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DOE OSTI · 2998822

A low-temperature, one-step synthesis for monazite can transform monazite into a readily usable advanced nuclear waste form

Zhoujin, Yunping [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000333073030)·Tisdale, Hunter B. [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000286693674)·Keerthisinghe, Navindra [Univ. of South Carolina, Columbia, SC (United States)] (ORCID:0000000331558456)·Morrison, Gregory [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000196749224)·Smith, Mark D. [Univ. of South Carolina, Columbia, SC (United States)] (ORCID:0000000169777131)·Hadermann, Joke [Univ. of Antwerp (Belgium)] (ORCID:0000000217562566)·Besmann, Theodore M. [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000155980550)·Amoroso, Jake [Savannah River National Laboratory (SRNL), Aiken, SC (United States)]·Loye, Hans-Conrad zur [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials; Savannah River National Laboratory (SRNL), Aiken, SC (United States)] (ORCID:0000000173519098)
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Abstract

It has been demonstrated that monazite-type materials are excellent candidates for nuclear waste forms, and hence, their facile synthesis is of great importance for the needed sequestration of existing nuclear waste. The synthesis of monazite, LaPO 4 , requires inconveniently high temperatures near 1000°C and generally involves the conversion of the presynthesized rhabdophane, LaPO 4 •nH 2 O, to the LaPO 4 monazite phase. During this structure transformation, the rhabdophane converts irreversibly to the thermodynamically stable monoclinic monazite structure. A low-temperature (185° to 260°C) mild hydrothermal acid-promoted synthesis of monazite is described that can both transform presynthesized rhabdophane or assemble reagents to the monoclinic monazite structure. The pH dependence of this reaction is detailed, and its applicability to the LnPO 4 (Ln = La, Ce, Pr, Nd, Sm-Gd), Ca 0.5 Th 0.5 PO 4 , and Sr 0.5 Th 0.5 PO 4 systems is discussed. The crystal growth of Ca 0.5 Th 0.5 PO 4 and Sr 0.5 Th 0.5 PO 4 is described, and their crystal structures were reported. In situ x-ray diffraction studies, performed as a function of temperature, provide insight into the structure transformation process.

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BiogeochemistryHydrothermal synthesisMonazite depositsNeodymium alloysPhosphatesSamarium alloysX ray diffraction analysis

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Zhoujin, Yunping [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000333073030), Tisdale, Hunter B. [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000286693674), Keerthisinghe, Navindra [Univ. of South Carolina, Columbia, SC (United States)] (ORCID:0000000331558456), Morrison, Gregory [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000196749224), Smith, Mark D. [Univ. of South Carolina, Columbia, SC (United States)] (ORCID:0000000169777131), Hadermann, Joke [Univ. of Antwerp (Belgium)] (ORCID:0000000217562566), Besmann, Theodore M. [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials] (ORCID:0000000155980550), Amoroso, Jake [Savannah River National Laboratory (SRNL), Aiken, SC (United States)], Loye, Hans-Conrad zur [Univ. of South Carolina, Columbia, SC (United States). Center for Hierarchical Waste Form Materials; Savannah River National Laboratory (SRNL), Aiken, SC (United States)] (ORCID:0000000173519098). 2025-03-21. A low-temperature, one-step synthesis for monazite can transform monazite into a readily usable advanced nuclear waste form. https://doi.org/10.1126/sciadv.adt3518

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