Two new compounds containing multidentate chelating organic residues of
N-(phophonomethyl)iminodiacetic acid (H
4pmida), [M(pyr)(H
2O)
4][M
2(Hpmida)
2(pyr)(H
2O)
2]·2(H
2O) (where pyr=pyrazine and M=Co
2+ or Ni
2+ 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 [M
2(Hpmida)
2(pyr)(H
2O)
2]
2− units in which one pyrazine ligand bridges two M
2+ cations which are completely trapped inside three five-membered chelate rings formed by the Hpmida
3− ligands. These moieties close pack in the
ac plane via a series of strong and highly directional O–H
![cdots, three dots, centered](http://www.sciencedirect.com/scidirimg/entities/22ef.gif)
O hydrogen bonds leading to the formation of anionic
![Click to view the MathML source](http://www.sciencedirect.com/cache/MiamiImageURL/B6TGS-4GV98D3-4-2/0?wchp=dGLbVtb-zSkzV)
layers. One-dimensional cationic
![Click to view the MathML source](http://www.sciencedirect.com/cache/MiamiImageURL/B6TGS-4GV98D3-4-3/0?wchp=dGLbVtb-zSkzV)
coordination polymers are placed in-between and strongly hydrogen-bonded to these layers. The magnetic properties of these two materials are also reported.