Study of the chemical durability of a hollandite mineral leached in both static and dynamic conditions

Year 2019, , 85 - 92, 30.06.2019

Fairouz Aouchiche Nour-el-hayet Kamel , Dalila Moudir Yasmina Mouheb Soumia Kamariz

https://doi.org/10.35208/ert.453417

Abstract

Hollandite is a ceramic
used for the confinement of cesium. In this study, we synthesized a hollandite
of chemical formula: K_0.28Ba_0.76Ti_7.10Cu_0.9O₁₆,
where K simulates cesium. This new formulation of a copper-containing hollandite
was synthesized by a double calcination; the first one at 950°C during 18 h,
and the second one at 1000°C during 6 h. The mineral was identified by X-ray
diffraction. Various leaching tests are employed in order to assess the
chemical durability of this mineral. The static test MCC1 gave elemental leaching
rates of: 7.097 10^-5 g cm^-2 d^-1 for Cu, 5.592
10^-7 g cm^-2 d^-1 for Ti and 4.630 10^-6
g cm^-2 d^-1 for Ba, after 42 days. This corresponds to
dissolved elements percentages of: 5.7% Cu, 0.0007% Ti and 0.2% Ba. The
equivalent amount of dissolved K is 0.0029%. A static test in the presence of a
clay barrier, gave the best leaching rates (at 42^nd day, NR<3.704
10^-7 g cm^-2 d^-1 of Cu, and <1.11 10^-9
g cm^-2 d^-1 of Ti and <3.67 10^-9 g cm^-2
d^-1 of Ba). This corresponds to 0.030% of Cu, 10^-6 % of
Ti and 0.002 % of Ba, and about 0.002% of K. In MCC5 dynamic test, the leaching
rates of Cu, Ti and Ba reached 2 10^-6, 1,468 10^-7, and
1.084 10^-5 g cm^-2 d^-1, respectively,
corresponding to 0.028% Cu, 0.0003% Ti, and 0.082% Ba, after seven days. The
estimated K leaching rate is 3.613 10^-6 g cm^-2 d^-1,
ie 0.082% K dissolved in the leachate. There is no passivation layer formation.
The MCC5 test is considered as a dissolution test.

