Halide-sodalites: thermal behavior at low temperatures and local deviations from the average structure

Marius Wolpmann; Martin Etter; Andrea Kirsch; Filippo Balzaretti; Wilke Dononelli; Lars Robben; Thorsten M. Gesing

doi:10.1515/zkri-2022-0037

Published by De Gruyter (O) November 4, 2022

Halide-sodalites: thermal behavior at low temperatures and local deviations from the average structure

Marius Wolpmann , Martin Etter , Andrea Kirsch , Filippo Balzaretti , Wilke Dononelli , Lars Robben and Thorsten M. Gesing

From the journal Zeitschrift für Kristallographie - Crystalline Materials

https://doi.org/10.1515/zkri-2022-0037

Showing a limited preview of this publication:

Abstract

Sodalites of the general type |Na₈X₂|[T¹T²O₄]₆ with X = Cl⁻, Br⁻, I⁻ have been synthesized for Al–Si, Ga–Si, Al–Ge and Ga–Ge as T¹–T² frameworks. The structures were examined using in-house and synchrotron X-ray diffraction, Raman spectroscopy, force-field structure optimizations and DFT based ab-initio molecular dynamics (MD) computations. Calculated phonon density of states (PDOS) of the 12 compounds show only minor differences within a framework composition with a lowering of certain phonon energies with increasing anion size. Earlier published Debye and Einstein temperatures obtained with a Debye-Einstein-anharmonicity (DEA) model approach are confirmed using the determined low-temperature lattice parameters (18 K–293 K) and show no correlation with the respective PDOS. Small-box refinements against radial pair distribution functions (PDF) allowed the determination of anisotropic displacement ellipsoids (ADP) for Na⁺ and O²⁻, indicating a strong dependency of the ADP of Na⁺ on the chemical composition. Significantly lower thermal displacements from MD calculations suggested an influence of structural displacements. For compounds with an aspherical ADP for sodium, structural models could be refined in which the sodium is located on two 8e or one 24i site (both partially occupied), and also temperature-dependent (100 K–300 K) for the compounds with Ga–Ge framework. 3D-plots of the bond-valence sums of Na⁺ further validate the structural differences. These results imply that the local structure of halide-sodalites in many cases is not best described by the known average structure and may even not be cubic.

Keywords: GULP; molecular dynamics; sodalite; total scattering

Corresponding author: Lars Robben, Institute of Inorganic Chemistry and Crystallography, University of Bremen, Leobener Straße 7, D-28359 Bremen, Germany; and MAPEX Center for Materials and Processes, University of Bremen, Bibliotheksstraße 1, D-28359 Bremen, Germany, E-mail: lrobben@uni-bremen.de

Funding source: Deutsche Forschungsgemeinschaft (DFG)

Award Identifier / Grant number: RO5995/2-1

Acknowledgement

We gratefully acknowledge the Deutsche Forschungsgemeinschaft (DFG) for financial support through RO5995/2-1 and within the large instrument program (INST 144/335-1 FUGG Raman spectrometer, INST 144/435-1 FUGG TD X-ray powder diffractometer and INST 144/458-1 FUGG Std. X-ray powder diffractometer). We also acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III beamlines P02.1 and P21.1. We would like to thank Dr. Soham Banerjee for assistance in using beamline P21.1. Beamtime was allocated for proposals I-20200180 and I-20200535. AK would like to thank Niels Lefeld and Mathias Gogolin for beamtime assistance.

Author contributions: All the authors have accepted responsibility for the entire content of this submitted manuscript and approved submission.
Research funding: This work was funded by Deutsche Forschungsgemeinschaft (DFG) (RO5995/2-1).
Conflict of interest statement: The authors declare no conflicts of interest regarding this article.

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Supplementary Material

The online version of this article offers supplementary material (https://doi.org/10.1515/zkri-2022-0037).

Received: 2022-06-02

Accepted: 2022-10-20

Published Online: 2022-11-04

Published in Print: 2023-01-27

Halide-sodalites: thermal behavior at low temperatures and local deviations from the average structure

Abstract

Acknowledgement

References

Supplementary Material

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