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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, LaPO4, requires inconveniently high temperatures near 1000 degrees C and generally involves the conversion of the presynthesized rhabdophane, LaPO4 center dot nH2O, to the LaPO4 monazite phase. During this structure transformation, the rhabdophane converts irreversibly to the thermodynamically stable monoclinic monazite structure. A low-temperature (185 degrees to 260 degrees 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 LnPO4 (Ln = La, Ce, Pr, Nd, Sm-Gd), Ca0.5Th0.5PO4, and Sr0.5Th0.5PO4 systems is discussed. The crystal growth of Ca0.5Th0.5PO4 and Sr0.5Th0.5PO4 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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