Structure and thermodynamics of calcium rare earth silicate oxyapatites, Ca2RE8(SiO4)6O2 (RE = Pr, Tb, Ho, Tm)

Strzelecki, Andrew C.; Ren, Yang; Chong, Saehwa; Riley, Brian J.; Xu, Hongwu; McCloy, John S.; Guo, Xiaofeng

doi:10.1007/s00269-022-01187-5

Structure and thermodynamics of calcium rare earth silicate oxyapatites, Ca₂RE₈(SiO₄)₆O₂ (RE = Pr, Tb, Ho, Tm)

Journal Article · 03 May 2022 · Physics and Chemistry of Minerals

DOI:https://doi.org/10.1007/s00269-022-01187-5· OSTI ID:1872438

Strzelecki, Andrew C. ^[1]; Ren, Yang ^[2]; Chong, Saehwa ^[3]; Riley, Brian J. ^[3]; Xu, Hongwu ^[4]; McCloy, John S. ^[5]; ^[6]

Washington State Univ., Pullman, WA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); City Univ. of Hong Kong, Kowloon (Hong Kong)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Arizona State Univ., Tempe, AZ (United States)
Washington State Univ., Pullman, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Washington State Univ., Pullman, WA (United States)

Calcium rare earth silicate oxyapatites, (Ca₂RE₈(SiO₄)₆O₂), are of interest as components of glass-ceramic nuclear waste forms. To assess their long-term behavior in a geologic repository, it is essential to determine their structure and thermodynamic stability at relevant conditions. Here, in this work, we performed detailed structural and thermodynamic investigations on Ca₂Pr₈(SiO₄)₆O₂, Ca₂Tb₈(SiO₄)₆O₂, Ca₂Ho₈(SiO₄)₆O₂, and Ca₂Tm₈(SiO₄)₆O₂ by high energy synchrotron powder X-ray diffraction combined with Rietveld analysis and high temperature oxide melt drop solution calorimetry. Enthalpies of formation from constituent oxides (ΔH_f,ox) were determined to be -765.1 ± 22.8 kJ/mol for Ca₂Pr₈(SiO₄)₆O₂; -638.9 ± 20.5 kJ/mol for Ca₂Tb₈(SiO₄)₆O₂; -643.3 ± 10.3 kJ/mol for Ca₂Ho₈(SiO₄)₆O₂; and -403.2 ± 5.1 kJ/mol for Ca₂Tm₈(SiO₄)₆O₂. These thermodynamic parameters were used in assessing the thermochemical stability of these phases in the presence of water vapor from room temperature to 600 K, as encountered in the subsurface environments of a geological repository.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-76RL01830; NE0008582; NE0008431; 89233218CNA000001; AC02-06CH11357

OSTI ID:: 1872438

Report Number(s):: PNNL-SA-167132

Journal Information:: Physics and Chemistry of Minerals, Vol. 49, Issue 5; ISSN 0342-1791

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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