Abstract
Structural phase transitions in hydrous Cs-exchanged natrolite (Cs-NAT-hyd) and anhydrous Cs-exchanged natrolite (Cs-NAT-anh) have been investigated as a function of pressure and temperature using micro-Raman scattering and synchrotron infrared (IR) spectroscopy with pure water as the penetrating pressure medium. The spectroscopic results indicate that Cs-NAT-hyd undergoes a reversible phase transition around 4.72 GPa accompanied by the discontinuous frequency shifts of the breathing vibrational modes of the four-ring and helical eight-ring units of the natrolite framework. On the other hand, we observe that Cs-NAT-anh becomes rehydrated at 0.76 GPa after heating to 100 °C and then transforms into two distinctive phases at 2.24 and 3.41 GPa after temperature treatments at 165 and 180 °C, respectively. Both of these high-pressure phases are characterized by the absence of the helical eight-ring breathing modes, which suggests the collapse of the natrolite channel and formation of dense high-pressure polymorphs. Together with the fact that these high-pressure phases are recoverable to ambient conditions, our results imply a novel means for radionuclide storage utilizing pressure and a porous material.
| Original language | English |
|---|---|
| Pages (from-to) | 2159-2164 |
| Number of pages | 6 |
| Journal | Journal of Physical Chemistry C |
| Volume | 116 |
| Issue number | 3 |
| DOIs | |
| Publication status | Published - 2012 Jan 26 |
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All Science Journal Classification (ASJC) codes
- Electronic, Optical and Magnetic Materials
- Energy(all)
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films
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High-pressure spectroscopic study of hydrous and anhydrous Cs-exchanged natrolites. / Liu, Dan; Seoung, Donghoon; Lee, Yongmoon; Liu, Zhenxian; Lee, Jong Won; Yoon, Ji Ho; Lee, Yongjae.
In: Journal of Physical Chemistry C, Vol. 116, No. 3, 26.01.2012, p. 2159-2164.Research output: Contribution to journal › Article
TY - JOUR
T1 - High-pressure spectroscopic study of hydrous and anhydrous Cs-exchanged natrolites
AU - Liu, Dan
AU - Seoung, Donghoon
AU - Lee, Yongmoon
AU - Liu, Zhenxian
AU - Lee, Jong Won
AU - Yoon, Ji Ho
AU - Lee, Yongjae
PY - 2012/1/26
Y1 - 2012/1/26
N2 - Structural phase transitions in hydrous Cs-exchanged natrolite (Cs-NAT-hyd) and anhydrous Cs-exchanged natrolite (Cs-NAT-anh) have been investigated as a function of pressure and temperature using micro-Raman scattering and synchrotron infrared (IR) spectroscopy with pure water as the penetrating pressure medium. The spectroscopic results indicate that Cs-NAT-hyd undergoes a reversible phase transition around 4.72 GPa accompanied by the discontinuous frequency shifts of the breathing vibrational modes of the four-ring and helical eight-ring units of the natrolite framework. On the other hand, we observe that Cs-NAT-anh becomes rehydrated at 0.76 GPa after heating to 100 °C and then transforms into two distinctive phases at 2.24 and 3.41 GPa after temperature treatments at 165 and 180 °C, respectively. Both of these high-pressure phases are characterized by the absence of the helical eight-ring breathing modes, which suggests the collapse of the natrolite channel and formation of dense high-pressure polymorphs. Together with the fact that these high-pressure phases are recoverable to ambient conditions, our results imply a novel means for radionuclide storage utilizing pressure and a porous material.
AB - Structural phase transitions in hydrous Cs-exchanged natrolite (Cs-NAT-hyd) and anhydrous Cs-exchanged natrolite (Cs-NAT-anh) have been investigated as a function of pressure and temperature using micro-Raman scattering and synchrotron infrared (IR) spectroscopy with pure water as the penetrating pressure medium. The spectroscopic results indicate that Cs-NAT-hyd undergoes a reversible phase transition around 4.72 GPa accompanied by the discontinuous frequency shifts of the breathing vibrational modes of the four-ring and helical eight-ring units of the natrolite framework. On the other hand, we observe that Cs-NAT-anh becomes rehydrated at 0.76 GPa after heating to 100 °C and then transforms into two distinctive phases at 2.24 and 3.41 GPa after temperature treatments at 165 and 180 °C, respectively. Both of these high-pressure phases are characterized by the absence of the helical eight-ring breathing modes, which suggests the collapse of the natrolite channel and formation of dense high-pressure polymorphs. Together with the fact that these high-pressure phases are recoverable to ambient conditions, our results imply a novel means for radionuclide storage utilizing pressure and a porous material.
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U2 - 10.1021/jp206678e
DO - 10.1021/jp206678e
M3 - Article
VL - 116
SP - 2159
EP - 2164
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 3
ER -