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

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Abstract

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. 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 (∆Hf,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.

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Acknowledgements

This research was supported by the institutional funds from the Department of Chemistry at Washington State University (WSU). We also acknowledge the support by the U.S. Department of Energy (DOE), Office of Nuclear Energy, Grants No. DE-NE0008582 and DE-NE0008431. Research presented in this article was also supported by the Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory (LANL). LANL, an affirmative action/equal opportunity employer, is managed by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under contract 89233218CNA000001. Portions of this research were also supported by collaboration, services, and infrastructure through the Nuclear Science Center User Facility at (WSU), and the Alexandra Navrotsky Institute for Experimental Thermodynamics. Portions of this research used Beamline 11-ID-C (XSD-SRS) of the Advance Photon Source (APS), a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory (ANL) under Contract No. DE-AC02-06CH11357. The authors acknowledge partial financial support from the U.S. Department of Energy Office of Nuclear Energy (DOE-NE). The Pacific Northwest National Laboratory is operated by Battelle under Contract Number DE-AC05-76RL01830.

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Authors and Affiliations

  1. Department of Chemistry, Washington State University, Pullman, WA, 99164, USA

    Andrew C. Strzelecki, John S. McCloy & Xiaofeng Guo

  2. Alexandra Navrotsky Institute for Experimental Thermodynamics, Washington State University, Pullman, WA, 99164, USA

    Andrew C. Strzelecki & Xiaofeng Guo

  3. Materials Science and Engineering, Washington State University, Pullman, WA, 99164, USA

    Andrew C. Strzelecki, John S. McCloy & Xiaofeng Guo

  4. Earth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    Andrew C. Strzelecki & Hongwu Xu

  5. X-Ray Science Division and Structural Science, Advanced Photon Source, Argonne National Laboratory, Lemont, IL, 60438, USA

    Yang Ren

  6. Department of Physics, City University of Hong Kong, Kowloon, Hong Kong, China

    Yang Ren

  7. Pacific Northwest National Laboratory, Richland, WA, 99352, USA

    Saehwa Chong, Brian J. Riley & John S. McCloy

  8. School of Mechanical and Materials Engineering, Washington State University, Pullman, WA, 99164, USA

    John S. McCloy

  9. School of Molecular Sciences and Center for Materials of the Universe, Arizona State University, Tempe, AZ, 85287, USA

    Hongwu Xu

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Contributions

XG and JSM conceived the research. ACS performed high temperature drop solution oxide melt calorimetry. YR performed ambient synchrotron XRD. ACS analyzed and refined all the synchrotron XRD. Samples were prepared by SC and BJR and supplied by JSM. All authors participated in discussions, interpretation of the data and writing of the manuscripts.

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Strzelecki, A.C., Ren, Y., Chong, S. et al. Structure and thermodynamics of calcium rare earth silicate oxyapatites, Ca2RE8(SiO4)6O2 (RE = Pr, Tb, Ho, Tm). Phys Chem Minerals 49, 13 (2022). https://doi.org/10.1007/s00269-022-01187-5

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