2002)
Breaux, G.A., Jarrold, M.F.: Probing helix formation in unsolvated peptides. J. Am. Chem. Soc. 125, 10740–10747 (2003)
Counterman, A.E., Clemmer, D.E.: Compact → extended helix transitions of polyalanine in vacuo. J. Phys. Chem. B. 107, 2111–2117 (2003)
Rossi, M., Blum, V., Kupser, P., Von Helden, G., Bierau, F., Pagel, K., Meijer, G., Scheffler, M.: Secondary structure of Ac-Alan-LysH+ polyalanine peptides (n = 5,10,15) in vacuo: helical or not? J. Phys. Chem. Lett. 1, 3465–3470 (2010)
Giles, K., Williams, J.P., Campuzano, I.: Enhancements in travelling wave ion mobility resolution. Rapid Commun. Mass Spectrom. 25, 1559–1566 (2011)
Ridgeway, M.E., Lubeck, M., Jordens, J., Mann, M., Park, M.A.: Trapped ion mobility spectrometry: a short review. Int. J. Mass Spectrom. 425, 22–35 (2018)
Michelmann, K., Silveira, J.A., Ridgeway, M.E., Park, M.A.: Fundamentals of trapped ion mobility spectrometry. J. Am. Soc. Mass Spectrom. 26, 14–24 (2014)
Badman, E.R., Myung, S., Clemmer, D.E.: Evidence for unfolding and refolding of gas-phase cytochrome c ions in a Paul trap. J. Am. Soc. Mass Spectrom. 16, 1493–1497 (2005)
Chen, S.H., Russell, D.H.: How closely related are conformations of protein ions sampled by IM-MS to native solution structures? J. Am. Soc. Mass Spectrom. 26, 1433–1443 (2015)
Bornschein, R.E., Niu, S., Eschweiler, J., Ruotolo, B.T.: Ion mobility–mass spectrometry reveals highly-compact intermediates in the collision induced dissociation of charge-reduced protein complexes. J. Am. Soc. Mass Spectrom. 27, 41–49 (2016)
Sun, Y., Vahidi, S., Sowole, M.A., Konermann, L.: Protein structural studies by traveling wave ion mobility spectrometry: a critical look at electrospray sources and calibration issues. J. Am. Soc. Mass Spectrom. 27, 31–40 (2016)
Hudgins, R.R., Mao, Y., Ratner, M.a., Jarrold, M.F.: Conformations of Gly(n)H+ and ala(n)H+ peptides in the gas phase. Biophys. J. 76, 1591–1597 (1999)
De Winter, J., Lemaur, V., Ballivian, R., Chirot, F., Coulembier, O., Antoine, R., Lemoine, J., Cornil, J., Dubois, P., Dugourd, P., Gerbaux, P.: Size dependence of the folding of multiply charged sodium cationized polylactides revealed by ion mobility mass spectrometry and molecular modelling. Chem. A Eur. J. 17, 9738–9745 (2011)
Tintaru, A., Chendo, C., Wang, Q., Viel, S., Quéléver, G., Peng, L., Posocco, P., Pricl, S., Charles, L.: Conformational sensitivity of conjugated poly(ethylene oxide)-poly(amidoamine) molecules to cations adducted upon electrospray ionization—a mass spectrometry, ion mobility and molecular modeling study. Anal. Chim. Acta. 808, 163–174 (2014)
von Helden, G., Wyttenbach, T., Bowers, M.T.: Inclusion of a MALDI ion source in the ion chromatography technique: conformational information on polymer and biomolecular ions. Int. J. Mass Spectrom. Ion Process. 146–147, 349–364 (1995)
Wyttenbach, T., Von Helden, G., Batka, J.J., Carlat, D., Bowers, M.T.: Effect of the long-range potential on ion mobility measurements. J. Am. Soc. Mass Spectrom. 8, 275–282 (1997)
Ujma, J., Giles, K., Morris, M., Barran, P.E.: New high resolution ion mobility mass spectrometer capable of measurements of collision cross sections from 150 to 520 K. Anal. Chem. 88, 9469–9478 (2016)
Dickinson, E.R., Jurneczko, E., Pacholarz, K.J., Clarke, D.J., Reeves, M., Ball, K.L., Hupp, T., Campopiano, D., Nikolova, P.V., Barran, P.E.: Insights into the conformations of three structurally diverse proteins: cytochrome c, p53, and MDM2, provided by variable-temperature ion mobility mass spectrometry. Anal. Chem. 87, 3231–3238 (2015)
Larriba, C., Hogan, C.J.: Ion mobilities in diatomic gases: measurement versus prediction with non-specular scattering models. J. Phys. Chem. A. 117, 3887–3901 (2013)
Larriba, C., Hogan, C.J.: Free molecular collision cross section calculation methods for nanoparticles and complex ions with energy accommodation. J. Comput. Phys. 251, 344–336 (2013)
Wu, T., Derrick, J., Nahin, M., Chen, X., Larriba-Andaluz, C.: Optimization of long range potential interaction parameters in ion mobility spectrometry. J. Chem. Phys. 148, 074102 (2018)
