Energetics of Salt-Bearing Sodalites, Na8Al6Si6O24X2 (X = SO4, ReO4, Cl, I): A Treatment Option for Pertechnetate-Enriched Nuclear Waste Streams

Lilova, Kristina; Pierce, Eric M.; Wu, Lili; Jubb, Aaron M.; Subramani, Tamilarasan; Navrotsky, Alexandra

doi:10.1021/acsearthspacechem.0c00244

Energetics of Salt-Bearing Sodalites, Na₈Al₆Si₆O₂₄X₂ (X = SO₄, ReO₄, Cl, I): A Treatment Option for Pertechnetate-Enriched Nuclear Waste Streams

Journal Article · Tue Nov 03 23:00:00 EST 2020 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.0c00244· OSTI ID:1782049

Lilova, Kristina ^[1]; ^[2]; Wu, Lili ^[3]; ^[2]; ^[1]; ^[1]

Arizona State Univ., Tempe, AZ (United States). Navrotsky Eyring Center for Materials of the Universe
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of California, Davis, CA (United States). Peter A. Rock Thermochemistry Laboratory and NEAT ORU

An alternative option for treating anion-enriched reprocessed nuclear waste streams is to immobilize technetium-99 (⁹⁹Tc, β = 293.7 keV, t_1/2 = 2.1 × 10⁵ years) and other anions in micro- and mesoporous materials. Here we determine the thermodynamic stability of anion bearing sodalites, Na₈Al₆Si₆O₂₄X₂ (X = SO₄, ReO₄, Cl, I), to improve our understanding of the driving forces that control framework assembly using high temperature oxide melt solution calorimetry. Raman and FTIR spectroscopy illustrate a strong dependence for vibrational features on anion size and enabled the development of a linear model that predicted the vibrational features for numerous anion bearing sodalites to within ±20 cm^–1 (i.e., OH, F, Br, ClO₄, NO₃, and MnO₄). The largest negative enthalpy of formation from elements and the lack of structural water demonstrate that the perrhenate sodalite (Na₈Al₆Si₆O₂₄[ReO₄]₂), a chemical analogue for pertechnetate sodalite (Na₈Al₆Si₆O₂₄[TcO₄]₂), is more thermodynamically stable than all other anion bearing sodalites evaluated. The enthalpies of the reaction between nepheline and the sodium salt, which provides the guest anion species, was negative only for the ReO₄ and NO₃ bearing sodalites. Overall, we report for the first time the enthalpy of the ion exchange reactions for different anion bearing sodalites relative to the perrhenate sodalite, which is a key step in gaining the ability to tune sodalite material properties and structure during treatment and the immobilization of ⁹⁹Tc in the presence of competing anions.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1782049

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 11 Vol. 4; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (46)

