Hydrothermal synthesis, structural characterisation and magnetic behaviour of hybrid complexes of N-(phosphonomethyl)iminodiacetate

Two new compounds containing multidentate chelating organic residues of N-(phophonomethyl)iminodiacetic acid (H4pmida), [M(pyr)(H2O)4][M2(Hpmida)2(pyr)(H2O)2]·2(H2O) (where pyr=pyrazine and M=Co2+ or Ni2+ for I and II, respectively) have been synthesised and structurally characterised by single-crystal and powder X-ray diffraction, elemental analysis, infrared spectroscopy, thermal analysis and solid-state 31P MAS NMR. The compounds contain discrete binuclear anionic [M2(Hpmida)2(pyr)(H2O)2]2− units in which one pyrazine ligand bridges two M2+ cations which are completely trapped inside three five-membered chelate rings formed by the Hpmida3− ligands. These moieties close pack in the ac plane via a series of strong and highly directional O-H⋯O hydrogen bonds leading to the formation of anionic [Co2(Hpmida)2(pyr)(H2O)2]n2n− layers. One-dimensional cationic [M(pyr)(H2O)4]n2n+ coordination polymers are placed in-between and strongly hydrogen-bonded to these layers. The magnetic properties of these two materials are also reported.