Abstract

The synthesis, structural characterization and magnetic study of novel CoII/4f and CoII/YIII clusters are described. In particular, the initial employment of di-2-pyridyl ketone, (py)2CO, in mixed metal Co/4f chemistry, provided access to four triangular clusters, [CoII2MIII{(py)2C(OEt)(O)}4(NO3)(H2O)]2[M(NO3)5](ClO4)2 (M = Gd, 1; Dy, 2; Tb, 3; Y, 4), where (py)2C(OEt)(O)− is the monoanion of the hemiketal form of (py)2CO. Clusters 1–4 are the first reported Co/4f (1–3) and Co/Y (4) species bearing (py)2CO or its derivatives, despite the fact that over 200 metal clusters bearing this ligand have been reported so far. Variable-temperature, solid-state dc and ac magnetic susceptibility studies were carried out on 1–4 and revealed the presence of weak ferromagnetic exchange interactions between the metal ions (JCo-Co = +1.3 and +0.40 cm−1 in 1 and 4, respectively; JCo-Gd = +0.09 cm−1 in 1). The ac susceptibility studies on 2 revealed nonzero, weak out-of-phase (χ’’M) signals below ~5 K.

Highlights

  • IntroductionThe synthesis and characterization of new mixed-metal 3d/4f clusters has attracted immense interest over the last few decades, due to their fascinating structural features (high nuclearities, unprecedented metal topologies, aesthetically pleasing architectures, etc.), as well as due to their interesting magnetic properties [1,2,3]

  • The synthesis and characterization of new mixed-metal 3d/4f clusters has attracted immense interest over the last few decades, due to their fascinating structural features, as well as due to their interesting magnetic properties [1,2,3]

  • 4f ions often favor the formation of heterometallic compounds that possess exceptionally high nuclearities, with representative examples being clusters of Ni64Gd96 [4], Ni76La60 [5], Ni54Gd54 [6], Cu36Dy24 [7], Ni10Gd42 [8], Ni30La20 [9,10], etc

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Summary

Introduction

The synthesis and characterization of new mixed-metal 3d/4f clusters has attracted immense interest over the last few decades, due to their fascinating structural features (high nuclearities, unprecedented metal topologies, aesthetically pleasing architectures, etc.), as well as due to their interesting magnetic properties [1,2,3]. 4f ions often favor the formation of heterometallic compounds that possess exceptionally high nuclearities, with representative examples being clusters of Ni64Gd96 [4], Ni76La60 [5], Ni54Gd54 [6], Cu36Dy24 [7], Ni10Gd42 [8], Ni30La20 [9,10], etc. This intriguing ability of 4f ions possibly stems from their strong oxophilicity, which, in combination with their high coordination numbers, results in the formation of hydroxo/oxo species that readily promote the aggregation process. Over 200 homo- and heterometallic compoundss haavvee nnooww beeenn reeppoorrtteedd,, ccoonnttaaiinniinngg ((ppyy))22CO and its derivatives, the absence of such Co//44ff cclluusstteerrss iiss nnoottiicceeaabbllee ccoonnssiiddeerriinnggtthheeggrreeaattddeevveellooppmmeennttoofftthhiissrreesseeaarrcchhfifeieldld

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