Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy

One approach to reduce the side effects of chemotherapy in cancer treatment is photodynamic therapy (PDT), which allows spatiotemporal control of the cytotoxicity. We have used the strategy of coordinating π-expansive ligands to increase the excited state lifetimes of Ir(III) half-sandwich complexes...

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Autores: Gonzalo-Navarro, Carlos, Zafon, Elisenda, Organero, Juan Angel, Jalón, Félix A., Lima, Joao Carlos, Espino, Gustavo, Rodríguez, Ana María, Santos, Lucía, Moro, Artur J., Barrabés, Sílvia, Castro, Jessica, Camacho-Aguayo, Javier, Massaguer, Anna, Manzano, Blanca R., Durá, Gema
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Universidad de Zaragoza
Repositorio:Zaguán. Repositorio Digital de la Universidad de Zaragoza
OAI Identifier:oai:zaguan.unizar.es:132292
Acceso en línea:http://zaguan.unizar.es/record/132292
Access Level:acceso abierto
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spelling Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic TherapyGonzalo-Navarro, CarlosZafon, ElisendaOrganero, Juan AngelJalón, Félix A.Lima, Joao CarlosEspino, GustavoRodríguez, Ana MaríaSantos, LucíaMoro, Artur J.Barrabés, SílviaCastro, JessicaCamacho-Aguayo, JavierMassaguer, AnnaManzano, Blanca R.Durá, GemaOne approach to reduce the side effects of chemotherapy in cancer treatment is photodynamic therapy (PDT), which allows spatiotemporal control of the cytotoxicity. We have used the strategy of coordinating π-expansive ligands to increase the excited state lifetimes of Ir(III) half-sandwich complexes in order to facilitate the generation of 1O2. We have obtained derivatives of formulas [Cp*Ir(C∧N)Cl] and [Cp*Ir(C∧N)L]BF4 with different degrees of π-expansion in the C∧N ligands. Complexes with the more π-expansive ligand are very effective photosensitizers with phototoxic indexes PI > 2000. Furthermore, PI values of 63 were achieved with red light. Time-dependent density functional theory (TD-DFT) calculations nicely explain the effect of the π-expansion. The complexes produce reactive oxygen species (ROS) at the cellular level, causing mitochondrial membrane depolarization, cleavage of DNA, nicotinamide adenine dinucleotide (NADH) oxidation, as well as lysosomal damage. Consequently, cell death by apoptosis and secondary necrosis is activated. Thus, we describe the first class of half-sandwich iridium cyclometalated complexes active in PDT.2024info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://zaguan.unizar.es/record/132292reponame:Zaguán. Repositorio Digital de la Universidad de Zaragozainstname:Universidad de ZaragozaInglésinfo:eu-repo/grantAgreement/ES/MCIU/PID2019-105408GB-I00info:eu-repo/grantAgreement/ES/MCIU/PID2021-127187OB-C21info:eu-repo/grantAgreement/ES/MCIU/PID2021-127187OB-C22info:eu-repo/semantics/openAccessoai:zaguan.unizar.es:1322922026-05-29T13:59:51Z
dc.title.none.fl_str_mv Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
title Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
spellingShingle Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
Gonzalo-Navarro, Carlos
title_short Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
title_full Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
title_fullStr Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
title_full_unstemmed Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
title_sort Ir(III) Half-Sandwich Photosensitizers with a p-Expansive Ligand for Efficient Anticancer Photodynamic Therapy
dc.creator.none.fl_str_mv Gonzalo-Navarro, Carlos
Zafon, Elisenda
Organero, Juan Angel
Jalón, Félix A.
Lima, Joao Carlos
Espino, Gustavo
Rodríguez, Ana María
Santos, Lucía
Moro, Artur J.
Barrabés, Sílvia
Castro, Jessica
Camacho-Aguayo, Javier
Massaguer, Anna
Manzano, Blanca R.
Durá, Gema
author Gonzalo-Navarro, Carlos
author_facet Gonzalo-Navarro, Carlos
Zafon, Elisenda
Organero, Juan Angel
Jalón, Félix A.
Lima, Joao Carlos
Espino, Gustavo
Rodríguez, Ana María
Santos, Lucía
Moro, Artur J.
Barrabés, Sílvia
Castro, Jessica
Camacho-Aguayo, Javier
Massaguer, Anna
Manzano, Blanca R.
Durá, Gema
author_role author
author2 Zafon, Elisenda
Organero, Juan Angel
Jalón, Félix A.
Lima, Joao Carlos
Espino, Gustavo
Rodríguez, Ana María
Santos, Lucía
Moro, Artur J.
Barrabés, Sílvia
Castro, Jessica
Camacho-Aguayo, Javier
Massaguer, Anna
Manzano, Blanca R.
Durá, Gema
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
description One approach to reduce the side effects of chemotherapy in cancer treatment is photodynamic therapy (PDT), which allows spatiotemporal control of the cytotoxicity. We have used the strategy of coordinating π-expansive ligands to increase the excited state lifetimes of Ir(III) half-sandwich complexes in order to facilitate the generation of 1O2. We have obtained derivatives of formulas [Cp*Ir(C∧N)Cl] and [Cp*Ir(C∧N)L]BF4 with different degrees of π-expansion in the C∧N ligands. Complexes with the more π-expansive ligand are very effective photosensitizers with phototoxic indexes PI > 2000. Furthermore, PI values of 63 were achieved with red light. Time-dependent density functional theory (TD-DFT) calculations nicely explain the effect of the π-expansion. The complexes produce reactive oxygen species (ROS) at the cellular level, causing mitochondrial membrane depolarization, cleavage of DNA, nicotinamide adenine dinucleotide (NADH) oxidation, as well as lysosomal damage. Consequently, cell death by apoptosis and secondary necrosis is activated. Thus, we describe the first class of half-sandwich iridium cyclometalated complexes active in PDT.
publishDate 2024
dc.date.none.fl_str_mv 2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://zaguan.unizar.es/record/132292
url http://zaguan.unizar.es/record/132292
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/ES/MCIU/PID2019-105408GB-I00
info:eu-repo/grantAgreement/ES/MCIU/PID2021-127187OB-C21
info:eu-repo/grantAgreement/ES/MCIU/PID2021-127187OB-C22
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv
publisher.none.fl_str_mv
dc.source.none.fl_str_mv reponame:Zaguán. Repositorio Digital de la Universidad de Zaragoza
instname:Universidad de Zaragoza
instname_str Universidad de Zaragoza
reponame_str Zaguán. Repositorio Digital de la Universidad de Zaragoza
collection Zaguán. Repositorio Digital de la Universidad de Zaragoza
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