In the cone conformation calix[4]arenes possess lower-rim polyphenolic pockets that are ideal for the complexation of various transition-metal centres. Reaction of these molecules with manganese salts in the presence of an appropriate base (and in some cases co-ligand) results in the formation of a family of calixarene-supported [Mn(III)(2)Mn(II)(2)] clusters that behave as single-molecule magnets (SMMs). Variation in the alkyl groups present at the upper-rim of the cone allows for the expression of a degree of control over the self-assembly of these SMM building blocks, whilst retaining the general magnetic properties. The presence of various different ligands around the periphery of the magnetic core has some effect over the extended self-assembly of these SMMs.
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Tetra-, tetradeca- and octadecametallic clusters of Mn.
Dalton Trans
May 2023
EaStCHEM School of Chemistry, The University of Edinburgh, David Brewster Road, Edinburgh, EH9 3FJ, Scotland, UK.
Reaction of equimolar amounts of MnBr·4HO and HL ((3,5-dimethyl-1-pyrazol-1-yl)methanol) in a basic MeCN solution leads to the formation of [MnII4(L)Br(HO)] (1), whose metallic skeleton is a [MnII4] tetrahedron and cluster core a [MnII4(μ-O)] cubane. Replacing MnBr·4HO with Mn(OCMe)·4HO affords [MnIII2MnII12O(L)(OAc)] (2) which is best described as a series of edge-sharing [Mn] tetrahedra that have self-assembled into a linear array in which each [Mn] pair is 'twisted' with respect to its neighbours in a corkscrew-like manner. Employment of the triangle [MnIII3O(OAc)(py)](ClO) as a reactant instead of a Mn salt results in the formation of [MnIII14MnII4O(L)(HL)(OAc)(HO)] (3) whose core is comprised of three vertex-sharing [MnIII4] butterflies flanked on either side by one [MnIII4] cubane and one [MnIII2MnII2] tetrahedron.
View Article and Find Full Text PDFOxidation state variation in bis-calix[4]arene supported decametallic Mn clusters.
Dalton Trans
December 2021
EastCHEM School of Chemistry, The University of Edinburgh, David Brewster Road, Edinburgh, Scotland, EH9 3FJ, UK.
The reaction of MnCl·4HO, HL (2,2'-bis--Bu-calix[4]arene) and NEt in a dmf/MeOH solvent mixture results in the formation of a mixed valent decametallic cluster of formula [MnII6MnIII4(L)(μ-OH)(μ-OH)(MeOH)(dmf)(MeCN)]·MeCN (3). Complex 3 crystallises in the monoclinic space group 2/ with the asymmetric unit comprising half of the compound. Structure solution reveals that the bis-calix[4]arene ligands are arranged such that one TBC[4] moiety in each has undergone inversion in order to accommodate a [MnIII4MnII6] metallic skeleton that describes three vertex-sharing [MnIII2MnII2] butterflies.
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Chemistry
June 2011
EastCHEM School of Chemistry, The University of Edinburgh, West Mains Road, Edinburgh, EH9 3 JJ, UK.
In the cone conformation calix[4]arenes possess lower-rim polyphenolic pockets that are ideal for the complexation of various transition-metal centres. Reaction of these molecules with manganese salts in the presence of an appropriate base (and in some cases co-ligand) results in the formation of a family of calixarene-supported [Mn(III)(2)Mn(II)(2)] clusters that behave as single-molecule magnets (SMMs). Variation in the alkyl groups present at the upper-rim of the cone allows for the expression of a degree of control over the self-assembly of these SMM building blocks, whilst retaining the general magnetic properties.
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Chem Commun (Camb)
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School of Chemistry, The University of Edinburgh, West Mains Road, Edinburgh, Scotland EH9 3JJ, UK.
Phosphinate ligands allow for the transformation of a calix[4]arene supported [Mn(III)(2)Mn(II)(2)] tetramer cluster motif into an unusual [Mn(III)Mn(II)](2) dimer of dimers; the clusters self-assemble in the crystal to form bi-layer arrays reminiscent of the typical packing of calixarene solvates.
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