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Two isostructural lanthanide amino-phosphonate complexes [Ln10(μ3-OH)3(µ-OH)(CO3)2(O2CtBu)15(O3PC6H10NH2)3(O3PC6H10NH3)2(H2O)2][Et2NH2] (Ln = Gd(III), 1 and Tb(III), 2) have been obtained through reflux reactions of lanthanide pivalates with, a functionalized phosphonate, (1-amino-1-cyclohexyl)phosphonic acid and diethylamine (Et2NH) in acetonitrile (MeCN) at 90 °C. Both compounds have been characterized with elemental analysis, single-crystal X-ray diffraction methods, and magnetic measurements. The molecular structure of compounds 1 and 2 reveal two highly unsymmetrical complexes comprising ten lanthanide metal centers, where the lanthanide metal ion centers in the cages are linked through pivalate units and further interconnected by CPO3 tetrahedra to build the crystal structure. The magnetic behavior of 1 and 2 was investigated between ambient temperature and ca. 2 K, the magnetic measurements for compound 1 suggests antiferromagnetic interactions between the Gd(III) metal ion centers at low temperatures. The large number of isotropic Gd(III) ions comprising 1 makes it a candidate for magnetocaloric applications, thus the magnetocaloric properties of this molecular cage were investigated indirectly through isothermal magnetisation curves. The magnetic entropy change was found to be 34.5 J kg−1K−1, making 1 a plausible candidate in magnetic cooling applications.

Synthesis, Crystal Structures, and Magnetic Properties of Lanthanide (III) Amino-Phosphonate Complexes