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Melilite-type and melilite-related compounds: structural variations along the join Sr2−x Ba x MgSi2O7 (0 ≤ x ≤ 2) and high-pressure behavior of the two end-members

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An Erratum to this article was published on 27 April 2012

Abstract

The structural variations along the solid solution Sr2−x Ba x MgSi2O7 (0 ≤ x ≤ 2), combined to the high-pressure characterization of the two end-members, have been studied. A topological change from the tetragonal (melilite-type) to the monoclinic (melilite-related) structure along the join Sr2MgSi2O7 (e.g., \( P\bar{4}2_{1} m \))–Ba2MgSi2O7 (e.g., C2/c) occurs with a Ba content higher than 1.6 apfu. Favored in the crystallization from a melt, the tetragonal form has a tetrahedral sheet topology exclusively based on five-membered rings, which provide a regular “4 up + 4 down” ligand arrangement. In contrast, the melilite-related structure, favored by solid-state reaction synthesis, is made by alternating six- and four-membered tetrahedral rings, which give an asymmetric arrangement of alternated “5 up + 3 down” and “3 up + 5 down” ligands around Sr or Ba. This latter configuration is characterized by an additional degree of freedom with Ba polyhedra hosted in the interlayer with a more irregular and compact coordination and longer Ba–O bond distances. Further insights into the relationships between the two melilite typologies were achieved by investigating the in situ high-pressure behavior of these systems. The synchrotron high-pressure experiments allowed to calculate the elastic moduli for the Sr melilite-type end-member and for the Ba monoclinic polymorph (Sr2MgSi2O7: K T0 = 107, K a=b  = 121, and K c  = 84 GPa; m-Ba2MgSi2O7: K T0 = 85, K a  = 96, K b  = 72, and K c  = 117 GPa) and compare them with those reported in the literature for åkermanite (Ca2MgSi2O7). The results show that, although the volume of Ba polyhedron in tetragonal polymorphs is larger than in the monoclinic forms, the interlayer compressibility is significantly lower in the former structures due to the occurrence of very short Ba–O distances. This unfavored Ba environment also makes tetragonal Ba2MgSi2O7 a metastable phase at room conditions, possibly favored by high pressure. However, no phase transition occurs from monoclinic to tetragonal form due to kinetic hindrance in reconstructing the sheet topology.

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Acknowledgments

Access to ID27 beamline at the European Synchrotron Radiation Facility (ESRF) was provided under the public beamtime program (exp. no. HS3936). We thank Pierre Bouvier (ESRF) and Michael Hanfland (ESRF) for advices and technical support. In addition, we are grateful to Luca Bindi and an anonymous referee for their constructive reviews, as well as to the criticisms raised by the editor Milan Rieder, which greatly improved the quality of this article.

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Authors and Affiliations

  1. Earth Science Department, University of Ferrara, Via Saragat 1, 44100, Ferrara, Italy

    Matteo Ardit & Giuseppe Cruciani

  2. Institute of Science and Technology for Ceramics (ISTEC-CNR), Via Granarolo 64, 48018, Faenza, Italy

    Michele Dondi

  3. Earth Science Department, University of Milano, Via Botticelli 23, 20133, Milano, Italy

    Marco Merlini

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  1. Matteo Ardit
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  2. Michele Dondi
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  4. Giuseppe Cruciani
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Correspondence to Matteo Ardit.

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Ardit, M., Dondi, M., Merlini, M. et al. Melilite-type and melilite-related compounds: structural variations along the join Sr2−x Ba x MgSi2O7 (0 ≤ x ≤ 2) and high-pressure behavior of the two end-members. Phys Chem Minerals 39, 199–211 (2012). https://doi.org/10.1007/s00269-011-0475-7

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