Tetranuclear and dinuclear phenoxido bridged copper complexes based on unsymmetrical thiosemicarbazone ligands
| Autor: | A.-T. Mansour, Marius Réglier, Rolf David, Christian Philouze, Hélène Jamet, Catherine Belle, Franc Meyer, Aurore Thibon-Pourret, S. Caldarelli, Ariane Jalila Simaan, Amélie Kochem, Serhiy Demeshko, James A. Isaac, Mehdi Yemloul |
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| Přispěvatelé: | Département de Chimie Moléculaire - Chimie Inorganique Redox (DCM - CIRE ), Département de Chimie Moléculaire (DCM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Georg-August-University = Georg-August-Universität Göttingen, Institut des Sciences Moléculaires de Marseille (ISM2), Aix Marseille Université (AMU)-École Centrale de Marseille (ECM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de recherches sur la catalyse (IRC), Centre National de la Recherche Scientifique (CNRS), Département de Chimie Moléculaire - Chimie Inorganique Redox Biomimétique (DCM - CIRE ), Georg-August-University [Göttingen] |
| Rok vydání: | 2018 |
| Předmět: |
010405 organic chemistry
Chemistry Ligand Substituent chemistry.chemical_element Nuclear magnetic resonance spectroscopy 010402 general chemistry Electrochemistry 01 natural sciences Copper 0104 chemical sciences Inorganic Chemistry chemistry.chemical_compound Crystallography Magic angle spinning [CHIM]Chemical Sciences [CHIM.COOR]Chemical Sciences/Coordination chemistry Acetonitrile Semicarbazone ComputingMilieux_MISCELLANEOUS |
| Zdroj: | Dalton Transactions Dalton Transactions, 2018, 47 (29), pp.9665-9676. ⟨10.1039/C8DT02452A⟩ Dalton Transactions, Royal Society of Chemistry, 2018, 47 (29), pp.9665-9676. ⟨10.1039/C8DT02452A⟩ |
| ISSN: | 1477-9234 1477-9226 |
| DOI: | 10.1039/c8dt02452a |
| Popis: | We report on the synthesis of new dinucleating phenol-based "end-off" compartmental ligands HLMeH and HLMe2 bearing two different binding sites, one bis(2-methylpyridyl)aminomethyl (BPA) and one thiosemicarbazone (TSC) site, and their corresponding copper(ii) complexes 1t and 2d. With the ligand HLMeH, a tetranuclear entity (1t) has been isolated in the solid state, whereas with HLMe2, which differs from HLMeH by a methyl substituent on the N-terminal amino group of the TSC arm, a dinuclear form (2d) is obtained. X-ray crystallography analysis shows that the nuclearity di vs. tetra is modulated by interactions between copper atoms and hydroxido bridges along with the sulphur atoms of TSC arms. From a magnetic point of view, 1t can be considered as an association of two dinuclear forms leading for both complexes to overall antiferromagnetic coupling. Analysis in acetonitrile solution of structure-property relationships has been carried out by comparing their UV/Vis, electrochemistry, ESI-MS, and NMR (variable temperature and DOSY = diffusion ordered spectroscopy) properties with trends from computational calculations (DFT). HRMAS-DOSY (High Resolution Magic Angle Spinning) NMR spectroscopy has been performed to evaluate the presence of different species in solution at room temperature. |
| Databáze: | OpenAIRE |
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