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Title: Anisotropic Elastic Behaviour and Structural Evolution of Zeolite Phillipsite at High Pressure: A Synchrotron Powder Diffraction Study

Abstract

The high-pressure (HP) elastic behavior and the P-induced evolution of a natural zeolite phillipsite, K{sub 2}Ca{sub n}Na{sub 2-n}Al{sub 4+n}Si{sub 12-n}O{sub 32}{center_dot}12H{sub 2}O (with n {<=} 2) [a = 9.9291(3), b = 14.2621(6), c = 8.6920(5) {angstrom}, {beta} = 124.592(3){sup o}, space group P2{sub 1}lm], has been investigated by in situ synchrotron X-ray powder diffraction up to 3.64 GPa using a diamond anvil cell and a nominally penetrating hydrous P-transmitting medium. No phase transition has been observed within the P-range investigated. Axial and volume bulk moduli have been calculated using a truncated second-order Birch-Murnaghan Equation-of-State. The refined elastic parameters are V{sub 0} = 1013.3(1) {angstrom}{sup 3}, K{sub 0} = 67(2) GPa[{beta} = 0.0149(5) GPa{sup -1}] for the unit-cell volume; a{sub 0} = 9.9290(7) {angstrom}, K(a) = 69(2) GPa [{beta}(a) = 0.0048(2) GPa{sup -1}] for the a-axis; b{sub 0} = 14.262(2) {angstrom}, K(b) = 49(2) GPa [{beta}(b) = 0.0068(3) GPa{sup -1}] for the b-axis and c{sub 0} = 8.691(1) {angstrom}, K(c) = 111(3) GPa [{beta}(c) = 0.00300(8) GPa{sup -1}] for the c-axis, with K(a):K(b):K(c) = 1.41:1:2.26. The magnitude of the principal unit-strain coefficients, between 0.0001 GPa and 3.64 GPa, were calculated. The unit-strain ellipsoid is oriented with {epsilon}{sub 1}{parallel}b, {epsilon}{sub 2} andmore » {epsilon}{sub 3} lying on the (0 1 0) plane with {epsilon}{sub 3} {angle} a = 115.1(3){sup o} and |{epsilon}{sub 1}|>|{epsilon}{sub 2}|>|{epsilon}{sub 3}||. The structural refinements performed at high-P allow to explain the reasons of the elastic anisotropy. The cooperative rotation of the tetrahedra increase the ellipticity of the channel systems, maintaining the original elliptical configuration (without any 'inversion' in ellipticity).« less

Authors:
;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
Doe - Office Of Science
OSTI Identifier:
929884
Report Number(s):
BNL-80459-2008-JA
TRN: US0806667
DOE Contract Number:
DE-AC02-98CH10886
Resource Type:
Journal Article
Resource Relation:
Journal Name: Microporous and Mesoporous Materials; Journal Volume: 105; Journal Issue: 3
Country of Publication:
United States
Language:
English
Subject:
43 PARTICLE ACCELERATORS; ANISOTROPY; DIAMONDS; DIFFRACTION; ELLIPTICAL CONFIGURATION; POWDERS; PRESSURE RANGE MEGA PA 10-100; ROTATION; SPACE GROUPS; SYNCHROTRON RADIATION; X-RAY DIFFRACTION; ZEOLITES; national synchrotron light source

