Results of 25 years of uranium compound research at the department of crystallography, St. Petersburg State University

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Abstract

The study of uranium-bearing natural and synthetic compounds has been one of the primary research focuses at the Department of Crystallography, St. Petersburg State University, for the past 25 years. During this period, the department's researchers have discovered three new uranium minerals, determined and refined the structures of 15 known mineral species, and synthesized and characterized over 370 new uranium compounds. These efforts have resulted in the publication of more than 200 scientific works, including three monographs and over 190 articles in leading international journals in the fields of mineralogy, crystallography, and chemistry. This review highlights the most significant and intriguing results, in the authors' view, from crystal-chemical studies of uranium compounds conducted by the Department of Crystallography at St. Petersburg State University over the past quarter-century.

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About the authors

V. V. Gurzhiy

St. Petersburg University

Author for correspondence.
Email: vladgeo17@mail.ru

Institute of Earth Sciences

Russian Federation, St. Petersburg

E. V. Nazarchuk

St. Petersburg University

Email: vladgeo17@mail.ru

Institute of Earth Sciences

Russian Federation, St. Petersburg

Y. G. Tagirova

St. Petersburg University

Email: vladgeo17@mail.ru

Institute of Earth Sciences

Russian Federation, St. Petersburg

S. V. Krivovichev

St. Petersburg University; Kola Science Centre RAS

Email: vladgeo17@mail.ru

Institute of Earth Sciences, Nanomaterials Research Centre

Russian Federation, St. Petersburg; Apatity

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Supplementary files

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2. Fig. 1. Coordination polyhedra of uranium atoms in uranyl compounds in atomic and polyhedral representations: tetragonal (a, b), pentagonal (c, d) and hexagonal dipyramid (d, e). The valence forces of U–O bonds in valence units (v. units) are indicated.

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3. Fig. 2. Scheme of topology construction. Unification of the hexagonal dipyramid Ur with the TO3 group through a common vertex and edge in the polyhedral (a) and ball-and-stick representation (b), as well as the corresponding black-and-white graph (c). A fragment of a dense structure with unification of polyhedra through common edges (d), O atoms that participate in the formation of bonds with more than one cation (d), and the anionic topology constructed from them (e).

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4. Fig. 3. Island complexes described in the structures of [C5H14N2]2[UO2(SO4)3] [131] (a), Rb6((UO2)(MoO4)4) [132] (b), [C3H12N2]2[(UO2)2(SO4)4(H2O)4](H2O)2 and [C3H12N2][(UO2)(SeO4)2(H2O)2](H2O) [133] (c), Na6((UO2)(MoO4)4) [134] and in the structure of the mineral bluelizardite Na7(UO2)(SO4)4CI(H2O)2 (d), Na3Tl3((UO2)(MoO4)4) [135] (e), [C4H14N2]2[UO2(SO4)3](H2O)2 [131], [C6H22N4]2[(UO2)2(SO4)6](H2O) [136] and [ZnC10N2H8]2[(UO2)(HPO4)3] [139] (e).

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5. Fig. 4. One-dimensional complexes in the structures of uranyl compounds with TO4 2– tetrahedra (T6+ = S, Cr, Se, Mo).

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6. Fig. 5. Layer of [(UO2)(CrO4)(NO3)]– from UrO3NO3 blocks (a) and their graph (b).

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7. Fig. 6. Nine types of layer topology with the ratio UO2 : TO4 = 2 : 3.

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8. Fig. 7. Layers in the structure of [iPrNH3]3[(UO2)3(CrO4)2O(OH)3] [197].

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9. Fig. 8. Projection of the structure of [Me2NH2]2[(UO2)4(MoO4)5(H2O)](H2O) onto the ab plane (a). Idealized graphs of fundamental chains (b) in the structures of (NH4)4[(UO2)5(MoO4)7](H2O) and M2(UO2)6(MoO4)7(H2O)n (M = Sr, Mg; n = 15, 18) (c).

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10. Fig. 9. Crystal structure of Rb2[(UO2)2(Si8O19)](H2O)2.5. Projection of the structure onto the ac plane (a). Single layer obtained by cutting a double silicate layer [Si8O19]6– (b).

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11. Fig. 10. Fragment of a layered complex of the composition [(UO2)(TO4)]2– (T = As, P) (a) and the corresponding black-and-white graph of the otenitic topology (b). Crystal structure of uramphite (c).

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12. Fig. 11. Crystals and structure of a synthetic analogue of ewingite: dendritic aggregate (a), packing of uranyl-carbonate clusters (b), main uranium-containing building blocks of the structure (c) and uranium-carbonate nanocluster (d, e).

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13. Fig. 12. Evolution of six studied metamict minerals with increasing temperature according to data [263–267].