Keywords

Hollandite, Cesium, Leaching, MCC1, MCC5

References

• Reference1 A.E. Ringwood, V.M. Oversby, S.E. Kesson, W. Sinclair, N. Ware, W. Hibberson, and A. Major, “immobilization of high-level nuclear reactor wastes in Synroc: a current appraisal”, Nuclear and Chemical Waste Management, vol. 2, pp.287-305, Oct. 1981.
• Reference2 Aubin-Chevaldonnet, “Synthèse, caractérisation et étude du comportement sous irradiation électronique de matrices de type hollandite destinées au confinement du césium radioactif”, thesis, Lab. Chimie Appliquée Etat Solid., Université Pierre et Marie Curie − PARIS VI, Paris, Nov. 2004.
• Reference3 A. Byström, and A. M. Byström, “The crystal structure of hollandite, the related manganese oxide minerals and α-MnO2”, Acta Cryst., vol. 3, pp. 146-154, Mar.1950.
• Reference4 R.W. Cheary, “An analysis of the structural characteristics of hollandite compounds”, Acta Cryst., vol. B42, pp. 229-236, June. 1986.
• Reference5 D.S. Filimonov, Z.-K. Liu, and C.A. Randall, “Synthesis and thermal stability of a new barium polytitanate compound, Ba1.054Ti0.946O2.946”, Mater. Res. Bull, vol. 37, pp. 467-473, March. 2002.
• Reference6 J.E. Post, R.B. Von Dreele, and P. R. Buseck, “Symmetry and cation displacements in hollandites: structure refinements of hollandite, cryptomelane and priderite”, Acta Crys, vol. B38, pp. 1056-1065, April 1982.
• Reference7 J. Vicat, E. Fanchon, P. Strobel, and D.T. Qui, “The structure of K1.33Mn8O16 and cation ordering in hollandite-type structures”, Acta Cryst, vol. B42, pp. 162-167, Apr. 1986.
• Reference8 J. Zhang, and C.W. Burnham, “Hollandite-type phases: Geometric consideration of unit-cell size and symmetry”, Am. Mineral, vol. 79, pp. 168-174, Jan.-Feb. 1994.
• Reference9 F. Angeli, P. McGlinn, and P. Frugier, “Chemical durability of hollandite ceramic for conditioning cesium”, J. Nucl. Mater, vol 380, pp. 59–69, Oct. 2008.
• Reference10 V. Aubin-Chevaldonnet, D. Caurant, A. Dannoux, D. Gourier, T. Charpentier, L. Mazerolles, and T. Advocat, “Preparation and characterization of (Ba,Cs)(M,Ti)8O16 (M = Al3+, Fe3+, Ga3+, Cr3+, Sc3+, Mg2+) hollandite ceramics developed for radioactive cesium immobilization”, J. Nucl. Mater, vol 366, pp. 137-160, June 2007.
• Reference11 A.Y. Leinekugel-le-Cocq, P. Deniard, S. Jobic, R. Cerny, F. Bart, and H. Emerich, “Synthesis and characterization of hollandite-type material intended for the specific containment of radioactive cesium”, J. Solid State Chem, vol 179, pp. 3196-3208, Oct. 2006.
• Reference12 V. Aubin-Chevaldonnet, P. Deniard, M. Evain, A.Y. Leinekugelle-Cocq-Errien, S. Jobic, D. Caurant, V. Petricek, and T. Advocat, “Incommensurate modulations in a hollandite phase Ba-x(Al,Fe)2xTi8-2xO16 intended for the storage of radioactive wastes: a (3+1) dimension structure determination”, Z. Kristallogr, vol 222, pp. 383-390, Jul. 2007.
• Reference13 M.L. Carter, E.R. Vance, D.R.G. Mitchell, J.V. Hanna, Z. Zhang, and E. Loi, “Fabrication, characterization, and leach testing of hollandite, (Ba,Cs)(Al,Ti)2Ti6O16”, J. Mater. Res, vol. 17, pp. 2578-2589, Oct. 2002.
• Reference14 E. Bart, G. Leturcq, and H. Rabiller, Iron-substituted Barium Hollandite Ceramics for Cesium Immobilization, Environnemental Issues and Waste Management Technologies in the Ceramic and Nuclear Industries IX, Part I: Ceramics for Waste or Nuclear Applications, vol. 155, pp. 11-20, April 2012.
• Reference15 M.L. Carter, E.R. Vance, G.R. Lumpkin, and G.R. Loi, “Aqueous dissolution of Rb-bearing hollandite and Synroc-C at 90 °C”, Mater. Res. Soc. Sym. Proc, vol. 663, pp. 381-388, Aug. 2000.
• Reference16 H. Rabiller, F. Bart, F.Miserque, G. Leturcq, D. Rigaud, Leaching behavior of hollandite ceramics for cesium immobilization, ATALANTE, Nimes, Juin 2004.
• Reference17 S.E. Kesson, and T. J. White, “Radius ratio tolerance factors and the stability of hollandites”,J. Solid State Chem, vol. 63, pp. 122-125, Jun 1986.
• Reference18 Philips X’Pert High Score Package, Diffraction Data CD-ROM, International Center for Diffraction Data, Newtown Square, PA, 2004.
• Reference19 D.M. Strachan, “Glass dissolution: Testing and modelling for long-term behavior”, Journal of Nuclear Materials, vol.298, pp. 69-77, Sep 2001.
• Reference20 JCPDS, PCPDFwin. Diffraction Data CD-ROM. International Center for Diffraction Data, Newtown Square, PA, 2004.
• Reference21 C. Fillet, and Nicolas Dacheux, Matrices céramiques pour conditionnements spécifiques, Dossier Techniques de l’Ingénieur bn3770, Ed. Techniques de l’Ingénieur, Paris, France, 2011.
• Reference22 G. Leturcq, P. Mcglinn, C. Barbé, M.G. Blackford, and K.S. Finnie, “Aqueous alteration of nearly pure Nd-doped zirconolite (Ca0.8Nd0.2ZrTi1.8Al0.2O7), a passivating layer control”, Applied geochemistry, vol. 20, pp. 899-906, May 2005.
• Reference23 G. Leturcq, T. Advocat, K. Hart, G. Berger, J. Lacombe, and A. Bonnetier, “Solubility study of Ti,Zr-based ceramics designed to immobilize long-lived radionuclides”, American Mineralogist, vol. 86, pp. 871–880, July 2001.
• Reference24 D. Bregiroux, “Synthèse par voie solide et frittage de céramiques à structure monazite”, thesis, faculté des sciences et techniques, Université de Limoges, France, Novembre 2005
• Reference25 N. Kamel, H. Ait amar, and S. Telmoune, “Study of the dissolution of three synthetic minerals: zirconolite, y-britholite and mono-silicate fluorapatite”, Annales de chimie et science des matériaux,vol. 32, pp: 547-559, March 2007.
• Reference26 Shabalin В., Titov Y., Zlobenko B., Bugera S., Ferric titanous hollandite analogues — Matrices for immobilization of Cs-containing radioactive waste: Synthesis and properties, Mineralogy, vol. 35, pp. 12-18, Nov. 2014.
• Reference27 T. Suzuki-Muresan , J. Vandenborre, A. Abdelouas, B. Grambow, and S. Utsunomiya, “Studies of (Cs,Ba)-hollandite dissolution under gamma irradiation at 95 °C and at pH 2.5, 4.4 and 8.6”, Journal of Nuclear Materials, Vol. 419, pp. 281–290, Dec 2011.
• Reference28 A.G. Solomah, P.G. Richardson, and A.K. McIlwain, “Phase identification, microstructural characterization, phase microanalyses and leaching performance evaluation of SYNROC-FA crystalline ceramic waste form”, Journal of Nuclear Materials, Vol. 148, pp. 157-165, Apr 1987.
• Reference29 S.P. Kumar, and B. Gopal, “Synthesis and leachability study of a new cesium immobilized langbeinite phosphate: KCsFeZrP3O12”, Journal of Alloys and Compounds, Vol. 615, pp. 419-423, Dec 2014.
• Reference30 Z. Klika, Z. Weiss, M. Mellini, and M. Drabek, “Water leaching of cesium from selected cesium mineral analogues”, Applied Geochemistry, Vol. 21, pp. 405–418, March 2006.