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Constructing Closed and Open {Mn8} Clusters
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DOI：10.1021/acs.cgd.2c00489.png)
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Abstract
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Use of the 1,3,5-tri(2-hydroxyethyl)-1,3,5-triazacyclohexane ligand, LH3, in manganese chemistry affords access to two structurally related {Mn-8} clusters: a closed {(Mn6Mn2II)-Mn-III} puckered square wheel of formula [Mn8L2(LH)O-3(OH)(2)(MeO)(2)Br(imH)(H2O)(3)] (Br) 3 (1; imH = imidazole ) and an open {Mn-8(III)} rod of formula [(Mn8L2O4)-L-III(aibH)(2)(aib)(2)(MeO)(6)(MeOH)(2)](NO3)(2) (2, aibH = 2-amino-isobutyric acid). In each case the triaza ligands, L/LH, direct the formation of {Mn-3} triangles with their N atoms preferentially bonding to the Jahn-Teller axes of the Mn-III ions. Subsequent self-assembly is dependent on the anion of the Mn salt and the identity of the organic coligand employed-the terminally bonded imidazole and the chelating/bridging amino acid. The {Mn-3} triangles fold up on themselves in 1, forming a wheel. However, the syn, syn-bridging carboxylates in 2 prevent this from happening, instead directing the formation of a linear rod. Magnetic susceptibility and magnetization measurements reveal competing ferro-and antiferromagnetic interactions in both complexes, the exchange being somewhat weaker in 1 due to the presence of Mn-II ions.
Keywords:
MANGANESE-CALCIUM CLUSTERS
OXYGEN-EVOLVING COMPLEX
MAGNETIC EXCHANGE
FAMILY
DIMERS
WHEEL
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