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dc.contributor.CRUESPUniversidade Estadual de Campinaspt_BR
dc.typeArtigo de periódicopt_BR
dc.titleInfinite zig-zag and cyclic-tetranuclear isomeric imidazolate-bridged polynuclear copper(II) complexes: Magnetic properties, catalytic activity and electrospray mass and tandem mass spectrometry characterizationpt_BR
dc.contributor.authorAlves, WApt_BR
dc.contributor.authorCerchiaro, Gpt_BR
dc.contributor.authorPaduan, Apt_BR
dc.contributor.authorTomazela, DMpt_BR
dc.contributor.authorEberlin, MNpt_BR
dc.contributor.authorFerreira, AMDpt_BR
unicamp.author.emailamdcferr@iq.usp.brpt_BR
unicamp.authorUniv Sao Paulo, Inst Quim, BR-05513970 Sao Paulo, Brazil Univ Sao Paulo, Inst Fis, Sao Paulo, Brazil Univ Estadual Campinas, Inst Quim, Lab Thomson Espectrometria Massas, Campinas, SP, Brazilpt_BR
dc.subjectcopper(II) complexespt_BR
dc.subjectESI mass spectrometrypt_BR
dc.subjectmagnetic propertiespt_BR
dc.subjectcatalytic activitypt_BR
dc.subject.wosBuilding-blockspt_BR
dc.subject.wosEpr-spectrapt_BR
dc.subject.wosCu-iipt_BR
dc.subject.wosTrinuclearpt_BR
dc.subject.wosDinuclearpt_BR
dc.subject.wosChemistrypt_BR
dc.subject.wosLigandpt_BR
dc.subject.wosHomochirogenesispt_BR
dc.subject.wosInterconversionpt_BR
dc.subject.wosDeprotonationpt_BR
dc.description.abstractTwo mononuclear copper(II) complexes 1 and 2 with the unsymmetrical tridentate ligands 2- and 4-[((imidazol-2-ylmethylidene)amino)ethyl]pyridine have been prepared. In alkaline solution, deprotonation of the imidazole moiety. in 1 and 2 promotes self-assembly, which yielded two structurally different species. Depending on the binding site in the imidazole ring, a polymeric complex with an infinite zig-zag-chain 3, or a cyclic-tetranuclear complex 4 is formed, as shown by spectroscopic and spectrometric analysis. Herein, structural characterization of these isomeric polynuclear complexes was performed by electrospray mass (ESI-MS) and tandem mass spectrometric experiments (ESI-MS/MS). Each isomer was shown to be stable in methanolic solutions and to display unique mass spectra with characteristic multiply charged molecular and fragment ions, corroborating previous data by EPR measurements. Magnetic data in the solid state fit a typical curve for an one-dimensional infinite regular chain system, with J= -(32.4 +/- 1.2) cm(-1) and g = 2.03 for 3, and that of a cyclic-tetranuclear structure with J = -(55.5 +/- 0.4) cm(-1) and g = 2.29 for 4. In the oxidation of 3,5-di-tert-butylcatechol (3,5-DTBC) by molecular oxygen, both complexes were shown to act as efficient catalysts, exhibiting very similar ratios: k(cat)/K-M = 9.12 x 10(6) mol(-1) dm(3) min(-1) for 3 and 8.73 x 10(6) mol(-1) dm(3) min(-1) for 4. These similar ratios indicate that interactions between the metal centres in 3 or 4 and the substrate in solution occur predominantly at the outside of the catalyst framework. (c) 2005 Elsevier B.V. All rights reserved.pt
dc.relation.ispartofInorganica Chimica Actapt_BR
dc.relation.ispartofabbreviationInorg. Chim. Actapt_BR
dc.publisher.cityLausannept_BR
dc.publisher.countrySuíçapt_BR
dc.publisherElsevier Science Sapt_BR
dc.date.issued2005pt_BR
dc.date.monthofcirculationSEP 1pt_BR
dc.identifier.citationInorganica Chimica Acta. Elsevier Science Sa, v. 358, n. 13, n. 3581, n. 3591, 2005.pt_BR
dc.language.isoenpt_BR
dc.description.volume358pt_BR
dc.description.issuenumber13pt_BR
dc.description.firstpage3581pt_BR
dc.description.lastpage3591pt_BR
dc.rightsfechadopt_BR
dc.rights.licensehttp://www.elsevier.com/about/open-access/open-access-policies/article-posting-policypt_BR
dc.sourceWeb of Sciencept_BR
unicamp.cruespUSPpt_BR
dc.identifier.issn0020-1693pt_BR
dc.identifier.wosidWOS:000232384400005pt_BR
dc.identifier.doi10.1016/j.ica.2005.06.006pt_BR
dc.date.available2014-11-19T15:32:43Z
dc.date.available2015-11-26T16:28:19Z-
dc.date.accessioned2014-11-19T15:32:43Z
dc.date.accessioned2015-11-26T16:28:19Z-
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dc.description.provenanceMade available in DSpace on 2015-11-26T16:28:19Z (GMT). No. of bitstreams: 2 WOS000232384400005.pdf: 419269 bytes, checksum: d0ebef291d4b3b263de2fd7925160f85 (MD5) WOS000232384400005.pdf.txt: 37849 bytes, checksum: 1be8a0e61ca8413c8c6298aa4207a926 (MD5) Previous issue date: 2005en
dc.identifier.urihttp://www.repositorio.unicamp.br/jspui/handle/REPOSIP/60152pt_BR
dc.identifier.urihttp://www.repositorio.unicamp.br/handle/REPOSIP/60152
dc.identifier.urihttp://repositorio.unicamp.br/jspui/handle/REPOSIP/60152-
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