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 language | English |
|---|---|
| Pages (from-to) | 1562-1567 |
| Number of pages | 6 |
| Journal | American Mineralogist |
| Volume | 100 |
| Issue number | 7 |
| DOIs | |
| Publication status | Published - 2015 Jul 1 |
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All Science Journal Classification (ASJC) codes
- Geophysics
- Geochemistry and Petrology
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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 journal › Article
TY - JOUR
T1 - Topotactic and reconstructive changes at high pressures and temperatures from Cs-natrolite to Cs-hexacelsian
AU - Hwang, Huijeong
AU - Seoung, Donghoon
AU - Gatta, G. Diego
AU - Blom, Douglas A.
AU - Vogt, Thomas
AU - Lee, Yongjae
PY - 2015/7/1
Y1 - 2015/7/1
N2 - 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.
AB - 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.
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U2 - 10.2138/am-2015-5090
DO - 10.2138/am-2015-5090
M3 - Article
AN - SCOPUS:84937790008
VL - 100
SP - 1562
EP - 1567
JO - American Mineralogist
JF - American Mineralogist
SN - 0003-004X
IS - 7
ER -