This thesis consists of the structures of two compounds as determined by single crystal x-ray diffraction. The first structure is that of a phosphazene - iodine complex: hexamethylcyclotriphosphazene - iodine (1:1 adduct) and the second structure is the redetermination of sodium formate. Crystals of hexamethylcyclotriphosphazene - iodine (1:1 adduct) are triclinic, a = 10.707(13), b = 8.873 (5), c = 8.871(6)Å, α = 96. 65 (6), β = 103.91 (12), ɤ = 97.81(12)°, Z = 2, space-group PI. The structure was determined with Mo-K« diffractometer data by Patterson and Fourier synthesis, and was refined by full-matrix least-squares calculations to R = 0.053 for 1934 observed reflexions. The iodine molecule is weakly bonded to a nitrogen atom on the phosphazene ring, N - I = 2.417(7), I - I = 2. 823 (1) Å, N - I - I = 177.8(2)°. The six-membered phosphazene ring is slightly, but significantly, ncn-planar, the conformation being that of a chair. The molecule has pseudo-m symmetry. Two distinct P-N bonds are present; the longer ones, mean P - N = 1.64 Å, involve the nitrogen that is weakly bonded to the iodine molecule, while the other four P-N bonds are equivalent, mean P - N = 1.598 Å. All the P - C bonds are equivalent, mean P - C = 1.789 Å. The mean endocyclic N - P - N and P - N - P angles are 114.7 and 124.0° respectively, while the mean exocyclic C - P - C angle is 104°. Crystals of sodium formate are mcnoclinic, a = 6.2590 (6), b = 6.7573 (16) , c = 6.716 (5) Å, β = 116.140(6)°, Z = 4, space-grcup C2/c. The structure was determined by direct methods, and was refined by electron density and full-matrix least-squares procedures to E = 0.022 for 250 reflexions. Sodium formate is planar and has C2V symmetry. Partial charges were refined on the formate ion. The partial charges found on each atom are as follows: 0 -0.23(1)e, C +0.16(3)e, H -0.49(10)e, and Sa +0.79(14)e. The sodium ion has six oxygen neighbours at an average distance of 2.45 Å and there are weak Na. ..0 interactions. There is a C - H...Na hydrogen bond which forms continuous rows of sodium formate ions. The C - 0 bond distance is 1.246(1)Å and the 0 - C - 0 angle is 126.3(2)°. / Science, Faculty of / Chemistry, Department of / Graduate