Abstract
The syntheses and structures of a family of five new Ln/3d cluster containing polyoxometalates (POMs) [{(GeW9O34)2LnIII3(CO3)(OH2)3}6{3MII2LnIII3(μ3‐OH)6(OH2)6}4]50− {Ln30M8}, where Ln = Gd or Y, and M = Zn, Mn, Co, are presented. This structural motif of a giant tetrahedron contains {LnIII3} and {MII2LnIII3}‐cluster units which are well‐isolated within the diamagnetic polyoxotungstate system. The magnetic properties of {Gd30Mn8}, {Y30Mn8} and {Gd30Zn8} can be successfully modeled using a Heisenberg approach. Investigation of their magnetocaloric effect (MCE) reveals that this can be tuned through variation of the 3d metal ion. This is the first such systematic study on heterometallic 3d‐4f‐ POM clusters. The {Gd30Zn8} analogue illustrates a promising way forward to magnetic cooling at sub‐Kelvin temperatures.
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