Dy4, Dy5, and Ho2 Complexes of an N3O2 Aminophenol Donor: A Dy5-µ3-Peroxide Single Molecule Magnet
The reactivity of the new flexible potentially pentadentate N3O2 aminophenol ligand H4Lr (2,2′-((pyridine-2,6-diylbis(methylene))bis(azanediyl))diphenol) towards different dysprosium salts and holmium(III) nitrate was investigated. Accordingly, this reactivity seems to greatly depend on the metal io...
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Published in | International journal of molecular sciences Vol. 24; no. 10; p. 9061 |
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Abstract | The reactivity of the new flexible potentially pentadentate N3O2 aminophenol ligand H4Lr (2,2′-((pyridine-2,6-diylbis(methylene))bis(azanediyl))diphenol) towards different dysprosium salts and holmium(III) nitrate was investigated. Accordingly, this reactivity seems to greatly depend on the metal ion and salt employed. In this way, the reaction of H4Lr with dysprosium(III) chloride in air leads to the oxo-bridged tetranuclear complex [Dy4(H2Lr)3(Cl)4(μ3-O)(EtOH)2(H2O)2]·2EtOH·H2O (1·2EtOH·H2O), while the same reaction just changing the chloride salt by the nitrate one renders the peroxo-bridged pentanuclear compound [Dy5(H2Lr)2(H2.5Lr)2(NO3)4(µ3-O2)2]·2H2O (2·2H2O), where both peroxo ligands seem to come from the fixation and reduction of atmospheric oxygen. However, if holmium(III) nitrate is used instead of dysprosium(III) nitrate, no evidence of a peroxide ligand is observed, and the dinuclear complex {[Ho2(H2Lr)(H3Lr)(NO3)2(H2O)2](NO3)} 2.5H2O (3·2.5H2O) is isolated. The three complexes were unequivocally characterized by X-ray diffraction techniques, and their magnetic properties were analyzed. Thus, while the Dy4 and Ho2 complexes do not show magnet-like behavior even in the presence of an external magnetic field, 2·2H2O is a single molecule magnet, with an Ueff barrier of 61.2 K (43.2 cm−1). This is the first homonuclear lanthanoid peroxide SMM, which also shows the highest barrier among the reported 4f/3d peroxide zero field SMMs to date. |
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AbstractList | The reactivity of the new flexible potentially pentadentate N3O2 aminophenol ligand H4Lr (2,2′-((pyridine-2,6-diylbis(methylene))bis(azanediyl))diphenol) towards different dysprosium salts and holmium(III) nitrate was investigated. Accordingly, this reactivity seems to greatly depend on the metal ion and salt employed. In this way, the reaction of H4Lr with dysprosium(III) chloride in air leads to the oxo-bridged tetranuclear complex [Dy4(H2Lr)3(Cl)4(μ3-O)(EtOH)2(H2O)2]·2EtOH·H2O (1·2EtOH·H2O), while the same reaction just changing the chloride salt by the nitrate one renders the peroxo-bridged pentanuclear compound [Dy5(H2Lr)2(H2.5Lr)2(NO3)4(µ3-O2)2]·2H2O (2·2H2O), where both peroxo ligands seem to come from the fixation and reduction of atmospheric oxygen. However, if holmium(III) nitrate is used instead of dysprosium(III) nitrate, no evidence of a peroxide ligand is observed, and the dinuclear complex {[Ho2(H2Lr)(H3Lr)(NO3)2(H2O)2](NO3)} 2.5H2O (3·2.5H2O) is isolated. The three complexes were unequivocally characterized by X-ray diffraction techniques, and their magnetic properties were analyzed. Thus, while the Dy4 and Ho2 complexes do not show magnet-like behavior even in the presence of an external magnetic field, 2·2H2O is a single molecule magnet, with an Ueff barrier of 61.2 K (43.2 cm−1). This is the first homonuclear lanthanoid peroxide SMM, which also shows the highest barrier among the reported 4f/3d peroxide zero field SMMs to date. The reactivity of the new flexible