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Anion-Directed Metallocages: A Study on the Tendency of Anion Templation.

Self-assembly of Cu(NO3 )2 ⋅3 H2 O and di(3-pyridylmethyl)amine (dpma) with addition of different acids (HNO3 , HOAc, HCl, HClO4 , HOTf, HPF6 , HBF4 , and H2 SO4 ) afforded a family of anion-templated tetragonal metallocages with a cationic prismatic structure of [(Gn- )⊂{Cu2 (Hdpma)4 }](8-n)+ (Gn- =NO3 - , PF6 - , SiF6 2- ) with different ligating anions/solvents (NO3 - , Cl- , ClO4 - , OTf- , H2 O) outside the cage. Systematic competitive experiments have rationalized the tendency of anion templation towards the formation of metallocages [(Gn- )⊂{Cu2 (Hdpma)4 }](8-n)+ as occurring in the order SiF6 2- ≈PF6 - >NO3 - >SO4 2- ≈ClO4 - ≈BF4 - . This sequence is mostly elucidated by shape control over size selectivity and electrostatic attraction between the cationic {Cu2 (Hdpma)4 }8+ host and the anionic guests. In addition, these results have also roughly ranked the anion coordination ability in the order Cl- , ClO4 - , OTf- >NO3 - >BF4 - , CH3 SO4 - . Magnetic studies of metallocages 1 t and 2-4 suggest that the fitted magnetic interaction, being weakly magnetically coupled overall, is interpreted as a result of the combination of intracage ferromagnetic coupling integrals and intercage antiferromagnetic exchange; both contributions are very weak and comparable in strength.

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