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Triple stranded Ni-metallacyclic complexes Na 2.5 [Ni 2 (bpcb) 3 ]·0.5OH·18.5H 2 O (1) and Na 2 [Ni 2 (bpzcb) 3 ]·16H 2 O (2), and double stranded Cu-metallacyclic complexes [Cu 2 (bpcb) 2 (H 2 O) 2 ]·8H 2 O (3) and [Cu 2 (bpzcb) 2 (H 2 O) 2 ]·4H 2 O (4) have been assembled from the tailored bisbidentate bridging ligands, 1,3-bis(pyrimidine-2-carboxamide)benzene (H 2 bpcb) and 1,3-bis(pyrazine-2-carboxamide)benzene (H 2 bpzcb), and the corresponding nitrate salts of the metal ions. Following the "complex as ligand" strategy, 1 can be assembled with either Ni 2+ , Co 2+ ions or the [Mn(acen)Cl] complex to afford unique, neutral, bent trinuclear molecules [M II Ni(bpcb) 3 ]·xH 2 O (5 and 6) and the 2D honeycomb-like complex (PPh 4 ){[Ni 2 (bpcb) 3 ] 2 [Mn(acen)] 3 } (7), respectively. In these cases, the Ni 2 units are linked to the corresponding metal ions through amidate oxygen atoms and the outward nitrogen atom of one of the pyrimidine rings of the bcpb ligand. The assembly of 2 with Ln 3+ ions (Ln 3+ = Tb, Gd) leads to one dimensional complexes of formula [{[Ni 2 (bpzcb) 3 ]Tb(H 2 O) 5 }(CF 3 SO 3 )·THF·5H 2 O] n (8) and [{[Ni 2 (bpzcb) 3 ]Ln(H 2 O) 4 (NO 3 )}·2THF·nH 2 O] n (9 and 10) (Ln 3+ = Gd and Tb), where the dinuclear Ni 2 units are joined to two Ln 3+ ions exclusively through amidate oxygen atoms of two different ligands. The analyses of the magnetic data indicate that 1-4 exhibit intradinuclear ferromagnetic interactions between the metal ions through a spin polarisation mechanism, as supported by DFT calculations. Trinuclear complexes 5 and 6 show predominant antiferromagnetic coupling, which is a result of an antiferromagnetic interaction between one of the Ni 2+ ions of the Ni 2 unit and the M 2+ ion through the pyrimidine bridging fragment that is stronger than the polarised ferromagnetic interaction between the Ni 2+ ions through the bpcb ligand in the dinuclear [Ni 2 (bpcb) 3 ] 2- moiety. Complex 7 shows a dominant antiferromagnetic interaction between the Ni 2+ and Mn 2+ , whereas the Ni 2 Ln (Ln 3+ = Gd, Tb) chain complexes present ferromagnetic interactions inside the Ni 2 mesocate unit as well as between the Ni 2+ ions of the Ni 2 unit and the Ln 3+ ions. The magnetic exchange interactions in these new materials have been experimentally analysed and supported by theoretical DFT studies.

dalton transactions

Synthetic ability of dinuclear mesocates containing 1,3-bis(diazinecarboxamide)benzene bridging ligands to form complexes of increased nuclearity. Crystal structures, magnetic properties and theoretical studies