| Sumario: | The solvothermal reaction of NiCl2·6H2O with 1,3,5-tri(2-hydroxyethyl)-1,3,5-triazacyclohexane, LH3, and Ln(OAc)3·4H2O in the presence of salicylaldehyde in MeOH leads to the formation of the dodecanuclear isostructural species [NiII8Ln4(L')8(OAc)4(OH)8(H2O)4]·xH2O (Ln = Dy, x = 6 (1); Gd, x = 24 (2); Y, x = 10 (3); L' = the dianion of the Schiff-base resulting from the reaction of salicylaldehyde and ethanolamine). The metallic core of the clusters describes a ring of corner-sharing {Ni2Ln2} cubanes assembled on a central, planar rectangular {Ln4} unit. Magnetization studies conducted on complexes 1-3 demonstrate the presence of dominant ferromagnetic exchange at low temperatures, which is largely attributed to the Ni⋯Ni interactions. The significant magnetocaloric effect observed in the Gd analogue has been assessed through heat capacity and magnetization measurements.
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