potentially pentadentate N 3 O 2 aminophenol ligand H 4 L r (2,2′-((pyridine-2,6-diylbis(methylene))bis(azanediyl))diphenol) towards different dysprosium salts and holmium(III) nitrate was investigated. Accordingly, this reactivity seems to greatly depend on the metal ion and salt employed. In this way, the reaction of H 4 L r with dysprosium(III) chloride in air leads to the oxo-bridged tetranuclear complex [Dy 4 (H 2 L r ) 3 (Cl) 4 (μ 3 -O)(EtOH) 2 (H 2 O) 2 ]·2EtOH·H 2 O ( 1 ·2EtOH·H 2 O), while the same reaction just changing the chloride salt by the nitrate one renders the peroxo-bridged pentanuclear compound [Dy 5 (H 2 L r ) 2 (H 2.5 L r ) 2 (NO 3 ) 4 (µ 3 -O 2 ) 2 ]·2H 2 O ( 2 ·2H 2 O), where both peroxo ligands seem to come from the fixation and reduction of atmospheric oxygen. However, if holmium(III) nitrate is used instead of dysprosium(III) nitrate, no evidence of a peroxide ligand is observed, and the dinuclear complex {[Ho 2 (H 2 L r )(H 3 L r )(NO 3 ) 2 (H 2 O) 2 ](NO 3 )} 2.5H 2 O ( 3 ·2.5H 2 O) is isolated. The three complexes were unequivocally characterized by X-ray diffraction techniques, and their magnetic properties were analyzed. Thus, while the Dy 4 and Ho 2 complexes do not show magnet-like behavior even in the presence of an external magnetic field, 2 ·2H 2 O is a single molecule magnet, with an U eff barrier of 61.2 K (43.2 cm −1 ). This is the first homonuclear lanthanoid peroxide SMM, which also shows the highest barrier among the reported 4f/3d peroxide zero field SMMs to date. |
Author | García-Deibe, Ana M Oreiro-Martínez, Paula Fondo, Matilde Corredoira-Vázquez, Julio Sanmartín-Matalobos, Jesús Nieto-Pastoriza, Daniel |
AuthorAffiliation | 2 Phantom-g, CICECO—Aveiro Institute of Materials, Department of Physics, University of Aveiro, 3810-193 Aveiro, Portugal 1 Departamento de Química Inorgánica, Facultade de Química, Universidade de Santiago de Compostela, 15782 Santiago de Compostela, Spain 3 Institute of Materials (iMATUS), Universidade de Santiago de Compostela, 15782 Santiago de Compostela, Spain |
AuthorAffiliation_xml | – name: 2 Phantom-g, CICECO—Aveiro Institute of Materials, Department of Physics, University of Aveiro, 3810-193 Aveiro, Portugal – name: 3 Institute of Materials (iMATUS), Universidade de Santiago de Compostela, 15782 Santiago de Compostela, Spain – name: 1 Departamento de Química Inorgánica, Facultade de Química, Universidade de Santiago de Compostela, 15782 Santiago de Compostela, Spain |
Author_xml | – sequence: 1 givenname: Julio orcidid: 0000-0002-7806-179X surname: Corredoira-Vázquez fullname: Corredoira-Vázquez, Julio – sequence: 2 givenname: Paula surname: Oreiro-Martínez fullname: Oreiro-Martínez, Paula – sequence: 3 givenname: Daniel surname: Nieto-Pastoriza fullname: Nieto-Pastoriza, Daniel – sequence: 4 givenname: Ana M. orcidid: 0000-0001-9127-0740 surname: García-Deibe fullname: García-Deibe, Ana M. – sequence: 5 givenname: Jesús orcidid: 0000-0002-9971-4657 surname: Sanmartín-Matalobos fullname: Sanmartín-Matalobos, Jesús – sequence: 6 givenname: Matilde orcidid: 0000-0002-7535-946X surname: Fondo fullname: Fondo, Matilde |
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SubjectTerms | Aminophenol Chloride Chlorides Dysprosium Ethanol Holmium Information storage lanthanoid Ligands Magnetic properties Metal ions N3O2 aminophenol Nitrates Peroxide peroxide ligand Single crystals SMM Solvents X-ray diffraction |
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Title | Dy4, Dy5, and Ho2 Complexes of an N3O2 Aminophenol Donor: A Dy5-µ3-Peroxide Single Molecule Magnet |
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