STUDY OF NEW MOLECULAR AND CRYSTAL STRUCTURES OF 4,4,10,10-TETRAMETHYL-1,3,7,9-TETRAAZOSPIRO[5.5]UNDECANE-2,8-DIONE AND ITS SALTS: MONOCHLORIDE, MONONITRATE, AND TETRAIODOTELLURATE

摘要

This is the first work to synthesize 4,4,10,10-tetramethyl-1,3,7,9-tetraazospiro[5.5]undecane-2,8-dione monohydrate, monochloride, mononitrate, and teteraiodotellurate: C_(11)H_(20)N_4O_2?H_2O (I), C_(11)H_(21)N_4O_2~+ ?Cl~– (II), C_(11)H_(21)N_4O_2~+ ? NO_3~? (III), and 2(C_(11)H_(21)N_4O_2~+)?TeI_4~(2?)?C_3H_6O (IV) and determine their structures. Crystals of I are monoclinic: space group P2_1/c, at 298 K a = 5.7118(7) ?, b = 17.842(2) ?, and c = 13.5905(16) ?; β = 91.621(11)°; V = 1384.5(3) ?~3; d_x = 1.239 g/cm~3, Z = 4. Crystals of II are tetragonal: space group P4_3, at 298 K a = 6.4134(3) ? and c = 34.292(2) ?; V = 1410.47(14) ?~3; d_x = 1.303 g/cm~3; Z = 4. Crystals of III are triclinic: space group P1, at 298 K a = 8.7614(14) ?, b = 9.3904(18) ?, and c = 10.028(2) ?; α = 63.27(2)°, β = 78.591(16)°, and γ = 84.308(15)°; V = 722.3(2) ?~3; d_x = 1.40 g/cm~3; Z = 2. Crystals of IV are triclinic: space group P1, at 100 K a = 10.4630(4) ?, b = 11.9372(6) ?, and c = 16.4118(5) ?; α = 72.058(3)°, β = 76.406(3)°, and γ = 87.029(3)°; V = 1895.04(12) ?~3; d_x = 2.06 g/cm~3; Z = 2. The synthesis of s and p metals with spirocarbone in acetone medium is found to be impossible due to the protonation by the oxygen atom of the carbonyl group. The main crystalline product of the complexation reaction is a monosalt. Evidence is provided that the recrystallization and drying of the synthesized spirocarbone preparation yields monohydrate (I); its purity and monophasity is confirmed by a Rietveld refinement of the powder X-ray pattern. The lattice parameters at room temperature are: a = 5.6885(12) ?, b = 17.8496(12) ?, and c = 13.518(3) ?; β = 91.449(15)°; V = 1372.1(4) ?~3. The sample is monophasic.