Progress and new directions in high temperature calorimetry Navrotsky, Alexandra Physics and Chemistry of Minerals, Vol. 2, Issue 1-2 https://doi.org/10.1007/BF00307526	journal	January 1977
Thermochemistry of carbonate-pyroxene equilibria Chai, Liang; Navrotsky, Alexandra Contributions to Mineralogy and Petrology, Vol. 114, Issue 2 https://doi.org/10.1007/BF00307751	journal	June 1993
The sodalite group of minerals Taylor, D. Contributions to Mineralogy and Petrology, Vol. 16, Issue 2 https://doi.org/10.1007/BF00372796	journal	January 1967
Cell parameter correlations in the aluminosilicate-sodalites Taylor, Derek Contributions to Mineralogy and Petrology, Vol. 51, Issue 1 https://doi.org/10.1007/BF00403511	journal	January 1975
Thermodynamic properties of synthetic calcium-free carbonate cancrinite Kurdakova, S. V.; Grishchenko, R. O.; Druzhinina, A. I. Physics and Chemistry of Minerals, Vol. 41, Issue 1 https://doi.org/10.1007/s00269-013-0625-1	journal	September 2013
Progress and new directions in high temperature calorimetry revisited Navrotsky, Alexandra Physics and Chemistry of Minerals, Vol. 24, Issue 3 https://doi.org/10.1007/s002690050035	journal	April 1997
Thermochemistry of glasses and liquids in the systems CaMgSi2O6-CaAl2Si2O8-NaAlSi3O8, SiO2-CaAl2Si2O8-NaAlSi3O8 and SiO2-Al2O3-CaO-Na2O Navrotsky, A.; Hon, R.; Weill, D. F. Geochimica et Cosmochimica Acta, Vol. 44, Issue 10 https://doi.org/10.1016/0016-7037(80)90107-6	journal	October 1980
Synthesis and structures of M8[ALSiO4]6·(XO4)2, M = Na, Li, K; X = Cl, Mn Sodalites Brenchley, Matthew E.; Weller, Mark T. Zeolites, Vol. 14, Issue 8 https://doi.org/10.1016/0144-2449(94)90125-2	journal	November 1994
Infrared spectra of anhydrous members of the sodalite family Henderson, C. M. B.; Taylor, D. Spectrochimica Acta Part A: Molecular Spectroscopy, Vol. 33, Issue 3-4 https://doi.org/10.1016/0584-8539(77)80032-9	journal	January 1977
High-pressure transformations in NaAlSiO4 and thermodynamic properties of jadeite, nepheline, and calcium ferrite-type phase Akaogi, M.; Tanaka, A.; Kobayashi, M. Physics of the Earth and Planetary Interiors, Vol. 130, Issue 1-2 https://doi.org/10.1016/S0031-9201(01)00305-3	journal	March 2002
The relation between zeolite framework structure and vibrational spectra de Man, A. J. M.; van Santen, R. A. Zeolites, Vol. 12, Issue 3 https://doi.org/10.1016/S0144-2449(05)80295-7	journal	March 1992
Experimental determination of the speciation, partitioning, and release of perrhenate as a chemical surrogate for pertechnetate from a sodalite-bearing multiphase ceramic waste form Pierce, E. M.; Lukens, W. W.; Fitts, J. P. Applied Geochemistry, Vol. 42 https://doi.org/10.1016/j.apgeochem.2013.12.017	journal	March 2014
Evidence of technetium and iodine release from a sodalite-bearing ceramic waste form Neeway, James J.; Qafoku, Nikolla P.; Williams, Benjamin D. Applied Geochemistry, Vol. 66 https://doi.org/10.1016/j.apgeochem.2015.12.017	journal	March 2016
FactSage thermochemical software and databases — recent developments Bale, C. W.; Bélisle, E.; Chartrand, P. Calphad, Vol. 33, Issue 2 https://doi.org/10.1016/j.calphad.2008.09.009	journal	June 2009
Perrhenate incorporation into binary mixed sodalites: The role of anion size and implications for technetium-99 sequestration Dickson, Johnbull O.; Harsh, James B.; Lukens, Wayne W. Chemical Geology, Vol. 395 https://doi.org/10.1016/j.chemgeo.2014.12.009	journal	February 2015
Low temperature heat capacity and thermodynamic functions of anion bearing sodalites Na8Al6Si6O24X2 (X = SO4, ReO4, Cl, I) Schliesser, Jacob; Lilova, Kristina; Pierce, Eric M. The Journal of Chemical Thermodynamics, Vol. 114 https://doi.org/10.1016/j.jct.2017.05.035	journal	November 2017
Performance of the Fluidized Bed Steam Reforming product under hydraulically unsaturated conditions Neeway, James J.; Qafoku, Nikolla P.; Williams, Benjamin D. Journal of Environmental Radioactivity, Vol. 131 https://doi.org/10.1016/j.jenvrad.2013.10.008	journal	May 2014
