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dc.contributor.authorRouco Méndez, Lara
dc.contributor.authorFernández García, María Isabel
dc.contributor.authorPedrido Castiñeiras, Rosa María
dc.contributor.authorBotana López, Luis Miguel
dc.contributor.authorEsteban Gómez, David
dc.contributor.authorPlatas Iglesias, Carlos
dc.contributor.authorManeiro Maneiro, Marcelino
dc.date.accessioned2020-05-29T17:54:56Z
dc.date.available2020-05-29T17:54:56Z
dc.date.issued2018
dc.identifier.citationRouco, L.; Fernández-García, M.I.; Pedrido, R.; Botana, L.M.; Esteban-Gómez, D.; Platas-Iglesias, C.; Maneiro, M. Modeling the OEC with Two New Biomimetic Models: Preparations, Structural Characterization, and Water Photolysis Studies of a Ba–Mn Box Type Complex and a Mn4N6 Planar-Diamond Cluster. Catalysts 2018, 8, 382
dc.identifier.urihttp://hdl.handle.net/10347/22700
dc.description.abstractThe oxygen-evolving complex (OEC) is the native enzyme that catalyzes the oxidation of water in natural photosynthesis. Two new classes of manganese cluster complexes of formula Ba2Mn2L12(H3L1)2(CH3OH)4 1 and Mn4L26Cl2 2 were prepared (H4L1 = N,N′-(ethane-1,2-diyl)bis(2-hydroxybenzamide); L2 = methyl picolinimidate) and characterized by standard techniques including microanalysis, IR spectroscopy, ESI spectrometry, and magnetic susceptibility measurements. X-ray diffraction studies of these complexes revealed (i) a box-type structure for 1 formed by two redox-active manganese(III) ions and two barium(II) ions connected by two bridging bisamido-bisphenoxy ligand molecules; and (ii) a planar-diamond array for Mn4N6 cluster 2 where the picolinimidates act as chelating ligands through the two nitrogen atoms. The ability of 1 and 2 to split water has been studied by means of water photolysis experiments. In these experiments, the oxygen evolution was measured in aqueous media in the presence of p-benzoquinone (acting as the hydrogen acceptor), the reduction of which was followed by UV-spectroscopy. The relevant photolytic activity found for 1 is in contrast to the inactivity of 2 in the photolytic experiments. This different behavior is discussed on the basis of the structure of the biomimetic models and the proposed reaction mechanism for this process supported by DFT calculations
dc.description.sponsorshipThe authors are grateful for the financial support given by the Xunta de Galicia (GRC2014/025 and METALBIO Network ED431D 2017/01)
dc.language.isoeng
dc.publisherMDPI
dc.rights© 2018 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/)
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/
dc.subjectArtificial photosynthesis
dc.subjectPhotocatalyst
dc.subjectWater splitting
dc.subjectManganese
dc.titleModeling the OEC with two new biomimetic models: preparations, structural characterization, and water photolysis studies of a Ba–Mn box type complex and a Mn4N6 Planar-diamond cluster
dc.typejournal article
dc.identifier.doi10.3390/catal8090382
dc.relation.publisherversionhttps://doi.org/10.3390/catal8090382
dc.type.hasVersionVoR
dc.identifier.essn2073-4344
dc.rights.accessRightsopen access
dc.contributor.affiliationUniversidade de Santiago de Compostela. Departamento de Farmacoloxía, Farmacia e Tecnoloxía Farmacéutica
dc.description.peerreviewedSI


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© 2018 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/)
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 © 2018 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/)





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