Synthesis, Spectroscopic Study, X-Ray Crystallography Investigation and Hirshfeld Surface Analysis of Three New Phosphorous-Nitrogen Compounds

New phosphorous-nitrogen compounds 2,3-F2—C6H3C(O)NHP(O)[N(CH3)CH2C6H5]2 (I), C6H5OP(O)[NHCH(CH3)2]2 (II) and (CH3O)2P(S)[NHC6H4NH]P(S)(OCH3)2 (III) were synthesized and characterized by 19F NMR for (I) and 1H, 13C, 31P NMR and IR and mass spectroscopy and single crystal X-ray determination for all three compounds. In the 31P NMR spectra, the 31P{1H} signals of (I), (II) and (III) are revealed at 12.95, 10.49 and 69.55 ppm, respectively. The chemical shits observed are within the expected values for analogous phsophoramide and thiophosphoramide compounds.1,2 In the crystal structure of (I), centrosymmetric dimers are built from pairs of N—H...O═P hydrogen bonds. In the structure (II), the molecules are aggregated in a one-dimensional arrangement via N—H...O═P hydrogen bonds along the b axis. In the structure (III), the two-dimensional array is generated from the N—H...O hydrogen bonds along the ab plane. In structure (II), the oxygen atom of P═O group is a better H-atom acceptor than the oxygen atom of the C6H5O group, as the latter oxygen atom doesn’t take part in hydrogen bonding interaction. The better hydrogen-bond acceptor capability