High-Temperature Thermodynamics of Cerium Silicates, A-Ce2Si2O7, and Ce4.67(SiO4)3O

Strzelecki, Andrew C.; Kriegsman, Kyle; Estevenon, Paul; Goncharov, Vitaliy; Bai, Jianming; Szenknect, Stephanie; Mesbah, Adel; Wu, Di; McCloy, John S.; Dacheux, Nicolas; Guo, Xiaofeng

doi:10.1021/acsearthspacechem.0c00231

Title: High-Temperature Thermodynamics of Cerium Silicates, A-Ce₂Si₂O₇, and Ce_4.67(SiO₄)₃O

Journal Article · Fri Oct 30 00:00:00 EDT 2020 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.0c00231· OSTI ID:1686245

Strzelecki, Andrew C. ^[1]; Kriegsman, Kyle ^[1]; Estevenon, Paul ^[2]; Goncharov, Vitaliy ^[1];

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Washington State Univ., Pullman, WA (United States). Alexandra Navrotsky Inst. for Experimental Thermodynamics
Univ. Montpellier, Marcoule (France). Inst. for the Separation Chemistry in Marcoule (ICSM), CNRS, CEA, ENSCM, DES, ISEC, and DMRC
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Univ. Montpellier, Marcoule (France). Inst. for the Separation Chemistry in Marcoule (ICSM), CNRS, CEA, and ENSCM
Washington State Univ., Pullman, WA (United States). Alexandra Navrotsky Inst. for Experimental Thermodynamics and Gene and Linda Voiland School of Chemical Engineering and Bioengineering
Washington State Univ., Pullman, WA (United States)

Lanthanide disilicates and oxyapatites have potential roles in high temperature applications as thermal (TBC) and environmental barrier coatings (EBC), or possible alteration phases in geological nuclear waste repositories. However, those Ce³⁺-bearing silicates have only been limitedly studied. In this work, we performed detailed structural and thermodynamic investigations on A-Ce₂Si₂O₇ (tetragonal, P4₁) and Ce_4.67(SiO₄)₃O (hexagonal, P6₃/m). The high temperature structural behaviors and coefficients of thermal expansion were determined by in situ high temperature synchrotron X-ray diffraction (HT-XRD) implemented with Rietveld analysis and thermogravimetric analysis coupled with differential scanning calorimetry (TGA-DSC). A-Ce₂Si₂O₇ was found to be stable in N₂ and air up to ~1483 K with anisotropic thermal expansion along the a and c axes (α_a= 12.3 × 10^-6K^-1 and α_c = 12.4 × 10^-6 K^-1). Ce_4.67(SiO₄)₃O had a slow partial oxidation between 533 K and 873 K to a new nonstoichiometric phase Ce³⁺_{_1.67-}xCe4⁺_xCe³⁺₃(SiO₄)₃O_1+0.5x, followed by a thermal decomposition to CeO₂ and SiO₂ at ~1000 K in air. By using high temperature oxide melt solution calorimetry at 973 K with lead borate as the solvent, the standard enthalpy of formation was determined for A-Ce₂Si₂O₇ (-3825.1 ± 6.0 kJ/mol) and Ce_4.67(SiO₄)₃O (-7391.3 ± 9.5 kJ/mol). Finally, these thermodynamic parameters were compared with those of CeO₂, CeSiO₄, and other silicate oxyapatites for examining their chemical stability in high temperature environments relevant for aeronautical applications, mineral formation, and nuclear fuel cycle.

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Research Organization:: Washington State Univ., Pullman, WA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC); Washington State University

Grant/Contract Number:: NE0008582; NE0008689; SC0012704

OSTI ID:: 1686245

Alternate ID(s):: OSTI ID: 1762749

Report Number(s):: BNL-220795-2021-JAAM; DE-NE0008689; TRN: US2204118

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

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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