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14. Fig. 13. Crystal structure of compounds of the Cs2[(AnO2)2(TO4)3] group (where An = U, Np; T = S, Se, Cr, Mo) (a); polyhedral representation of the layer (b) and the corresponding graphs (c).

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15. Fig. 14. Use of chromium(VI) oxide in the synthesis of chromates and polychromates from aqueous solutions. Examples of island (0D), chain (1D) and layered (2D) complexes are shown.

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16. Fig. 15. Layered uranyl-selenate complexes of the composition [(UO2)2(SeO4)3(H2O)]2– and the corresponding real graphs demonstrating different topological types.

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17. Fig. 16. Uranyl sulfate layer in the structure of (C6H16N2)(H5O2)[(UO2)2(SO4)3(HSO4)] [301] (a); the arrangement of interlayer molecules relative to the black-and-white graph of the inorganic layer (b).

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18. Fig. 17. Scheme of construction of structures with layers of [(UO2)2(T6+O4)3(H2O)]2– (T6+ = S, Cr, Se) from racemic pairs.

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19. Fig. 18. Packing of water protonated molecules in the interlayer space of the structures [(H5O2)3(H9O4)](C8H16O4)2[(UO2)2(SeO4)3(H2O)]2 (a) and [(H5O2)(H3O)3](C10H20O5)[(UO2)3(SeO4)5(H2O)] (b) [310]. Hydrogen bonds are shown by dotted lines.

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20. Fig. 19. Island complexes [(UO2)(CrO4)(H2O)3]0 (a) and [(UO2)4(H2O)12(CrO4)2(Cr2O7)2(Cr3O10)]2– (b).

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21. Fig. 20. Chains of [(UO2)2(CrO4)2(Cr2O7)2(H2O)]4– (a) and [(UO2)3(CrO4)4(Cr2O7)2]6– (b).

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22. Fig. 21. Schematic diagram of the structure of the hemispheres (a) and projections of the structure of [iPrNH3]10[(UO2)13(Cr12 5+O42)(Cr6+O4)6(H2O)6](H2O)6 (b).

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23. Fig. 22. Crystal structure of (H3O)2[C12H30N2]3[(UO2)4(SeO4)8](H2O)5 [328].

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24. Fig. 23. Combination of uranium polyhedra to form the [Ur9O24]6+ complex (a) and the method of joining such complexes into a layer. Diameter of the channel, the walls of which are built of silicon and uranium polyhedra (b). L1 layers in the Rb2O(UO2)2O(Si3O8) structure (c). Separation of complexes in layers in the U3O8 structure (d). The method of unfolding the tubular complex [(UO2)(Si6O17)]8– (d) onto a plane (e).

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25. Fig. 24. Crystal structures of (H3O)2K[(H3O)@([18]crown-6)][(UO2)3(SeO4)5](H2O)4 [220] (a) and K5[(UO2)3(SeO4)5](NO3)H2O3.5 [342, 343] (b); cross-section of nanotubulene in the polyhedral (c) and ball-and-stick models (d).

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26. Fig. 25. Division of [(UO2)3(MoO4)5]4– layers into fundamental chains.

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27. Fig. 26. Division of the [(UO2)2(TO4)3(H2O)]2– (a) and [(UO2)3(TO4)5]4– (b) layers into their constituent chains A and B. The method of stacking chains A and B in the [(UO2)5(TO4)8(H2O)]6– layers (c). Chains A and A1 are connected by a mirror plane of symmetry.

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28. Fig. 27. The studied nanotubulenes in the structures K5(UO2)3(SeO4)5(NO3) 3.5(H2O) (a), Na(phgH)7[(UO2)6(SO4)10](H2O)3.5 (b), (C4H12N)14[(UO2)10(SeO4)17(H2O)] (c). The method of cutting the nanotubulene and unfolding it into layers. Representation of the fundamental chains from which the walls of the nanotubulenes are built. Each color corresponds to the chain type.

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29. Fig. 28. Dimension fields in the compositional diagram of the UO2TO4–A2TO4–H2O system (A is a monovalent cation; T is S, Se, Cr, Mo; n = 2(q – p)), compiled on the basis of structural data [297]. The corrected dimension fields based on the new structural data are shown by bold dotted lines. A list of compounds and relevant references are given in [381].

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30. Fig. 29. Scheme of displacement of selenate tetrahedra as a result of hydrogen interaction with guanidinium molecules in the structure of [CH6N3]2[(UO2)2(SeO4)3] (a) and superposition of guanidinium cations on the black-and-white graph of the inorganic layer (b). Legend: H-bonds are dotted lines, flags “O in P2” and “O in P21212” indicate the positions of oxygen atoms during structure refinement in space groups P2 and P21212, respectively.

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31. Fig. 30. Distribution of the contribution of topological complexity to the total information complexity of the crystal structure of the studied natural and synthetic uranyl sulfates and selenites.

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