Topotactic and reconstructive changes at high pressures and temperatures from Cs-natrolite to Cs-hexacelsian

Huijeong Hwang, Donghoon Seoung, G. Diego Gatta, Douglas A. Blom, Thomas Vogt, Yongjae Lee

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Synchrotron X-ray powder diffraction experiments have been performed on dehydrated Csexchanged natrolite to systematically investigate successive transitions under high pressures and temperatures. At pressures above 0.5(1) GPa using H2O as a pressure-transmitting medium and after heating to 100 °C, dehydrated Cs16Al16Si24O80 (deh-Cs-NAT) transforms to a hydrated phase Cs16Al16Si24O80·16H2O (Cs-NAT-II), which has a ca. 13.9% larger unit-cell volume. Further compression and heating to 1.5 GPa and 145 °C results in the transformation of Cs-NAT-II to Cs16Al16Si32O96 (anh-Cs-POL), a H2O-free pollucite-like triclinic phase with a 15.6% smaller unit-cell volume per 80 framework oxygen atoms (80Of). At pressures and temperatures of 3.7 GPa and 180 °C, a new phase Cs1.547Al1.548Si6.452O16 (Cs-HEX) with a hexacelsian framework forms, which has a ca. 1.8% smaller unit-cell volume per 80Of. This phase can be recovered after pressure release. The structure of the recovered Cs-HEX has been refined in space group P63/mcm with a = 5.3731(2) Å and c = 16.6834(8) Å, and also been confirmed by HAADF-STEM real space imaging. Similar to the hexacelsian feldspar (i.e., BaAl2Si2O8), Cs-HEX contains Cs+ cations that act as bridges between the upper and lower layers composed of tetrahedra and are hexa-coordinated to the upper and lower 6-membered ring windows. These pressure-and temperature-induced reactions from a zeolite to a feldspar-like material are important constraints for the design of materials for Cs+ immobilization in nuclear waste disposal.

Original languageEnglish
Pages (from-to)1562-1567
Number of pages6
JournalAmerican Mineralogist
Volume100
Issue number7
DOIs
Publication statusPublished - 2015 Jul 1

Fingerprint

natrolite
feldspar
Temperature
cells
heating
waste disposal
Radioactive Waste
radioactive wastes
Zeolites
Heating
immobilization
tetrahedrons
zeolite
radioactive waste
oxygen atoms
Synchrotrons
synchrotrons
Waste disposal
transform
X ray powder diffraction

All Science Journal Classification (ASJC) codes

  • Geophysics
  • Geochemistry and Petrology

Cite this

Hwang, Huijeong ; Seoung, Donghoon ; Gatta, G. Diego ; Blom, Douglas A. ; Vogt, Thomas ; Lee, Yongjae. / Topotactic and reconstructive changes at high pressures and temperatures from Cs-natrolite to Cs-hexacelsian. In: American Mineralogist. 2015 ; Vol. 100, No. 7. pp. 1562-1567.
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title = "Topotactic and reconstructive changes at high pressures and temperatures from Cs-natrolite to Cs-hexacelsian",
abstract = "Synchrotron X-ray powder diffraction experiments have been performed on dehydrated Csexchanged natrolite to systematically investigate successive transitions under high pressures and temperatures. At pressures above 0.5(1) GPa using H2O as a pressure-transmitting medium and after heating to 100 °C, dehydrated Cs16Al16Si24O80 (deh-Cs-NAT) transforms to a hydrated phase Cs16Al16Si24O80·16H2O (Cs-NAT-II), which has a ca. 13.9{\%} larger unit-cell volume. Further compression and heating to 1.5 GPa and 145 °C results in the transformation of Cs-NAT-II to Cs16Al16Si32O96 (anh-Cs-POL), a H2O-free pollucite-like triclinic phase with a 15.6{\%} smaller unit-cell volume per 80 framework oxygen atoms (80Of). At pressures and temperatures of 3.7 GPa and 180 °C, a new phase Cs1.547Al1.548Si6.452O16 (Cs-HEX) with a hexacelsian framework forms, which has a ca. 1.8{\%} smaller unit-cell volume per 80Of. This phase can be recovered after pressure release. The structure of the recovered Cs-HEX has been refined in space group P63/mcm with a = 5.3731(2) {\AA} and c = 16.6834(8) {\AA}, and also been confirmed by HAADF-STEM real space imaging. Similar to the hexacelsian feldspar (i.e., BaAl2Si2O8), Cs-HEX contains Cs+ cations that act as bridges between the upper and lower layers composed of tetrahedra and are hexa-coordinated to the upper and lower 6-membered ring windows. These pressure-and temperature-induced reactions from a zeolite to a feldspar-like material are important constraints for the design of materials for Cs+ immobilization in nuclear waste disposal.",
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Topotactic and reconstructive changes at high pressures and temperatures from Cs-natrolite to Cs-hexacelsian. / Hwang, Huijeong; Seoung, Donghoon; Gatta, G. Diego; Blom, Douglas A.; Vogt, Thomas; Lee, Yongjae.

In: American Mineralogist, Vol. 100, No. 7, 01.07.2015, p. 1562-1567.

Research output: Contribution to journalArticle

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AU - Hwang, Huijeong

AU - Seoung, Donghoon

AU - Gatta, G. Diego

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AU - Lee, Yongjae

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