title: An IMS-IMS threshold method for semi-quantitative determination of activation barriers: Interconversion of prolinecis↔transforms in triply protonated bradykinin.
abstract: Collisional activation of selected conformations by multidimensional ion mobility spectrometry (IMS-IMS), combined with mass spectrometry (MS), is described as a method to determine semi-quantitative activation energies for interconversion of different structures of the nonapeptide bradykinin (BK, Arg-Pro-Pro-Gly-Phe-Ser-Pro-Phe-Arg). This analysis is based on a calibration involving collision-induced dissociation measurements of ions with known dissociation energies (i.e., "thermometer" ions) such as leucine enkephalin, BK, and amino acid-metal cation systems. The energetic barriers between six conformations of [BK+3H]3+range from 0.23 ±0.01 to 0.55 ±0.03 eV. Prior results indicate that the major peaks in the IMS distributions correspond to specific combinations ofcisandtransconfigurations of the three proline residues in the peptide sequence. The analysis allows us to directly assess pathways for specific transitions. The combination of structural assignments, experimentally determined barrier heights, onset of the quasi-equilibrium region, and dissociation threshold are used to derive a semi-quantitative potential energy surface for main features of [BK+3H]3+.
authors.affiliation: Department of Chemistry, Indiana University, Bloomington, Indiana 47405 United States.
authors.forename: Nicholas A
authors.initials: NA
authors.lastname: Pierson
authors.affiliation: Department of Chemistry, Indiana University, Bloomington, Indiana 47405 United States.
authors.forename: David E
authors.initials: DE
authors.lastname: Clemmer
keywords: activation energy; ion mobility spectrometry; multi-dimensional; peptide conformation
references.citation: Anal Chem. 2005 May 15;77(10):3330-9
references.pmid: 15889926
references.citation: J Phys Chem A. 2008 Apr 17;112(15):3319-27
references.pmid: 18355061
references.citation: J Am Soc Mass Spectrom. 1998 Aug;9(8):743-59
references.pmid: 9692251
references.citation: Science. 1991 Dec 13;254(5038):1598-603
references.pmid: 1749933
references.citation: J Am Chem Soc. 1973 Sep 5;95(18):5946-8
references.pmid: 4733830
references.citation: J Am Chem Soc. 2006 Sep 6;128(35):11713-9
references.pmid: 16939296
references.citation: Biopolymers. 1975 Jun;14(6):1121-32
references.pmid: 1164539
references.citation: Annu Rev Anal Chem (Palo Alto Calif). 2008;1:293-327
references.pmid: 20636082
references.citation: Biopolymers. 1977 Jul;16(7):1465-72
references.pmid: 880368
references.citation: Mass Spectrom Rev. 2005 Jul-Aug;24(4):508-48
references.pmid: 15389847
references.citation: J Biomol Tech. 2002 Jun;13(2):56-61
references.pmid: 19498967
references.citation: Rapid Commun Mass Spectrom. 1994 May;8(5):394-400
references.pmid: 8025335
references.citation: Nature. 1971 Mar 12;230(5289):100-2
references.pmid: 4927005
references.citation: J Phys Chem B. 2010 Jun 17;114(23):7777-83
references.pmid: 20469905
references.citation: J Phys Chem B. 2011 Apr 21;115(15):4509-15
references.pmid: 21449553
references.citation: Chem Rev. 2001 Feb;101(2):391-444
references.pmid: 11712253
references.citation: Nat Struct Biol. 1997 Jan;4(1):10-9
references.pmid: 8989315
references.citation: Fold Des. 1997;2(4):S69-75
references.pmid: 9269572
references.citation: Mass Spectrom Rev. 2003 May-Jun;22(3):158-81
references.pmid: 12838543
references.citation: J Mass Spectrom. 2000 Dec;35(12):1391-8
references.pmid: 11180629
references.citation: J Am Chem Soc. 2013 Feb 27;135(8):3186-92
references.pmid: 23373819
references.citation: J Am Soc Mass Spectrom. 2005 Jun;16(6):893-905
references.pmid: 15878286
references.citation: Nature. 2007 Dec 13;450(7172):964-72
references.pmid: 18075575
references.citation: J Phys Chem B. 2006 Apr 13;110(14):7528-37
references.pmid: 16599534
references.citation: J Phys Chem A. 2006 Mar 23;110(11):3933-46
references.pmid: 16539415
references.citation: Chem Rev. 1999 Oct 13;99(10):3037-80
references.pmid: 11749510
references.citation: Anal Chem. 2010 Mar 15;82(6):2294-302
references.pmid: 20151701
references.citation: Annu Rev Phys Chem. 2014;65:175-96
references.pmid: 24328447
references.citation: Anal Chem. 1998 Oct 1;70(19):4111-9
references.pmid: 9784749
references.citation: Mass Spectrom Rev. 2011 Mar-Apr;30(2):298-320
references.pmid: 20669325
references.citation: Acc Chem Res. 2004 Dec;37(12):989-98
references.pmid: 15609991
references.citation: J Am Chem Soc. 2013 Dec 26;135(51):19147-53
references.pmid: 24313458
references.citation: Science. 2002 Jun 28;296(5577):2369-73
references.pmid: 12029064
references.citation: J Am Chem Soc. 2011 Sep 7;133(35):13810-3
references.pmid: 21830821
references.citation: Mass Spectrom Rev. 2009 Jul-Aug;28(4):640-54
references.pmid: 19338048
references.citation: Annu Rev Phys Chem. 1997;48:545-600
references.pmid: 9348663
references.citation: J Am Soc Mass Spectrom. 2007 Feb;18(2):322-31
references.pmid: 17084091
references.citation: Biochem J. 1956 Dec;64(4):701-5
references.pmid: 13382822
references.citation: J Phys Chem A. 2008 Feb 14;112(6):1286-93
references.pmid: 18215025
references.citation: J Am Chem Soc. 1996 Jul 31;118(30):7178-89
references.pmid: 16525512
references.citation: Mass Spectrom Rev. 2005 Mar-Apr;24(2):135-67
references.pmid: 15389858
references.citation: J Mass Spectrom. 2013 Mar;48(3):379-83
references.pmid: 23494795
references.citation: Proc Natl Acad Sci U S A. 2009 Dec 8;106(49):20746-51
references.pmid: 19923435
references.citation: J Am Soc Mass Spectrom. 2013 Mar;24(3):365-80
references.pmid: 23389479
references.citation: Anal Chem. 1998 Jun 1;70(11):2236-42
references.pmid: 9624897
references.citation: Anal Chem. 2000 Jul 1;72(13):2737-40
references.pmid: 10905301
references.citation: Anal Bioanal Chem. 2008 Jun;391(3):905-9
references.pmid: 18320175
references.citation: Proc Natl Acad Sci U S A. 1971 Nov;68(11):2712-5
references.pmid: 5288248
references.citation: J Am Soc Mass Spectrom. 1998 Apr;9(4):333-40
references.pmid: 9879363
references.citation: J Phys Chem A. 2008 Oct 16;112(41):10071-85
references.pmid: 18808103
references.citation: J Mass Spectrom. 2004 Oct;39(10):1091-112
references.pmid: 15481084
references.citation: Anal Chem. 2006 Jun 15;78(12):4161-74
references.pmid: 16771547
references.citation: Biophys Chem. 2004 Oct 1;111(2):135-42
references.pmid: 15381311
references.citation: J Am Chem Soc. 2002 May 15;124(19):5481-5
references.pmid: 11996590