New Np(VI) and Pu(VI) pyrazine-2-carboxylates isostructural with the uranyl complex [UO 2 . (C 4 H 3 N 2 COO) 2 (H 2 O)] . 2H 2 O were synthesized from aqueous solutions. The unit cell parameters of [NpO 2 . (C 4 H 3 N 2 COO) 2 (H 2 O)] . 2H 2 O and [PuO 2 (C 4 H 3 N 2 COO) 2 (H 2 O)] . 2H 2 O were calculated from the powder X-ray patterns. The thermal behavior of the complexes suggests that the Np(VI) compound contains superstoichiometric water molecules, which are also manifested in the IR spectrum. The absorption spectra of the compounds show that the pyrazinecarboxylic acid anion is a strong complexing agent with respect to Np(VI) and Pu(VI).Among the known uranyl compounds, complexes with various N-donor ligands form a large group [1,2]. Structural studies of uranyl compounds with pyridine and its derivatives showed that the nitrogen atoms of the pyridine rings are strong electron donors with respect to uranium atom and enter into its nearest surrounding of a typical geometry. The coordination polyhedron (CP) of uranium atom is a penta-or hexagonal bipyramid. The axial sites are occupied by the oxygen atoms of the UO 2 2+ group. The composition of the equatorial space of the uranyl ion and, in particular, the number of coordinated nitrogen atoms are determined by the type of ligands; the uranyl complexes are very diverse in structure. For example, the structure of [(UO 2 )(NO 3 ){2,6-(CCH 3 NNH(C 5 H 4 N)-2`) 2 C 5 H 3 N}] 2 [(UO 2 )(NO 3 ) 4 ] [3] includes two crystallographically independent uranium atoms. The CP of the first of them is a hexagonal bipyramid whose equatorial plane is formed by five nitrogen atoms of the organic ligand and oxygen atom of the monodentate nitrate ion; it contains four five-membered metallocycles. The oxygen atoms of two monodentate and two bidentate nitrate ions surround the second uranium atom. Formation of chelate rings involving the nitrogen atom of the pyridine ring and oxygen atom of the carboxy group is characteristic of uranyl pyridinedicarboxylates, including anions of picolinic (2-pyridinecarboxylic) and dipicolinic (2,6-pyridinedicarboxylic) acids. In the uranyl complex with nicotinic (3-pyridinecarboxylic) acid anion, formation of such a chelate ring is sterically hindered, and only the oxygen atom of the carboxy group coordinates to the uranyl ion [7]. Alcock et al.[8] synthesized a uranyl complex with pyrazine-2-carboxylic acid, [UO 2 (C 4 H 3 . N 2 COO) 2 (H 2 O)] . 2H 2 O, and studied its structure. Taking into account the mutual arrangement of the nitrogen atoms of the aromatic ring and the arrangement of the carboxy group at its coordination to uranyl, they noted that, among two donor nitrogen atoms of the pyrazine ring, only the nitrogen atom adjacent to the carboxy group coordinates to uranyl, although theoretically pyrazine can be a bridging ligand and form a polymeric structure. A similar effect is observed in transition metal complexes with pyrazine-2-carboxylic acid [9].In this work, we studied complexes of Np(VI) and Pu(VI) with pyrazine-2-carboxylic ...