ISSN 10703284, Russian Journal of Coordination Chemistry, 2013, Vol. 39, No. 3, pp. 234–238. © Pleiades Publishing, Ltd., 2013. Original Russian Text © O.V. Kovalchukova, A.I. Stash, Dinh Do Nguyen, S.B. Strashnova, V.K. Bel’skii, 2013, published in Koordinatsionnaya Khimiya, 2013, Vol. 39, No. 3, pp. 136–140. 234 This work was intended to continue our manyyear investigations of the structures and complexation reactions of tetraoxopyridines. For instance, ammo nium 4nitro2,3,5,6tetraoxopyridinate, (NH 4 ) 2 (C 5 HO 6 N 2 ) 2 , is a precursor for the synthesis of coordi nation compounds containing the tetraoxopyridinate anion. Earlier, we have studied the structure of (NH 4 ) 2 (C 5 HO 6 N 2 ) 2 by Xray diffraction [1], obtained the complexes М(H 2 O) 6 (C 5 HN 2 O 6 ) 2 2H 2 O (М = Ni 2+ , Cu 2+ , Co 2+ , and Zn 2+ ) in the crystalline state, and structurally identified the complex Ni(H 2 O) 6 (C 5 HN 2 O 6 ) 2 2H 2 O [2]. Unusual solva tolytic decomposition of the pyridine ring of (NH 4 ) 2 (C 5 HN 2 O 6 ) 2 into 2methyl1,3diazolium hydro bis(oxamate) has been studied in [3]. The crystal structures of sodium 4nitro2,3,5,6tetraoxopyridi nate trihydrate and ammonium sodium bis(4nitro 2,3,5,6tetraoxopyridinate) monohydrate have been examined in [4]. In the present work, we obtained hexaaquacad mium(II) and hexaaquacobalt(II) 4nitro2,3,5,6 tetraoxopyridinates, [Cd(H 2 O) 6 ](C 5 HN 2 O 6 ) 2 2H 2 O (I) and [Co(H 2 O) 6 ](C 5 HN 2 O 6 ) 2 2H 2 O (II), and the product of their cocrystallization, [Cd 0.32 Co 0.68 (H 2 O) 6 ](C 5 HN 2 O 6 ) 2 2H 2 O (III). In addi tion, we determined their crystal and molecular struc tures and studied their properties. EXPERIMENTAL Cobalt(II) and cadmium(II) chloride hydrates (reagent grade) were used; (NH 4 ) 2 (C 5 HO 6 N 2 ) 2 was prepared as described in [5, 6]. Synthesis of metal complexes. An appropriate metal chloride (5 mmol) was dissolved in ethanol (10– 20 mL) and the resulting solution was brought to boil ing. Then a hot solution of (NH 4 ) 2 (C 5 HO 6 N 2 ) 2 in acetonitrile was added dropwise. The reaction mixture was kept on a water bath for 30 min, cooled, and left for several days until precipitation occurred. The pre cipitates were filtered off, washed with ethanol, and dried to constant weights. The yields of the complexes were 30–45%. Yellowbrown single crystals suitable for Xray diffraction were obtained by recrystallization from ethanol. The contents of the metals were determined by spectrophotometry. Chemical analyses for nitrogen For Cd(H 2 O) 6 (C 5 HO 6 N 2 ) 2 2H 2 O (I) (М = 662.71) anal. calcd. (%): С, 18.12; N, 8.45; Н, 3.35; Cd, 16.96. Found (%): С, 17.88; N, 8.72; Н, 3.17; Cd, 17.30. For Co(H 2 O) 6 (C 5 HO 6 N 2 ) 2 2H 2 O (II) (M = 609.23) anal. calcd. (%): C, 19.72; N, 9.20; H, 3.64; Co, 9.67. Found (%): C, 20.14; N, 9.24; H, 3.01; Co, 9.37. Hexaaquacobalt(II) and Hexaaquacadmium(II) 4Nitro2,3,5,6 Tetraoxopyridinates [M(H 2 O) 6 ](C 5 HN 2 O 6 ) 2 · 2H 2 O (M = Co and Cd): Synthesis, Structures, and Properties O. V. Kovalchukova a, *, A. I. Stash b , Dinh Do Nguyen a , S. B. Strashnova a , and V. K. Bel’skii b a Peoples Friendship University, ul. MiklukhoMaklaya 6, Moscow, Russia b Karpov Research Institute of Physical Chemistry, ul. Vorontsovo pole 10, Moscow, Russia *email: okovalchukova@mail.ru Received July 12, 2012 Abstract—The complexes [Cd(H 2 O) 6 ](C 5 HN 2 O 6 ) 2 2H 2 O (I) and [Co(H 2 O) 6 ](C 5 HN 2 O 6 ) 2 2H 2 O (II) were obtained in the crystalline state by reactions of cobalt chloride and cadmium chloride with ammonium 4nitro2,3,5,6tetraoxopyridinate, (NH 4 ) 2 (C 5 HO 6 N 2 ) 2 . Their cocrystallization gave the heterometallic complex [Cd 0.32 Co 0.68 (H 2 O) 6 ](C 5 HN 2 O 6 ) 2 2H 2 O (III). The crystal and molecular structures of complexes IIII were determined by Xray diffraction. It was demonstrated that the complexation reactions occur by replacement of two ammonium cations 4nitro2,3,5,6tetraoxopyridinate by the complex cations [M(H 2 O) 6 ] 2+ . The tetraoxopyridinate anions and the complex cations are hydrogenbonded through the coordinated and crystallization water molecules as well as through the O atoms of the organic anion. The thermolysis of complexes I and II was examined by TGA. DOI: 10.1134/S1070328413030044