Structural characterization of pure Na-nephelines synthesized by zeolite conversion route Dimitrijevic, Radovan; Dondur, Vera; Vulic, Predrag Journal of Physics and Chemistry of Solids, Vol. 65, Issue 10 https://doi.org/10.1016/j.jpcs.2004.03.005	journal	October 2004
An international initiative on long-term behavior of high-level nuclear waste glass Gin, S.; Abdelouas, A.; Criscenti, L. J. Materials Today, Vol. 16, Issue 6 https://doi.org/10.1016/j.mattod.2013.06.008	journal	June 2013
Formation and hydration enthalpies of the hydrosodalite family of materials Moloy, Eric C.; Liu, Qingyuan; Navrotsky, Alexandra Microporous and Mesoporous Materials, Vol. 88, Issue 1-3 https://doi.org/10.1016/j.micromeso.2005.09.020	journal	January 2006
Synthesis and structure of perrhenate sodalite Mattigod, Shas V.; Peter McGrail, B.; McCready, David E. Microporous and Mesoporous Materials, Vol. 91, Issue 1-3 https://doi.org/10.1016/j.micromeso.2005.11.025	journal	April 2006
Energetics of cancrinite: Effect of salt inclusion Liu, Qingyuan; Navrotsky, Alexandra; Jove-Colon, Carlos F. Microporous and Mesoporous Materials, Vol. 98, Issue 1-3 https://doi.org/10.1016/j.micromeso.2006.09.008	journal	January 2007
Immobilization and exchange of perrhenate in sodalite and cancrinite Dickson, Johnbull O.; Harsh, James B.; Flury, Markus Microporous and Mesoporous Materials, Vol. 214 https://doi.org/10.1016/j.micromeso.2015.05.011	journal	September 2015
The influence of the long-range order on the vibrational spectra of structures based on sodalite cage Mikuła, A.; Król, M.; Koleżyński, A. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 144 https://doi.org/10.1016/j.saa.2015.02.073	journal	June 2015
On art and science in curve-fitting vibrational spectra Meier, Robert J. Vibrational Spectroscopy, Vol. 39, Issue 2 https://doi.org/10.1016/j.vibspec.2005.03.003	journal	October 2005
Structure and Thermochemistry of Perrhenate Sodalite and Mixed Guest Perrhenate/Pertechnetate Sodalite Pierce, Eric M.; Lilova, Kristina; Missimer, David M. Environmental Science & Technology, Vol. 51, Issue 2 https://doi.org/10.1021/acs.est.6b01879	journal	December 2016
Vibrational Spectroscopy of Sodalite: Theory and Experiments Mofrad, Amir Mehdi; Peixoto, Caio; Blumeyer, Jack The Journal of Physical Chemistry C, Vol. 122, Issue 43 https://doi.org/10.1021/acs.jpcc.8b07633	journal	September 2018
Energetics of Mesoporous Silica: Investigation into Pore Size and Symmetry Trofymluk, Olga; Levchenko, Andrey A.; Tolbert, Sarah H. Chemistry of Materials, Vol. 17, Issue 14 https://doi.org/10.1021/cm050366g	journal	July 2005
Ionic radii in aqueous solutions Marcus, Yizhak Chemical Reviews, Vol. 88, Issue 8 https://doi.org/10.1021/cr00090a003	journal	December 1988
Competitive Incorporation of Perrhenate and Nitrate into Sodalite Dickson, Johnbull O.; Harsh, James B.; Flury, Markus Environmental Science & Technology, Vol. 48, Issue 21 https://doi.org/10.1021/es503156v	journal	October 2014
Computer simulation and interpretation of the infrared and Raman spectra of sodalite frameworks Creighton, J. A.; Deckman, H. W.; Newsam, J. M. The Journal of Physical Chemistry, Vol. 98, Issue 2 https://doi.org/10.1021/j100053a018	journal	January 1994
Fourier transform far-infrared spectroscopic study of cation and anion dynamics in M,X sodalites, where M = lithium(1+), sodium(1+), potassium(1+), rubidium(1+), cadmium(2+); X = chloride, bromide, iodide, perchlorate, hydroxide Godber, John; Ozin, Geoffrey A. The Journal of Physical Chemistry, Vol. 92, Issue 17 https://doi.org/10.1021/j100328a032	journal	August 1988
Topotactic Transformations of Sodalite Cages: Synthesis and NMR Study of Mixed Salt-Free and Salt-Bearing Sodalites Trill, Henning; Eckert, Hellmut; Srdanov, Vojislav I. Journal of the American Chemical Society, Vol. 124, Issue 28 https://doi.org/10.1021/ja012765s	journal	July 2002
