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Synyhesis, structure, spectroscopy and redox chemistry of square-planar nickel(II) complexes with tetradentate o-phenylenedioxamidates and related ligands

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Synyhesis, structure, spectroscopy and redox chemistry of square-planar nickel(II) complexes with tetradentate o-phenylenedioxamidates and related ligands

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dc.contributor.author Ottenwaelder, X. es_ES
dc.contributor.author Aukauloo, A. es_ES
dc.contributor.author Journaux, Y. es_ES
dc.contributor.author Carrasco, R. es_ES
dc.contributor.author Cano, J. es_ES
dc.contributor.author Cervera, B. es_ES
dc.contributor.author Castro, I. es_ES
dc.contributor.author Cureli, S. es_ES
dc.contributor.author Muñoz Roca, María Del Carmen es_ES
dc.contributor.author Roselló, A. L. es_ES
dc.contributor.author Soto, B. es_ES
dc.contributor.author Ruiz-García, R. es_ES
dc.date.accessioned 2020-03-16T14:46:53Z
dc.date.available 2020-03-16T14:46:53Z
dc.date.issued 2005 es_ES
dc.identifier.issn 1477-9226 es_ES
dc.identifier.uri http://hdl.handle.net/10251/138964
dc.description.abstract [EN] A series of four-coordinate square-planar nickel(II) complexes of o-phenylenebis(N¿-methyloxamidate) (L1) and related o-phenylene(N¿-methyloxamidate)oxamate (L2) and o-phenylenebis(oxamate) (L3) tetradentate ligands have been synthesized and characterized structurally, spectroscopically and electrochemically. The parent nickel(II)¿L1 complex presents an intense MLCT band in the UV region (¿max = 357 nm) and a distinctive 1 s ¿ 4p CT satellite in the Ni K-edge XANES spectrum (E = 8339.2 eV). These features together with the short Ni¿N(amidate) bond lengths (1.85¿1.93 Å) as revealed by the analysis of the Ni K-edge EXAFS spectrum and confirmed by single-crystal X-ray diffraction are typical of square-planar low spin (S = 0) NiII ions. The dianionic nickel(II) complexes, [NiIILi]2¿ (i = 1¿3), experience two redox processes in acetonitrile at 25 °C. The first redox process, at moderately low potentials (E1 = 0.12¿0.52 V vs. SCE), is a reversible one-electron metal-centered oxidation to the corresponding monoanionic nickel(III) complexes, [NiIIILi]¿. The second redox process, at relatively high potentials (E2 = 0.86¿1.04 V vs. SCE), is a quasireversible to irreversible one-electron oxidation largely centered on the o-benzenediamidate fragment of the non-innocent ligand, yielding the corresponding neutral nickel(III) complexes with a o-benzosemiquinonediimine ¿-cation radical ligand, [NiIII(Li)¿+]. The singly and doubly oxidized species of the parent nickel(II)¿L1 complex have been prepared by chemical oxidation and characterized spectroscopically in acetonitrile at ¿40 °C. The stable singly oxidized nickel(III)¿L1 species presents an intense LMCT band in the NIR region (¿max = 910 nm) and a rhombic X-band EPR spectrum (g1 = 2.193, g2 = 2.080 and g3 = 2.006) characteristic of square-planar low spin (S = 1/2) NiIII ions. The unstable double oxidized nickel(III)¿L1 ¿-cation radical species exhibits a rather intense visible band (¿max = 645 nm) that is tentatively assigned as a MLCT transition from the NiIII-benzosemiquinone type ground state to the NiIV excited state. es_ES
dc.description.sponsorship This work was supported by the Ministerio de Ciencia y Tecnología (MCYT) (Spain) through the Plan Nacional de Investigación Científica, Desarrollo e Innovación Tecnológica (I + D + I) (BQU2001 2928) and the Ramón y Cajal programs. Further support from the European Community through the Human Potential Program Access to research infrastructures (Project CC005 97) is also acknowledged. B. S. thanks the Universitat de Valencia for a grant through the Una Nau de Solidaritat program. We are specially thankful to Dr I. Fernandez (Universitat de València) and Dr F. Villain (Universite Pierre et Marie Curie) for their assistance with the NMR and X-ray absorption measurements, respectively, and to Dr R. Pratt and Prof. T. D. P. Stack (Stanford University) for providing the thianthrenyl salt and access to low-temperature UV/VIS/NIR equipment, respectively es_ES
dc.language Inglés es_ES
dc.publisher The Royal Society of Chemistry es_ES
dc.relation.ispartof Dalton Transactions es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject.classification FISICA APLICADA es_ES
dc.title Synyhesis, structure, spectroscopy and redox chemistry of square-planar nickel(II) complexes with tetradentate o-phenylenedioxamidates and related ligands es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1039/B502478A es_ES
dc.relation.projectID info:eu-repo/grantAgreement/EC//CC005 97 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MICYT//BQU2001-2928/ES/Msíntesis, Estructura y Propiedades Magnéticas de Compuestos con Interacción de Canje entre Centros Metálicos/ es_ES
dc.rights.accessRights Cerrado es_ES
dc.contributor.affiliation Universitat Politècnica de València. Departamento de Física Aplicada - Departament de Física Aplicada es_ES
dc.description.bibliographicCitation Ottenwaelder, X.; Aukauloo, A.; Journaux, Y.; Carrasco, R.; Cano, J.; Cervera, B.; Castro, I.... (2005). Synyhesis, structure, spectroscopy and redox chemistry of square-planar nickel(II) complexes with tetradentate o-phenylenedioxamidates and related ligands. Dalton Transactions. 15:2516-2525. https://doi.org/10.1039/B502478A es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1039/B502478A es_ES
dc.description.upvformatpinicio 2516 es_ES
dc.description.upvformatpfin 2525 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 15 es_ES
dc.relation.pasarela S\230680 es_ES
dc.contributor.funder European Commission es_ES
dc.contributor.funder Ministerio de Ciencia y Tecnología es_ES
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