Cyclophosphazene supramolecular assemblies:: N-H•••N and C-H•••N mediated supramolecular networks in the crystal structures of N3P3[N(Me)NH2]6 and spiro-N3P3[O2C12H8][N(Me)NH2]4

Cyclophosphazene hydrazides, N3P3[N(Me) NH2](6) 1 and spiro-N3P3[O2C12H8][N(Me)NH2](4) 2 have been found to organize themselves in supramolecular assemblies in the solid state. Thus, 1 forms a hexagonal close-packed sheet in which each molecule interacts with its six nearest neighbors. All the three ring nitrogen atoms act as proton acceptors while one N(Me) NH2 substituent on each phosphorus atom acts as a proton donor. Compound 2 forms a double chain in which two ring nitrogen atoms act as proton acceptors and one N( Me) NH2 substituent of each phosphorus atom acts as a proton donor. The supramolecular assembly of 1 is further elaborated by intermolecular C-H...N interactions.