Synthetic, structural and spectroscopic studies on mono- and bi-arylimido functionalized hexamolybdates bearing the strong electron-withdrawing nitro group, (Bu4N)2[Mo6O18(NAr)] and (Bu4N)2[Mo6O17(NAr)2] (Aro-NO2–C6H4)

Two novel mono- and bi-functionalized organoimido derivatives of hexamolybdates bearing the strong electron-withdrawing nitro group, (Bu4N)2[Mo6O17( NAr)2] (1) and (Bu4N)2[Mo6O18( NAr)] (2) (Ar o-NO2–C6H4) have been synthesized for the first time via the reaction of hexamolybdate ions and 2 equivalent of aromatic amines with an excessive dehydrating agent N,N′-dicyclohexylcarbodiimide (DCC). By controlling the amount of DCC, such two derivatives can be selectively prepared in reasonable yields, which have been characterized with UV/vis, IR, 1H NMR, ESI-mass spectrometry and single-crystal X-ray diffraction techniques. The influences of [NAr] ligands and [NAr] incorporation number on properties and supermolecular assembly of such two derivatives have been systematically investigated.