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Article: Energetics and dynamics of electron transfer and proton transfer in dissociation of metalIII(salen)-peptide complexes in the gas phase

TitleEnergetics and dynamics of electron transfer and proton transfer in dissociation of metalIII(salen)-peptide complexes in the gas phase
Authors
Issue Date2008
PublisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journals/jacsat/index.html
Citation
Journal Of The American Chemical Society, 2008, v. 130 n. 10, p. 3218-3230 How to Cite?
AbstractTime- and collision energy-resolved surface-induced dissociation (SID) of ternary complexes of CoIII(salen)+, Fe III(salen)+, and MnIII(salen)+ with several angiotensin peptide analogues was studied using a Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS) specially equipped to perform SID experiments. Time-resolved fragmentation efficiency curves (TFECs) were modeled using an RRKM-based approach developed in our laboratory. The approach utilizes a very flexible analytical expression for the internal energy deposition function that is capable of reproducing both single-collision and multiple-collision activation in the gas phase and excitation by collisions with a surface. The energetics and dynamics of competing dissociation pathways obtained from the modeling provides important insight on the competition between proton transfer, electron transfer, loss of neutral peptide ligand, and other processes that determine gas-phase fragmentation of these model systems. Similar fragmentation behavior was obtained for various CoIII(salen)-peptide systems of different angiotensin analogues. In contrast, dissociation pathways and relative stabilities of the complexes changed dramatically when cobalt was replaced with trivalent iron or manganese. We demonstrate that the electron-transfer efficiency is correlated with redox properties of the metalIII(salen) complexes (Co > Fe > Mn), while differences in the types of fragments formed from the complexes reflect differences in the modes of binding between the metal-salen complex and the peptide ligand. RRKM modeling of time- and collision-energy-resolved SID data suggests that the competition between proton transfer and electron transfer during dissociation of CoIII(salen)-peptide complexes is mainly determined by differences in entropy effects while the energetics of these two pathways are very similar. © 2008 American Chemical Society.
Persistent Identifierhttp://hdl.handle.net/10722/68921
ISSN
2015 Impact Factor: 13.038
2015 SCImago Journal Rankings: 7.123
ISI Accession Number ID
References

 

DC FieldValueLanguage
dc.contributor.authorLaskin, Jen_HK
dc.contributor.authorYang, Zen_HK
dc.contributor.authorChu, IKen_HK
dc.date.accessioned2010-09-06T06:08:55Z-
dc.date.available2010-09-06T06:08:55Z-
dc.date.issued2008en_HK
dc.identifier.citationJournal Of The American Chemical Society, 2008, v. 130 n. 10, p. 3218-3230en_HK
dc.identifier.issn0002-7863en_HK
dc.identifier.urihttp://hdl.handle.net/10722/68921-
dc.description.abstractTime- and collision energy-resolved surface-induced dissociation (SID) of ternary complexes of CoIII(salen)+, Fe III(salen)+, and MnIII(salen)+ with several angiotensin peptide analogues was studied using a Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS) specially equipped to perform SID experiments. Time-resolved fragmentation efficiency curves (TFECs) were modeled using an RRKM-based approach developed in our laboratory. The approach utilizes a very flexible analytical expression for the internal energy deposition function that is capable of reproducing both single-collision and multiple-collision activation in the gas phase and excitation by collisions with a surface. The energetics and dynamics of competing dissociation pathways obtained from the modeling provides important insight on the competition between proton transfer, electron transfer, loss of neutral peptide ligand, and other processes that determine gas-phase fragmentation of these model systems. Similar fragmentation behavior was obtained for various CoIII(salen)-peptide systems of different angiotensin analogues. In contrast, dissociation pathways and relative stabilities of the complexes changed dramatically when cobalt was replaced with trivalent iron or manganese. We demonstrate that the electron-transfer efficiency is correlated with redox properties of the metalIII(salen) complexes (Co > Fe > Mn), while differences in the types of fragments formed from the complexes reflect differences in the modes of binding between the metal-salen complex and the peptide ligand. RRKM modeling of time- and collision-energy-resolved SID data suggests that the competition between proton transfer and electron transfer during dissociation of CoIII(salen)-peptide complexes is mainly determined by differences in entropy effects while the energetics of these two pathways are very similar. © 2008 American Chemical Society.en_HK
dc.languageengen_HK
dc.publisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journals/jacsat/index.htmlen_HK
dc.relation.ispartofJournal of the American Chemical Societyen_HK
dc.titleEnergetics and dynamics of electron transfer and proton transfer in dissociation of metalIII(salen)-peptide complexes in the gas phaseen_HK
dc.typeArticleen_HK
dc.identifier.openurlhttp://library.hku.hk:4550/resserv?sid=HKU:IR&issn=0002-7863&volume=130&spage=3218&epage=3230&date=2008&atitle=Energetics+and+Dynamics+of+Electron+Transfer+and+Proton+Transfer+in+Dissociation+of+MetalIII(salen)-Peptide+Complexes+in+the+Gas+Phaseen_HK
dc.identifier.emailChu, IK:ivankchu@hku.hken_HK
dc.identifier.authorityChu, IK=rp00683en_HK
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1021/ja077690sen_HK
dc.identifier.pmid18266367-
dc.identifier.scopuseid_2-s2.0-41449109213en_HK
dc.identifier.hkuros141980en_HK
dc.relation.referenceshttp://www.scopus.com/mlt/select.url?eid=2-s2.0-41449109213&selection=ref&src=s&origin=recordpageen_HK
dc.identifier.volume130en_HK
dc.identifier.issue10en_HK
dc.identifier.spage3218en_HK
dc.identifier.epage3230en_HK
dc.identifier.isiWOS:000253854400064-
dc.publisher.placeUnited Statesen_HK
dc.identifier.scopusauthoridLaskin, J=7102409836en_HK
dc.identifier.scopusauthoridYang, Z=7405435606en_HK
dc.identifier.scopusauthoridChu, IK=7103327484en_HK

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