Zirconolite is one of the most important matrix materials for nuclear waste immobilization.In this study,Sm was employed as the surrogate of trivalent actinides.Sm-doped zirconolite-rich waste forms were readily prepa...Zirconolite is one of the most important matrix materials for nuclear waste immobilization.In this study,Sm was employed as the surrogate of trivalent actinides.Sm-doped zirconolite-rich waste forms were readily prepared by combustion synthesis(CS)using CuO as the oxidant.Two different schemes with or without Al2O3 as the charge compensator were carried out simultaneously.The results demonstrate that Al2O3 addition results in complex phase composition.On the other hand,the samples without Al2O3 addition show desirable products of zirconolite and pyrochlore.The EDX analysis shows that Sm is concurrently incorporated into the Ca and Zr sites of zirconolite,which transforms to pyrochlore structure with high Sm2O3 contents.The aqueous durability of representative Sm-doped sample(Sm-0.6)was investigated.The 42 days normalized leaching rate of Sm is as low as 6.41×10-7 g/(m2 d),which exhibits high durability of Sm-doped sample.展开更多
Samarium（Sm） has been widely used in making aluminum（Al）-Sm magnet alloy materials. The research team for this study developed a molten salt electrolyte system which directly produces AI-Sm alloy to replace the en...Samarium（Sm） has been widely used in making aluminum（Al）-Sm magnet alloy materials. The research team for this study developed a molten salt electrolyte system which directly produces AI-Sm alloy to replace the energy intensive conventional distillation technology. In this study, molten melt density was measured and operation conditions were optimized to separate AI-Sm alloy product from the fluoride molten melt electrolysis media based on density differences, Archimedes＇ principle was applied to measure density for the basic molten fluoride system（BMFS： Na_3 AlF_6-AlF_3-LiF-MgF_2）electrolysis media in the temperature range from 905 to 1055 ℃.The impact of temperature（t） and the Al_2O_3 and Sm_2O_3 addition ratio（w_（（Al2O3））,w_（（Sm2O3）） in the basic fluoride system on molten melt density was examined. The fluoride molten melt density relationship was determined to be：ρ=3.11701-0.00802 w_（（Al2O3））＋0.027825 w_（（Sm2O3））-0.00117 t. The test results showed that molten density decreases with increase in temperature and Al_2O_3 addition ratio, and increases with the addition of Sm_2O_3, and/or Al_2O_3＋Sm_2O_3. The separation of Al-Sm（density 2.3 g/cm^3） product melt from the BMFS melt is achieved by controlling the BMFS density to less than 2.0 g/cm3. It is concluded that the optimal operation conditions to control the BMFS molten salt density to less than 2.0 g/cm^3 are：maintain addition of Al_2O_3＋Sm_2 O_3（w_（（Al2O3））＋w_（（Sm2O3））〈9% of Na_3AlF_6,Al_2O_3/Sm_2O_3 ratio（w_（（Al2O3））：w_（（Sm2O3）））〉 7：3, and temperature between 965 and 995 ℃.展开更多
基金Projects supported by the National Natural Science Foundation of China(51202203,51672228)the Project of State Key Laboratory of Environment-friendly Energy Materials(17FKSY0104)Science Development Foundation of China Academy of Engineering Physics
文摘Zirconolite is one of the most important matrix materials for nuclear waste immobilization.In this study,Sm was employed as the surrogate of trivalent actinides.Sm-doped zirconolite-rich waste forms were readily prepared by combustion synthesis(CS)using CuO as the oxidant.Two different schemes with or without Al2O3 as the charge compensator were carried out simultaneously.The results demonstrate that Al2O3 addition results in complex phase composition.On the other hand,the samples without Al2O3 addition show desirable products of zirconolite and pyrochlore.The EDX analysis shows that Sm is concurrently incorporated into the Ca and Zr sites of zirconolite,which transforms to pyrochlore structure with high Sm2O3 contents.The aqueous durability of representative Sm-doped sample(Sm-0.6)was investigated.The 42 days normalized leaching rate of Sm is as low as 6.41×10-7 g/(m2 d),which exhibits high durability of Sm-doped sample.
基金Project supported by the National Natural Science Foundation of China(51564015,51674126)Graduate Student Innovation Special Fund of Jiangxi Province(YC2015-B064)+2 种基金Science and Technology Research Project of Jiangxi Department of Education(GJJ150664)Outstanding doctoral dissertation project fund of JXUST(YB2016007)Scientific Research Fund of JXUST(NSFJ2014-G09)
文摘Samarium（Sm） has been widely used in making aluminum（Al）-Sm magnet alloy materials. The research team for this study developed a molten salt electrolyte system which directly produces AI-Sm alloy to replace the energy intensive conventional distillation technology. In this study, molten melt density was measured and operation conditions were optimized to separate AI-Sm alloy product from the fluoride molten melt electrolysis media based on density differences, Archimedes＇ principle was applied to measure density for the basic molten fluoride system（BMFS： Na_3 AlF_6-AlF_3-LiF-MgF_2）electrolysis media in the temperature range from 905 to 1055 ℃.The impact of temperature（t） and the Al_2O_3 and Sm_2O_3 addition ratio（w_（（Al2O3））,w_（（Sm2O3）） in the basic fluoride system on molten melt density was examined. The fluoride molten melt density relationship was determined to be：ρ=3.11701-0.00802 w_（（Al2O3））＋0.027825 w_（（Sm2O3））-0.00117 t. The test results showed that molten density decreases with increase in temperature and Al_2O_3 addition ratio, and increases with the addition of Sm_2O_3, and/or Al_2O_3＋Sm_2O_3. The separation of Al-Sm（density 2.3 g/cm^3） product melt from the BMFS melt is achieved by controlling the BMFS density to less than 2.0 g/cm3. It is concluded that the optimal operation conditions to control the BMFS molten salt density to less than 2.0 g/cm^3 are：maintain addition of Al_2O_3＋Sm_2 O_3（w_（（Al2O3））＋w_（（Sm2O3））〈9% of Na_3AlF_6,Al_2O_3/Sm_2O_3 ratio（w_（（Al2O3））：w_（（Sm2O3）））〉 7：3, and temperature between 965 and 995 ℃.
