A Series of Weakley-type Polyoxomolybdates: Synthesis, Characterization, and Magnetic Properties by a Combined Experimental and Theoretical Approach.

Using DCC as the dehydrating agent, a series of Weakley-type polyoxomolybdates [Bu4 N]3 {Ln[Mo5 O13 (OMe)4 (NO)]2 } (Ln = Tb, Dy, Ho, Er) were synthesized in a one-pot reaction and structurally characterized by elemental, IR, UV-vis analysis, PXRD, and single-crystal X-ray diffraction. Furthermore, the static and dynamic measurements were utilized to investigate their magnetic performances. Typically, slow relaxation of magnetization was observed for Dy analogues with an energy barrier for the reversal of the magnetization of 50 K, which is the highest barrier height observed on the polyoxomolybdates-based single-molecule magnets (SMMs). For a deep understanding of the appearance of the SMM behavior on Weakley-type polyoxomolybdates series, ab initio calculations on {Dy[Mo5 O13 (OMe)4 (NO)]2 }3- have been conducted.