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Structural behavior of Tl-exchanged natrolite at high pressure depending on the composition of pressure-transmitting medium

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Abstract

The structural evolution of Tl-exchanged natrolite with idealized formula Tl2[Al2Si3O10]·2H2O, compressed in penetrating (water:ethanol 1:1) and non-penetrating (paraffin) media, was studied up to 4 GPa. The presence of Tl+ with non-bonded electron lone pairs, which can be either stereo-chemically active or passive, determines distinctive features of the high-pressure behavior of the Tl-form. The effective volume of assemblages Tl+(O,H2O) n depends on the E-pairs activity: single-sided coordination correlates with smaller volumes. At ambient conditions, there are two types of Tl positions, only one of them having a nearly single-sided coordination as a characteristic of stereo-activity of the Tl+ E pair. Upon the compression in paraffin, a phase transition occurs: a 5% volume contraction of flexible natrolite framework is accompanied by the conversion of all the Tl+ cations into stereo-chemically active state with a single-sided coordination. This effect requires the reconstruction of all the extra-framework subsystems with the inversion of the cation and H2O positions. The compression in water-containing medium leads to the increase of H2O content up to three molecules pfu through the filling of partly vacant positions. This hinders a single-sided coordination of Tl ions and preserves the configuration of their ion-molecular subsystem. It is likely that the extra-framework subsystem is responsible for the super-structure modulation.

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Acknowledgements

This study was supported by the Russian Foundation of Basic Researches (Grant 16-05-00401) and bу state assignment project (0330-2016-0004). Structural experiments were carried out involving the equipment belonging to the Siberian Synchrotron and Terahertz Radiation Centre (SSTRC).

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Authors and Affiliations

  1. V. S. Sobolev Institute of Geology and Mineralogy, Siberian Branch of Russian Academy of Sciences, Novosibirsk, Russia

    Yu. V. Seryotkin, A. Yu. Likhacheva, S. N. Dementiev & S. V. Rashchenko

  2. Novosibirsk State University, Novosibirsk, Russia

    Yu. V. Seryotkin & S. V. Rashchenko

  3. A.V. Nikolaev Institute of Inorganic Chemistry, Siberian Branch of Russian Academy of Sciences, Novosibirsk, Russia

    V. V. Bakakin

  4. G. I. Budker Institute of Nuclear Physics, Siberian Branch of Russian Academy of Sciences, Novosibirsk, Russia

    A. Yu. Likhacheva

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  1. Yu. V. Seryotkin
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  4. S. N. Dementiev
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  5. S. V. Rashchenko
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Correspondence to Yu. V. Seryotkin.

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Seryotkin, Y.V., Bakakin, V.V., Likhacheva, A.Y. et al. Structural behavior of Tl-exchanged natrolite at high pressure depending on the composition of pressure-transmitting medium. Phys Chem Minerals 44, 615–626 (2017). https://doi.org/10.1007/s00269-017-0887-0

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  • DOI: https://doi.org/10.1007/s00269-017-0887-0

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