Several new bulky salen-type Schiff base ligands and their complexes with first-row transition metals Co, Cu, Fe, Mn and Ni have been synthesized and characterized. The ligands contain tert-butyl and methyl(triphenylphosphonium chloride) substituents in aromatic rings providing flexible solubility properties. Crystal structures of some of the complexes were determined.
Two bimetallic assemblies K[Cu(cyclam)][Fe(CN) 6 ]ؒ4H 2 O 1 and [Cu(L)][Cu(L 1 )][Fe(CN) 6 ]ؒ6.5H 2 O 2 (cyclam = 1,4,8,11-tetraazacyclotetradecane; L = N,NЈ-bis(2-pyridylmethylene)-1,3-propanediamine and L 1 = N-2-pyridylmethylene-1,3-propanediamine) have been prepared from the reaction of [Fe(CN) 6 ] 3Ϫ and the precursors [Cu(cyclam)] 2ϩ and [Cu(L)] 2ϩ , respectively, and their structure and magnetic properties studied. The structure of 1 consists of polymeric zigzag chains of alternating [Fe(CN) 6 ] 3Ϫ and [Cu(cyclam)] 2ϩ units, K ϩ cations and crystal water molecules. In the crystals the chains are linked by CN-K-NC interactions, to form a two-dimensional layer structure. Magnetic measurements show a weak ferromagnetic intrachain interaction based on the strict orthogonality of the magnetic orbitals of the Fe III and Cu II . In the structure of 2 each [Cu(L 1 )] 2ϩ unit is bonded to centrosymmetric [Fe(CN) 6 ] 4Ϫ and [Cu(L)Fe(CN) 6 Cu(L)] units through two cis bridging cyanide ligands. Owing to the symmetry, a unique one-dimensional zigzag chain structure is formed through trans bridging cyanide ligands of the two crystallographically non-equivalent [Fe(CN) 6 ] 4Ϫ groups. In the course of the reaction the [Fe(CN) 6 ] 3Ϫ ion undergoes a reduction to [Fe(CN) 6 ] 4Ϫ whereas the [Cu(L)] 2ϩ ion partly hydrolyses to [Cu(L 1 )] 2ϩ . Compound 2 is essentially paramagnetic within the chain.
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