Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency

The preparation of highly efficient photoluminescent rare-earth based coordination compounds, characterized by photoluminescence quantum yield (PLQY) over 90% and thermal/chemical stability that allows their processing in various media (aqueous solutions, polymeric films, etc.) holds enormous signif...

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Autores: Razquin Bobillo, Laura, Zabala Lekuona, Andoni, García Martínez, José Ángel, Rodríguez Diéguez, Antonio, Cepeda Ruiz, Javier
Formato: artículo
Fecha de publicación:2024
País:España
Recursos:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/70935
Acesso em linha:http://hdl.handle.net/10810/70935
Access Level:acceso abierto
Palavra-chave:coordination polymers
DFT calculations
highly efficient photoluminescence
water-soluble complex
thin films
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spelling Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum EfficiencyRazquin Bobillo, LauraZabala Lekuona, AndoniGarcía Martínez, José ÁngelRodríguez Diéguez, AntonioCepeda Ruiz, Javiercoordination polymersDFT calculationshighly efficient photoluminescencewater-soluble complexthin filmsThe preparation of highly efficient photoluminescent rare-earth based coordination compounds, characterized by photoluminescence quantum yield (PLQY) over 90% and thermal/chemical stability that allows their processing in various media (aqueous solutions, polymeric films, etc.) holds enormous significance in their applicability. Herein, a family of isostructural coordination polymers (CPs) with 6-methyl-2-oxonicotinate (6m2onic) ligand, chemically and structurally characterized as {[M(6m2onic)4Na(H2O)3]·8H2O}n [where M(III) = Eu (1Eu), Tb (2Tb), Gd (3Gd), Y (4Y) and Eu0.5Tb0.5 (5Eu-Tb)], are reported. Their peculiar crystal structure, based on a hydrogen-bonded framework of 1D arrays in which octacoordinated metal centers (established by four chelating 6m2onic ligands) and Na centers are sequentially linked, gives rise to an excellent metal–organic system benefitting from not only bright PL emissions in solid state but also enough chemical and thermal stability as to yield PL water-soluble complexes and photostable thin-films. In particular, the terbium(III)-based counterpart highlights for its first-in-class PLQY and versatility, which imbues the compound with efficiencies of 97% in bulk state, 35% in aqueous solution, 85% in polymer-based thin-films and 15% after its calcination at 250 °C. The experimental photophysical characterization in those media, involving also pH-responsive behavior, is well supported by a solid theoretical analysis of their intramolecular transfers and electronic transitions.This work has been funded by the Spanish Ministry of Science, Innovation and Universities (TED2021-132440B-I00), Red Guipuzcoana de Ciencia, Tecnología e Innovación (FA385/2023, DG23/16), Gobierno Vasco/Eusko Jaurlaritza (IT1755-22 and IT1500-22), and Junta de Andalucía (FQM-394, B-FQM-734-UGR2). LRB thanks his predoctoral fellowship to UPV/EHU. The authors thank for technical and human support provided by SGIker (UPV/EHU/ ERDF, EU).Wiley202420242024info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/70935reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/MICINN/TED2021-132440B-I00/https://onlinelibrary.wiley.com/doi/full/10.1002/adom.202401472info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc/4.0/© 2024 The Author(s). Advanced Optical Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.oai:addi.ehu.eus:10810/709352026-06-18T09:23:17Z
dc.title.none.fl_str_mv Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
title Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
spellingShingle Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
Razquin Bobillo, Laura
coordination polymers
DFT calculations
highly efficient photoluminescence
water-soluble complex
thin films
title_short Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
title_full Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
title_fullStr Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
title_full_unstemmed Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
title_sort Water Soluble Rare-Earth(III) based Coordination Polymers with Luminescence Versatility in Various Media: Reaching the Sky of Quantum Efficiency
dc.creator.none.fl_str_mv Razquin Bobillo, Laura
Zabala Lekuona, Andoni
García Martínez, José Ángel
Rodríguez Diéguez, Antonio
Cepeda Ruiz, Javier
author Razquin Bobillo, Laura
author_facet Razquin Bobillo, Laura
Zabala Lekuona, Andoni
García Martínez, José Ángel
Rodríguez Diéguez, Antonio
Cepeda Ruiz, Javier
author_role author
author2 Zabala Lekuona, Andoni
García Martínez, José Ángel
Rodríguez Diéguez, Antonio
Cepeda Ruiz, Javier
author2_role author
author
author
author
dc.subject.none.fl_str_mv coordination polymers
DFT calculations
highly efficient photoluminescence
water-soluble complex
thin films
topic coordination polymers
DFT calculations
highly efficient photoluminescence
water-soluble complex
thin films
description The preparation of highly efficient photoluminescent rare-earth based coordination compounds, characterized by photoluminescence quantum yield (PLQY) over 90% and thermal/chemical stability that allows their processing in various media (aqueous solutions, polymeric films, etc.) holds enormous significance in their applicability. Herein, a family of isostructural coordination polymers (CPs) with 6-methyl-2-oxonicotinate (6m2onic) ligand, chemically and structurally characterized as {[M(6m2onic)4Na(H2O)3]·8H2O}n [where M(III) = Eu (1Eu), Tb (2Tb), Gd (3Gd), Y (4Y) and Eu0.5Tb0.5 (5Eu-Tb)], are reported. Their peculiar crystal structure, based on a hydrogen-bonded framework of 1D arrays in which octacoordinated metal centers (established by four chelating 6m2onic ligands) and Na centers are sequentially linked, gives rise to an excellent metal–organic system benefitting from not only bright PL emissions in solid state but also enough chemical and thermal stability as to yield PL water-soluble complexes and photostable thin-films. In particular, the terbium(III)-based counterpart highlights for its first-in-class PLQY and versatility, which imbues the compound with efficiencies of 97% in bulk state, 35% in aqueous solution, 85% in polymer-based thin-films and 15% after its calcination at 250 °C. The experimental photophysical characterization in those media, involving also pH-responsive behavior, is well supported by a solid theoretical analysis of their intramolecular transfers and electronic transitions.
publishDate 2024
dc.date.none.fl_str_mv 2024
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/70935
url http://hdl.handle.net/10810/70935
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/MICINN/TED2021-132440B-I00/
https://onlinelibrary.wiley.com/doi/full/10.1002/adom.202401472
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by-nc/4.0/
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc/4.0/
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Wiley
publisher.none.fl_str_mv Wiley
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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