Hendecanuclear [Cu6Gd5] magnetic cooler with high molecular symmetry of D3h

[Display omitted] A new family of isostructural 3d-4f polymetallic complexes, formulated as [Cu6Ln5(μ3−OH)9 (C4H8O2N)6(C5H4ON)6(H2O)9]·(ClO4)6·(H2O)22 (Ln = Pr, 1; Nd, 2; Sm, 3; Eu, 4; Gd, 5), was successfully isolated through the simple hydrolysis reaction of 2-aminoisobutyric acid, 2-hydroxypyridine, Cu(CH3COO)2·H2O, and Ln(ClO4)3·6H2O. Notably, the [Cu6Ln5] clusters with high molecular symmetry of D3h are rare examples of 2-aminoisobutyric acid-based 3d-4f clusters. The successful theoretical modeling of 5 yielded that the Gd-Gd exchange is of order 0.2 K, whereas the Gd-Cu exchange is an order of magnitude larger. Magnetization data collected for complex 5 yield a magnetic entropy change (−ΔSm) of 19.6 J kg−1 K−1 at 3 K and 7 T, which may be attributed to the weak magnetic interactions between the component metal ions.