Abstract
The work reviews the structure, non-stoichiometry, and ionic mobility of molybdates, tungstates, and other compounds crystallizing in the structure type of alluaudite (Na, Ca)(Fe, Mn, Mg)3(PO4)3 with the general Moore′s crystal chemical formula X(2)X(1)M(1)M(2)2(TO4)3, where X are large cations Na+, Ca2+, K+, Pb2+, etc., with the coordination number 8; M are octahedral cations, T = P, As, V, S, Mo, W. Using this formula and the corresponding site occupancies, possible limits of double molybdate and tungstate compositions of the alluaudite family are determined. Various types of distortions (superstructures) of alluaudite are considered; several groups of phases with different symmetries, numbers of anions in the unit cell, and vector relations with the unit cell of the original alluaudite structure are distinguished. It is shown that chains of partially defective positions X(2) and X(1) aligned along axis c play a key role in the transport of sodium cations in the alluaudite type phases. Phosphates and sulfates with alluaudite structure exhibit mainly 1D transport of sodium ions; however, calculations of the bond-valence sum maps, NMR data, and ab initio calculations show that 2D transport in the (100) plane is possible in complex molybdates and tungstates due to the transport of Na+ ions between X(2)–X(2) and X(1)–X(1) channels through the bridging site M(1). It is shown that the family of alluaudite-related (pseudo)orthorhombic triple molybdates Na10Cs4M5(MoO4)12 (M = Mn, Co) and Na25Cs8R5(MoO4)24 (R = Fe, Sc, In) also exhibits 2D diffusion of sodium ions via successive zigzag ion hoppings and that 3D transport may appear at elevated temperatures.
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Notes
* According to the notations of this work, α refers to the low-temperature modification.
* In contrast to the common viewpoint [75] that associates the term “daltonide” with the topology of phase diagrams and extrema of the properties of compounds with variable composition, we follow the crystal-chemical interpretation by G. B. Bokii and consider daltonide as a non-stoichiometric compound with Dalton points where the structure is completely or partially ordered at one or more crystallographic sites within (or at the borders of) the homogeneity region. In our opinion, the knowledge of the structure and the identification of such points is absolutely necessary to construct a meaningful crystal-chemical classification of non-stoichiometric compounds as phases that are formed similarly to substitution-, interstitial-, or omission solid solutions.
* The BVS contour maps (isosurfaces) for sodium cations were constructed from the atomic coordinates of Na2.56Fe1.72(SO4)3 and the structures of other compounds discussed below using the 3DBVSMAPPER software [89].
* The composition of this phase was determined from structural data and needs verification (see the above discussion).
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This work was carried out within the State Assignments of Nikolaev Institute of Inorganic Chemistry SB RAS, Baikal Institute of Nature Management SB RAS, M. N. Mikheev Institute of Metal Physics UB RAS, Institute of Solid State Chemistry UB RAS, and partially funded by RFBR (projects 16-03-00510 and 17-03-00333). The part of the research devoted to the determination of the mechanism of diffusion of sodium ions in molybdates was funded by the Russian Science Foundation (project 18-12-00395).
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Russian Text © The Author(s), 2022, published in Zhurnal Strukturnoi Khimii, 2022, Vol. 63, No. 7, 96516.https://doi.org/10.26902/JSC_id96516
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Solodovnikov, S.F., Gulyaeva, O.A., Savina, A.A. et al. MOLYBDATES AND TUNGSTATES OF THE ALLUAUDITE FAMILY: CRYSTAL CHEMISTRY, COMPOSITION, AND IONIC MOBILITY. J Struct Chem 63, 1101–1133 (2022). https://doi.org/10.1134/S0022476622070071
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DOI: https://doi.org/10.1134/S0022476622070071