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Effect of Metal Environment and Immobilization on the Catalytic Activity of a Cu Superoxide Dismutase Mimic

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dc.citation.titleInorganics
dc.citation.volume1-19
dc.contributor.orcidhttps://orcid.org/0009-0001-5428-1130
dc.contributor.orcidhttps://orcid.org/0000-0003-3339-0239
dc.contributor.orcidhttps://orcid.org/0000-0002-1547-6891
dc.creatorRichezzi, Micaela
dc.creatorFerreyra, Joaquín
dc.creatorSignorella, Sharon
dc.creatorPalopoli, Claudia
dc.creatorTerrestre, Gustavo
dc.creatorPellegri, Nora
dc.creatorHureau, Christelle
dc.creatorSignorella, Sandra R.
dc.date.accessioned2023-12-21T17:32:31Z
dc.date.available2023-12-21T17:32:31Z
dc.date.issued2023-10-27
dc.description.abstractThe Cu(II)/Cu(I) conversion involves variation in the coordination number and geometry around the metal center. Therefore, the flexibility/rigidity of the ligand plays a critical role in the design of copper superoxide dismutase (SOD) mimics. A 1,3-Bis[(pyridin-2-ylmethyl)(propargyl)amino]propane (pypapn), a flexible ligand with an N4-donor set, was used to prepare [Cu(pypapn)(ClO4)2], a trans-Cu(II) complex whose structure was determined by the X-ray diffraction. In DMF or water, perchlorate anions are exchanged with solvent molecules, affording [Cu(pypan)(solv)2]2+ that catalyzes O2•− dismutation with a second-order rate constant kMcF = 1.26 × 107 M−1 s−1, at pH 7.8. This high activity results from a combination of ligand flexibility, total charge, and labile binding sites, which places [Cu(pypapn)(solv)2]2+ above other mononuclear Cu(II) complexes with more favorable redox potentials. The covalent anchoring of the alkyne group of the complex to azide functionalized mesoporous silica through “click” chemistry resulted in the retention of the SOD activity and improved stability. A dicationic Cu(II)-N4-Schiff base complex encapsulated in mesoporous silica was also tested as an SOD mimic, displaying higher activity than the free complex, although lower than [Cu(pypapn)(solv)2]2+. The robustness of covalently attached or encapsulated doubly charged Cu(II) complexes in a mesoporous matrix appears as a suitable approach for the design of copper-based hybrid catalysts for O2•− dismutation under physiological conditions.
dc.description.filFil: Richezzi, Micaela. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario (IQUIR-CONICET); Argentina.
dc.description.filFil: Ferreyra, Joaquín. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario (IQUIR-CONICET); Argentina.
dc.description.filFil: Signorella, Sharon. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario (IQUIR-CONICET); Argentina.
dc.description.filFil: Palopoli, Claudia. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario (IQUIR-CONICET); Argentina.
dc.description.filFil: Terrestre, Gustavo. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario (IQUIR-CONICET); Argentina.
dc.description.filFil: Pellegri, Nora. Universidad Nacional de Rosario. Facultad de Ciencias Exactas, Ingeniería y Agrimensura. Instituto de Física Rosario (IFIR-CONICET); Argentina.
dc.description.filFil: Hureau, Christelle. Université de Toulouse. Laboratoire de Chimie de Coordination (LCC-CNRS); France.
dc.description.filFil: Signorella, Sandra R. Universidad Nacional de Rosario. Facultad de Ciencias Bioquímicas y Farmacéuticas. Instituto de Química Rosario (IQUIR-CONICET); Argentina.
dc.description.sponsorshipUniversidad Nacional de Rosario (UNR): PID 8002019040023UR, PID 80020220700136UR
dc.description.sponsorshipConsejo Nacional de Investigaciones Científicas y Técnicas (CONICET): PIP-0852, PUE-0068
dc.description.sponsorshipAgencia Nacional de Promoción Científica y Tecnológica (ANPCyT): PICT-2019-03276
dc.description.sponsorshipCentre National de la Recherche Scientifique (CNRS): PICS-07121
dc.description.versionpeerreviewed
dc.identifier.issn2304-6740
dc.identifier.urihttps://hdl.handle.net/2133/26641
dc.language.isoen
dc.publisherMDPI
dc.relation.publisherversionhttps://doi.org/10.3390/inorganics11110425
dc.relation.publisherversionhttps://www.mdpi.com/2304-6740/11/11/425
dc.rightsopenAccess
dc.rights.holderRichezzi, Micaela
dc.rights.holderFerreyra, Joaquín
dc.rights.holderSignorella, Sharon
dc.rights.holderSignorella, Sandra R.
dc.rights.holderTerrestre, Gustavo
dc.rights.holderPalopoli, Claudia
dc.rights.holderPellegri, Nora
dc.rights.holderHureau, Christelle
dc.rights.holderUniversidad Nacional de Rosario
dc.rights.textAttribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/
dc.subjectCu-based SOD mimic
dc.subjectStructure
dc.subjectMesoporous silica
dc.subjectClick chemistry
dc.subjectSOD activity
dc.titleEffect of Metal Environment and Immobilization on the Catalytic Activity of a Cu Superoxide Dismutase Mimic
dc.typearticulo
dc.type.collectionarticulo
dc.type.versionpublishedVersion

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(FBIOyF) Departamento de Química Física - Artículo de Revista