Mostrar el registro sencillo del ítem
dc.contributor.author
Cattaneo, Mauricio
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.contributor.author
Parada, Giovanny A.
dc.contributor.author
Tenderholt, Adam L.
dc.contributor.author
Kaminsky, Werner
dc.contributor.author
Mayer, James M.
dc.date.available
2021-11-25T13:32:00Z
dc.date.issued
2021-10-21
dc.identifier.citation
Cattaneo, Mauricio; Parada, Giovanny A.; Tenderholt, Adam L.; Kaminsky, Werner; Mayer, James M.; Structural, electronic, and thermochemical preference for multi-PCET reactivity of ruthenium(II)-amine and ruthenium(IV)-amido complexes; Wiley VCH Verlag; European Journal of Inorganic Chemistry; 2021; 39; 21-10-2021; 4066-4073
dc.identifier.issn
1434-1948
dc.identifier.uri
http://hdl.handle.net/11336/147392
dc.description.abstract
The multiredox reactivity of bioinorganic cofactors is often coupled to proton transfers. Here we investigate the structural, thermochemical, and electronic structure of ruthenium-amino/amido complexes with multi- proton-coupled electron transfer reactivity. The bis(amino)ruthenium(II) and bis(amido)ruthenium(IV) complexes [RuII(bpy)(en*)2]2+ (RuII-H0 ) and [RuIV(bpy)(en*-H2)2]2+ (RuIV-H2 ) interconvert reversibly with the transfer of 2e-/2H+ (bpy = 2,2'-bipyridine, en* = 2,3-diamino-2,3-dimethylbutane). X-ray structures allow correlations between the structural and electronic parameters, and the thermochemical data of the 2e-/2H+ multi-square grid scheme. Redox potentials, acidity constants and DFT calculations reveal potential intermediates implicated in 2e-/2H+ reactivity with organic reagents in non-protic solvents, which shows a strong inverted redox potential favouring 2e-/2H+ transfer. This is suggested to be an attractive system for potential one-step (concerted) transfer of 2e-and 2H+ due to the small changes of the pseudo-octahedral geometries and the absence of charge change, indicating a relatively small overall reorganization energy.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
Wiley VCH Verlag
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.rights
info:eu-repo/semantics/restrictedAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
AMIDO COMPLEXES
dc.subject
ELECTRONIC STRUCTURE
dc.subject
PCET
dc.subject
REDOX CHEMISTRY
dc.subject
RUTHENIUM
dc.subject
MULTIREDOX
dc.subject.classification
Química Inorgánica y Nuclear
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.subject.classification
Ciencias Químicas
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.title
Structural, electronic, and thermochemical preference for multi-PCET reactivity of ruthenium(II)-amine and ruthenium(IV)-amido complexes
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2021-11-23T13:38:01Z
dc.identifier.eissn
1099-0682
dc.journal.volume
2021
dc.journal.number
39
dc.journal.pagination
4066-4073
dc.journal.pais
Alemania
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.journal.ciudad
Weinheim
dc.description.fil
Fil: Cattaneo, Mauricio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; Argentina
dc.description.fil
Fil: Parada, Giovanny A.. University of Yale; Estados Unidos. College of New Jersey; Estados Unidos
dc.description.fil
Fil: Tenderholt, Adam L.. University of Washington; Estados Unidos
dc.description.fil
Fil: Kaminsky, Werner. University of Washington; Estados Unidos
dc.description.fil
Fil: Mayer, James M.. University of Yale; Estados Unidos
dc.journal.title
European Journal of Inorganic Chemistry
![Se ha confirmado la validez de este valor de autoridad por un usuario](/themes/CONICETDigital/images/authority_control/invisible.gif)
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ejic.202100604
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1002/ejic.202100604
Archivos asociados