Mixed Halide Sodalite Solid Solution Systems. Hydrothermal Synthesis and Structural Characterization by Solid State NMR Trill, Henning; Eckert, Hellmut; Srdanov, Vojislav I. The Journal of Physical Chemistry B, Vol. 107, Issue 34 https://doi.org/10.1021/jp0224618	journal	August 2003
Structure and IR Vibrational Spectra of Na ₈ [AlSiO ₄ ] ₆ (BH ₄ ) ₂ : Comparison of Theory and Experiment Schneider, Alexander G.; Bredow, Thomas; Schomborg, Lars The Journal of Physical Chemistry A, Vol. 118, Issue 34 https://doi.org/10.1021/jp503027h	journal	August 2014
Thermodynamics of solvation of ions. Part 5.—Gibbs free energy of hydration at 298.15 K Marcus, Yizhak J. Chem. Soc., Faraday Trans., Vol. 87, Issue 18 https://doi.org/10.1039/FT9918702995	journal	January 1991
Structural trends in the sodalite family Johnson, Geoffrey M.; Mead, Philip J.; Weller, Mark T. Physical Chemistry Chemical Physics, Vol. 1, Issue 15 https://doi.org/10.1039/a903373d	journal	January 1999
The Raman spectrum and analysis of phonon modes in sodalite Ariai, J.; Smith, S. R. P. Journal of Physics C: Solid State Physics, Vol. 14, Issue 8 https://doi.org/10.1088/0022-3719/14/8/015	journal	March 1981
Nepheline Solid Solution in the System NaAISiO4-KAISiO4-SiO2 Hamilton, D. L.; Mackenzie, W. S. Journal of Petrology, Vol. 1, Issue 1 https://doi.org/10.1093/petrology/1.1.56	journal	February 1960
Progress and New Directions in Calorimetry: A 2014 Perspective Navrotsky, Alexandra Journal of the American Ceramic Society, Vol. 97, Issue 11 https://doi.org/10.1111/jace.13278	journal	October 2014
Structure and properties of tecto-gallosilicates II. Sodium chloride, bromide and iodide sodalites Gesing, Thorsten M. Zeitschrift für Kristallographie, Vol. 222, Issue 6 https://doi.org/10.1524/zkri.2007.222.6.289	journal	January 2007
Symmetry relationships of sodalite (SOD) – type crystal structures Fischer, Reinhard X.; Baur, W. H. Zeitschrift für Kristallographie, Vol. 224, Issue 4 https://doi.org/10.1524/zkri.2009.1147	journal	January 2009
The Crystal Chemistry of Nepheline Tait, K. T.; Sokolova, E.; Hawthorne, F. C. The Canadian Mineralogist, Vol. 41, Issue 1 https://doi.org/10.2113/gscanmin.41.1.61	journal	February 2003
Thermochemistry and phase equilibria in calcium zeolites Kiseleva, Irina; Navrotsky, Alexandra; Belitsky, Igor A. American Mineralogist, Vol. 81, Issue 5-6 https://doi.org/10.2138/am-1996-5-613	journal	June 1996
Thermochemical study of calcium zeolites—heulandite and stilbite Kiseleva, I.; Navrotsky, A.; Belitsky, I. American Mineralogist, Vol. 86, Issue 4 https://doi.org/10.2138/am-2001-0408	journal	April 2001
Crystal properties and energetics of synthetic kaolinite Fialips, Claire-Isabelle; Navrotsky, Alexandra; Petit, Sabine American Mineralogist, Vol. 86, Issue 3 https://doi.org/10.2138/am-2001-2-313	journal	March 2001

Similar Records

Structure and Thermochemistry of Perrhenate Sodalite and Mixed Guest Perrhenate/Pertechnetate Sodalite

Journal Article · Sun Dec 04 23:00:00 EST 2016 · Environmental Science and Technology · OSTI ID:1409615

Structure and Thermochemistry of Perrhenate Sodalite and Mixed Guest Perrhenate/Pertechnetate Sodalite

Journal Article · Sun Dec 04 23:00:00 EST 2016 · Environmental Science and Technology · OSTI ID:1340434

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
enthalpy of formation
ion exchange
perrhenate sodalite
radioactive waste
thermodynamics

Energetics of Salt-Bearing Sodalites, Na8Al6Si6O24X2 (X = SO4, ReO4, Cl, I): A Treatment Option for Pertechnetate-Enriched Nuclear Waste Streams

Citation Formats

References (46)

Similar Records

Related Subjects

Energetics of Salt-Bearing Sodalites, Na₈Al₆Si₆O₂₄X₂ (X = SO₄, ReO₄, Cl, I): A Treatment Option for Pertechnetate-Enriched Nuclear Waste Streams