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dc.contributor.author | Rouco Méndez, Lara |
dc.contributor.author | Fernández García, María Isabel |
dc.contributor.author | Pedrido Castiñeiras, Rosa María |
dc.contributor.author | Botana López, Luis Miguel |
dc.contributor.author | Esteban Gómez, David |
dc.contributor.author | Platas Iglesias, Carlos |
dc.contributor.author | Maneiro Maneiro, Marcelino |
dc.date.accessioned | 2020-05-29T17:54:56Z |
dc.date.available | 2020-05-29T17:54:56Z |
dc.date.issued | 2018 |
dc.identifier.citation | Rouco, 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.uri | http://hdl.handle.net/10347/22700 |
dc.description.abstract | The 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.sponsorship | The authors are grateful for the financial support given by the Xunta de Galicia (GRC2014/025 and METALBIO Network ED431D 2017/01) |
dc.language.iso | eng |
dc.publisher | MDPI |
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.uri | http://creativecommons.org/licenses/by/4.0/ |
dc.subject | Artificial photosynthesis |
dc.subject | Photocatalyst |
dc.subject | Water splitting |
dc.subject | Manganese |
dc.title | 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 |
dc.type | journal article |
dc.identifier.doi | 10.3390/catal8090382 |
dc.relation.publisherversion | https://doi.org/10.3390/catal8090382 |
dc.type.hasVersion | VoR |
dc.identifier.essn | 2073-4344 |
dc.rights.accessRights | open access |
dc.contributor.affiliation | Universidade de Santiago de Compostela. Departamento de Farmacoloxía, Farmacia e Tecnoloxía Farmacéutica |
dc.description.peerreviewed | SI |
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