The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States

The Ru complex [RuII(bda‐κ‐N2O2)(N‐NH2)2] (1; bda2−=2,2′‐bipyridine‐6,6′‐dicarboxylate, N‐NH2=4‐(pyridin‐4‐yl)aniline) was used as a synthetic intermediate to prepare new RuII and RuIII bda complexes that contain NO+, MeCN, or H2O ligands. In acidic solution complex 1 reacts with an excess of NO+ (g...

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Autores: Matheu, Roc, Ghaderian, Abolfazl, Francàs, Laia, Chernev, Petko, Ertem, Mehmed Z., Benet-Buchholz, Jordi, Batista, Victor, Haumann, Michael, Gimbert-Suriñach, Carolina, Sala, Xavier, LLobet, Antoni
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/334659
Acceso en línea:http://hdl.handle.net/2072/334659
https://doi.org/10.1002/chem.201801236
Access Level:acceso abierto
Palabra clave:54
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spelling The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation StatesMatheu, RocGhaderian, AbolfazlFrancàs, LaiaChernev, PetkoErtem, Mehmed Z.Benet-Buchholz, JordiBatista, VictorHaumann, MichaelGimbert-Suriñach, CarolinaSala, XavierLLobet, Antoni54The Ru complex [RuII(bda‐κ‐N2O2)(N‐NH2)2] (1; bda2−=2,2′‐bipyridine‐6,6′‐dicarboxylate, N‐NH2=4‐(pyridin‐4‐yl)aniline) was used as a synthetic intermediate to prepare new RuII and RuIII bda complexes that contain NO+, MeCN, or H2O ligands. In acidic solution complex 1 reacts with an excess of NO+ (generated in situ from sodium nitrite) to form a new Ru complex in which the aryl amine ligand N−NH2 is transformed into a diazonium salt [N‐N2+=4‐(pyridin‐4‐yl)benzenediazonium)] together with the formation of a new Ru(NO) moiety in the equatorial zone, to generate [RuII(bda‐κ‐N2O)(NO)(N‐N2)2]3+ (23+). Here the bda2− ligand binds in a κ‐N2O tridentate manner with a dangling carboxylate group. Similarly, complex 1 can also react with a coordinating solvent, such as MeCN, at room temperature to give [RuII(bda‐κ‐N2O)(MeCN)(N‐NH2)2] (3). In acidic aqueous solutions, a related reaction occurs in which solvent water coordinates to the Ru center to form {[RuII{bda‐κ‐(NO)3}(H2O)(N‐NH3)2](H2O)n}2+ (42+) and is strongly hydrogen‐bonded with additional water molecules in the second coordination sphere. Furthermore, under acidic conditions the aniline ligands are also protonated to form the corresponding anilinium cationic ligands N‐NH3+. Additionally, the one‐electron oxidized complex {[RuIII{bda‐κ‐(NO)3.5}(H2O)(N‐NH3)2](H2O)n}3+ (53+) was characterized, in which the fractional value in the κ notation indicates the presence of an additional contact to the pseudo‐octahedral geometrWiley2018info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersion12838 p.application/pdfhttp://hdl.handle.net/2072/334659https://doi.org/10.1002/chem.201801236RECERCAT (Dipòsit de la Recerca de Catalunya)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésChemistry: A European JournalL'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:recercat.cat:2072/3346592026-05-29T05:05:01Z
dc.title.none.fl_str_mv The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
title The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
spellingShingle The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
Matheu, Roc
54
title_short The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
title_full The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
title_fullStr The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
title_full_unstemmed The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
title_sort The Behavior of the Ru-bda Water Oxidation Catalysts at Low Oxidation States
dc.creator.none.fl_str_mv Matheu, Roc
Ghaderian, Abolfazl
Francàs, Laia
Chernev, Petko
Ertem, Mehmed Z.
Benet-Buchholz, Jordi
Batista, Victor
Haumann, Michael
Gimbert-Suriñach, Carolina
Sala, Xavier
LLobet, Antoni
author Matheu, Roc
author_facet Matheu, Roc
Ghaderian, Abolfazl
Francàs, Laia
Chernev, Petko
Ertem, Mehmed Z.
Benet-Buchholz, Jordi
Batista, Victor
Haumann, Michael
Gimbert-Suriñach, Carolina
Sala, Xavier
LLobet, Antoni
author_role author
author2 Ghaderian, Abolfazl
Francàs, Laia
Chernev, Petko
Ertem, Mehmed Z.
Benet-Buchholz, Jordi
Batista, Victor
Haumann, Michael
Gimbert-Suriñach, Carolina
Sala, Xavier
LLobet, Antoni
author2_role author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv 54
topic 54
description The Ru complex [RuII(bda‐κ‐N2O2)(N‐NH2)2] (1; bda2−=2,2′‐bipyridine‐6,6′‐dicarboxylate, N‐NH2=4‐(pyridin‐4‐yl)aniline) was used as a synthetic intermediate to prepare new RuII and RuIII bda complexes that contain NO+, MeCN, or H2O ligands. In acidic solution complex 1 reacts with an excess of NO+ (generated in situ from sodium nitrite) to form a new Ru complex in which the aryl amine ligand N−NH2 is transformed into a diazonium salt [N‐N2+=4‐(pyridin‐4‐yl)benzenediazonium)] together with the formation of a new Ru(NO) moiety in the equatorial zone, to generate [RuII(bda‐κ‐N2O)(NO)(N‐N2)2]3+ (23+). Here the bda2− ligand binds in a κ‐N2O tridentate manner with a dangling carboxylate group. Similarly, complex 1 can also react with a coordinating solvent, such as MeCN, at room temperature to give [RuII(bda‐κ‐N2O)(MeCN)(N‐NH2)2] (3). In acidic aqueous solutions, a related reaction occurs in which solvent water coordinates to the Ru center to form {[RuII{bda‐κ‐(NO)3}(H2O)(N‐NH3)2](H2O)n}2+ (42+) and is strongly hydrogen‐bonded with additional water molecules in the second coordination sphere. Furthermore, under acidic conditions the aniline ligands are also protonated to form the corresponding anilinium cationic ligands N‐NH3+. Additionally, the one‐electron oxidized complex {[RuIII{bda‐κ‐(NO)3.5}(H2O)(N‐NH3)2](H2O)n}3+ (53+) was characterized, in which the fractional value in the κ notation indicates the presence of an additional contact to the pseudo‐octahedral geometr
publishDate 2018
dc.date.none.fl_str_mv 2018
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/2072/334659
https://doi.org/10.1002/chem.201801236
url http://hdl.handle.net/2072/334659
https://doi.org/10.1002/chem.201801236
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Chemistry: A European Journal
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 12838 p.
application/pdf
dc.publisher.none.fl_str_mv Wiley
publisher.none.fl_str_mv Wiley
dc.source.none.fl_str_mv RECERCAT (Dipòsit de la Recerca de Catalunya)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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