Abstract
Two isostructural polymetallic complexes [Mn(μ3-O)2(CH3COO)4(L1)4]- and [Mn(μ3-O)2(CH3COO)4(L2)4]- have been synthesised by using two Schiff base ligands derived from 3,5-diamino-1,2,4-triazole, following two different preparative routes, either using the pre-formed ligand (for L1) or via a metal-mediated template synthesis (for L2). The {Mn} structure is unusual, being based on two corner-sharing perpendicular {Mn3} triangles forming a twisted bow-tie. The magnetic studies reveal antiferromagnetic coupling between Mn(iii) ions while electrochemical experiments are consistent with a quasi-reversible Mn(iii)↔Mn(iv) redox process at the central manganese ion.
Highlights
Manganese is an excellent candidate for the synthesis and study of new molecular magnetic materials[1,2,3,4,5] with a range of accessible oxidation states from Mn(II) to Mn(IV).[6,7,8]
Mn(III) ions are employed in the design of nanomagnets due to the characteristic magnetic anisotropy (D),[9,10,11,12] whereas Mn(II) ions are used in molecular magnetic refrigerants, considering the relatively large number of unpaired electrons and the typical isotropic octahedral environment.[13,14]
Schiff base ligands have been used in this type of strategy,[20,21,22] and in some cases, these ligands can provide additional redox aWestChem, School of Chemistry, University of Glasgow, University Avenue, Glasgow, G12 8QQ, UK
Summary
Manganese is an excellent candidate for the synthesis and study of new molecular magnetic materials[1,2,3,4,5] with a range of accessible oxidation states from Mn(II) to Mn(IV).[6,7,8] Mn(III) ions are employed in the design of nanomagnets due to the characteristic magnetic anisotropy (D),[9,10,11,12] whereas Mn(II) ions are used in molecular magnetic refrigerants, considering the relatively large number of unpaired electrons and the typical isotropic octahedral environment.[13,14] In addition, the stability of these multiple oxidation states provides an opportunity to explore the redox properties in polymetallic Mn complexes.[15,16,17] The synthetic routes to these complexes are mainly serendipitous self-assembly, which commonly uses flexible ligands, and/or rational design, which involves more rigid, polycompartmental ligands.[18,19,20] One of the advantages of the second approach is the degree of control in the assembly of the metal ions through the pre-design of the ligand. The iminic bonds make the ligand flexible enough to accommodate different coordination environments based on the type and/or valence of the metal ions
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