Citation Formats

Gatta,G., and Lee, Y. Anisotropic Elastic Behaviour and Structural Evolution of Zeolite Phillipsite at High Pressure: A Synchrotron Powder Diffraction Study. United States: N. p., 2007. Web. doi:10.1016/j.micromeso.2007.01.031.
Gatta,G., & Lee, Y. Anisotropic Elastic Behaviour and Structural Evolution of Zeolite Phillipsite at High Pressure: A Synchrotron Powder Diffraction Study. United States. doi:10.1016/j.micromeso.2007.01.031.
Gatta,G., and Lee, Y. Mon . "Anisotropic Elastic Behaviour and Structural Evolution of Zeolite Phillipsite at High Pressure: A Synchrotron Powder Diffraction Study". United States. doi:10.1016/j.micromeso.2007.01.031.
@article{osti_929884,
title = {Anisotropic Elastic Behaviour and Structural Evolution of Zeolite Phillipsite at High Pressure: A Synchrotron Powder Diffraction Study},
author = {Gatta,G. and Lee, Y.},
abstractNote = {The high-pressure (HP) elastic behavior and the P-induced evolution of a natural zeolite phillipsite, K{sub 2}Ca{sub n}Na{sub 2-n}Al{sub 4+n}Si{sub 12-n}O{sub 32}{center_dot}12H{sub 2}O (with n {<=} 2) [a = 9.9291(3), b = 14.2621(6), c = 8.6920(5) {angstrom}, {beta} = 124.592(3){sup o}, space group P2{sub 1}lm], has been investigated by in situ synchrotron X-ray powder diffraction up to 3.64 GPa using a diamond anvil cell and a nominally penetrating hydrous P-transmitting medium. No phase transition has been observed within the P-range investigated. Axial and volume bulk moduli have been calculated using a truncated second-order Birch-Murnaghan Equation-of-State. The refined elastic parameters are V{sub 0} = 1013.3(1) {angstrom}{sup 3}, K{sub 0} = 67(2) GPa[{beta} = 0.0149(5) GPa{sup -1}] for the unit-cell volume; a{sub 0} = 9.9290(7) {angstrom}, K(a) = 69(2) GPa [{beta}(a) = 0.0048(2) GPa{sup -1}] for the a-axis; b{sub 0} = 14.262(2) {angstrom}, K(b) = 49(2) GPa [{beta}(b) = 0.0068(3) GPa{sup -1}] for the b-axis and c{sub 0} = 8.691(1) {angstrom}, K(c) = 111(3) GPa [{beta}(c) = 0.00300(8) GPa{sup -1}] for the c-axis, with K(a):K(b):K(c) = 1.41:1:2.26. The magnitude of the principal unit-strain coefficients, between 0.0001 GPa and 3.64 GPa, were calculated. The unit-strain ellipsoid is oriented with {epsilon}{sub 1}{parallel}b, {epsilon}{sub 2} and {epsilon}{sub 3} lying on the (0 1 0) plane with {epsilon}{sub 3} {angle} a = 115.1(3){sup o} and |{epsilon}{sub 1}|>|{epsilon}{sub 2}|>|{epsilon}{sub 3}||. The structural refinements performed at high-P allow to explain the reasons of the elastic anisotropy. The cooperative rotation of the tetrahedra increase the ellipticity of the channel systems, maintaining the original elliptical configuration (without any 'inversion' in ellipticity).},
doi = {10.1016/j.micromeso.2007.01.031},
journal = {Microporous and Mesoporous Materials},
number = 3,
volume = 105,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}
  • The elastic behaviour and the pressure (P) induced structural evolution of Na6Cs2Ga6Ge6O24 Ge(OH)6, a synthetic compound isotypic with cancrinite (CAN topology), have been investigated up to 5.01(5) GPa by means of in situ X-ray synchrotron powder diffraction with a diamond anvil cell and using a nominally penetrating hydrous P-transmitting medium (methanol:ethanol:water = 16:3:1). No evidence of phase-transition was observed within the P-range investigated.
  • No abstract prepared.
  • The high-pressure elastic behavior of a synthetic zeolite mordenite, Na{sub 6}Al{sub 6.02}Si{sub 42.02}O{sub 96}{center_dot}19H{sub 2}O [a=18.131(2), b=20.507(2), c=7.5221(5) Angstroms, space group Cmc2{sub 1}], has been investigated by means of in situ synchrotron X-ray powder diffraction up to 5.68 GPa. No phase transition has been observed within the pressure range investigated. Axial and volume bulk moduli have been calculated using a truncated second-order Birch-Murnaghan equation-of-state (II-BM-EoS). The refined elastic parameters are: V{sub 0}=2801(11) Angstroms{sup 3}, K{sub T0}= 41(2) GPa for the unit-cell volume; a 0=18.138(32) Angstroms, K {sub T0}(a)=70(8) GPa for the a-axis; b 0=20.517(35) Angstroms, K{sub T0}(b)=29(2) GPa for themore » b-axis and c 0=7.531(5) Angstroms, K {sub T0}(c)=38(1) GPa for the c-axis [K {sub T0}(a): K {sub T0}(b): K {sub T0} (c)=2.41:1.00:1.31]. Axial and volume Eulerian finite strain versus 'normalized stress' plots (fe-Fe plot) show an almost linear trend and the weighted linear regression through the data points yields the following intercept values: Fe(0)=39(4) GPa for V; Fe {sub a} (0)=65(18) GPa for a; Fe {sub b} (0)=28(3) GPa for b; Fe {sub c} (0)=38(2) GPa for c. The magnitudes of the principal Lagrangian unit-strain coefficients, between 0.47 GPa (the lowest HP-data point) and each measured P>0.47 GPa, were calculated. The unit-strain ellipsoid is oriented with {var_epsilon}{sub 1} || b, {var_epsilon}{sub 2} || c, {var_epsilon}{sub 3} || a and |{var_epsilon}{sub 1}|> |{var_epsilon}{sub 2}|> |{var_epsilon}{sub 3}|. Between 0.47 and 5.68 GPa the relationship between the unit-strain coefficient is {var_epsilon}{sub 1}: {var_epsilon}{sub 2}: {var_epsilon}{sub 3}=2.16:1.81:1.00. The reasons of the elastic anisotropy are discussed.« less
  • No abstract prepared.
  • High-resolution nuclear magnetic resonance (NMR) spectra and synchrotron x-ray powder diffraction data have been obtained from a well-crystallized highly dealuminated sample of the zeolite ZSM-11. The Rietveld profile technique has been applied to the synchrotron data to give the first detailed refinement of the idealized structure derived ten years ago by distance least-squares modeling methods (G. T. Kokotailo, P. Chu, S. L. Lawton, and W. M. Meier, Nature 275, 119 (1078)), which involves 54 variable atomic positional parameters. The structure is tetragonal (a = 20.065 A, c = 13.408 A at 25 /sup 0/C) and consistent with the previously reportedmore » tetragonal space group I4-barm2, but the NMR spectra indicate local deviations from this symmetry that disappear at 100 /sup 0/C.ion« less