• Nuclear Engineering and Technology
• /
• 제51권1호
• /
• pp.257-262
• /
• 2019

The control of microstructure is critical for the porous fuel particles used for infiltrating actinide nuclides. This study concerns the effect of heating processes on properties and microstructure of the fuel particles. The uniform gel precursor beads were synthesized by a microfluidic sol-gel process and then the porous $CeO_2$ microspheres, as a surrogate for the ceramic nuclear fuel particles, were obtained by heating treatment of the gel precursors. The fabricated $CeO_2$ microspheres have a narrow size distribution and good sphericity due to the feature of microfluidics. The effects of heating processes parameters, such as heating mode and peak temperatures on the properties of microspheres were studied in detail. An optimized heating mode and the peak temperature of $650^{\circ}C$ were selected to produce porous $CeO_2$ microspheres. The optimized heating mode can avoid the appearance of broken or crack microspheres in the heating process, and as-prepared porous microspheres were of suitable pore size distribution and pore volume for loading minor actinide (MA) solution by an infiltration method that is used for fabrication of MA-bearing nuclear fuel beads. After the infiltration process, $1000^{\circ}C$ was selected as the final temperature to improve the compressive strength of microspheres.

• Nuclear Engineering and Technology
• /
• 제53권2호
• /
• pp.603-610
• /
• 2021

The major drawback of zirconia-based materials, in view of their applications as targets for minor actinide transmutation, is their poor thermal conductivity. The addition of MgO, which has high thermal conductivity, to zirconia-based materials is expected to improve their thermal conductivity. On these grounds, the present study aims at phase characterization and thermophysical property evaluation of neodymium-substituted zirconia (Zr_0.8Nd_0.2O_1.9; using Nd₂O₃ as a surrogate for Am₂O₃) and its composites with MgO. The composite was prepared by a solid-state reaction of Zr_0.8Nd_0.2O_1.9 (synthesized by gel combustion) and commercial MgO powders at 1773 K. Phase characterization was carried out by X-ray diffraction and the microstructural investigation was performed using a scanning electron microscope equipped with energy dispersive spectroscopy. The linear thermal expansion coefficient of Zr_0.8Nd_0.2O_1.9 increases upon composite formation with MgO, which is attributed to a higher thermal expansivity of MgO. Similarly, specific heat also increases with the addition of MgO to Zr_0.8Nd_0.2O_1.9. Thermal conductivity was calculated from measured thermal diffusivity, temperature-dependent density and specific heat values. Thermal conductivity of Zr_0.8Nd_0.2O_1.9-MgO (50 wt%) composite is more than that of typical UO₂ fuel, supporting the potential of Zr_0.8Nd_0.2O_1.9-MgO composites as target materials for minor actinides transmutation.

• Nuclear Engineering and Technology
• /
• 제44권7호
• /
• pp.767-772
• /
• 2012

In support of optimizing electrorefining technology for treating spent nuclear fuel, lithium drawdown has been investigated for separating actinides from molten salt electrolyte. Drawdown reaction selectivity is a major issue that requires investigation, since the goal is to remove actinides while leaving the fission products and other components in the salt. A series of lithium drawdown tests with surrogate fission product chlorides was run to obtain selectivity data with non-radioactive salts, develop a predictive model, and draw conclusions about the viability of using this process with actinide-loaded salt. Results of tests with CsCl, $LaCl_3$, $CeCl_3$, and $NdCl_3$ are reported here. Equilibrium was typically achieved in less than 10 hours of contact between lithium metal and molten salt under well-stirred conditions. Maintaining low oxygen and water impurity concentrations (<10 ppm) in the atmosphere was observed to be critical to minimize side reactions and maintain stable salt compositions. An equilibrium model has been formulated and fit to the experimental data. Good fits to the data were achieved. Based on analysis and results obtained to date, it is concluded that clean separation between minor actinides and lanthanides will be difficult to achieve using lithium drawdown.

• Nuclear Engineering and Technology
• /
• 제54권5호
• /
• pp.1623-1634
• /
• 2022

A new irradiation loop design has been developed, which provides the ability to carry out radiolytic resistance studies of extraction systems simulating process relevant conditions in an easy and simple way. The step-by-step loop configuration permits an easy modification of settings and has a relative low volume requirement. This irradiation loop has been initially set up to test the main EURO-GANEX process steps: the lanthanide (Ln) and actinide (An) co-extraction followed by the transuranic (TRU) stripping. The performance and changes in the composition have been analyzed during the irradiation experiment by different techniques: gamma spectroscopy and ICP-MS for the extraction and corrosion behavior of the full system, and HPLC-MS and Raman spectroscopy to determine the degradation of the organic and aqueous solvents, respectively. The Ln and An co-extraction step and the corrosion that occurred during the first irradiation step revealed the favorable expected results according to literature. The effects of acidity changes occurred during the irradiation process, the presence of stainless corrosion products in solution as well as the new possible degradation compounds have been explored in the An stripping step. The results obtained demonstrate the importance of developing realistic irradiation experiments where different factors affecting the performance can be easily studied and isolated.

• Nuclear Engineering and Technology
• /
• 제52권5호
• /
• pp.1013-1021
• /
• 2020

A combination of simultaneous thermal analysis, evolved gas analysis and non-ambient XRD techniques was used to characterise and investigate the conversion reactions of ammonium uranates into uranium oxides. Two solid phases of the ternary system NH₃ - UO₃ - H₂O were synthesised under specified conditions. Microspheres prepared by the sol-gel method via internal gelation were identified as 3UO₃·2NH₃·4H₂O, whereas the product of a typical ammonium diuranate precipitation reaction was associated to the composition 3UO₃·NH₃·5H₂O. The thermal decomposition profile of both compounds in air feature distinct reaction steps towards the conversion to U₃O₈, owing to the successive release of water and ammonia molecules. Both compounds are converted into α-U₃O₈ above 550 ℃, but the crystallographic transition occurs differently. In compound 3UO₃·NH₃·5H₂O (ADU) the transformation occurs via the crystalline β-UO₃ phase, whereas in compound 3UO₃·2NH₃·4H₂O (microspheres) an amorphous UO₃ intermediate was observed. The new insights obtained on these uranate systems improve the information base for designing and synthesising minor actinide-containing target materials in future applications.

• 한국광물학회지
• /
• 제16권4호
• /
• pp.307-320
• /
• 2003

Fe­석류석인 경우, 사면체 배위를 하는 Fe의 이온반경이 Si보다 크기 때문에 고준위 방사성 폐기물에 다량 함유되어 있는 악티나이드 원소들을 고정화시킬 수 있는 매트릭스로 고려되고 있다. 따라서 본 연구에서는 $Ca_{2,5}$C $e_{0.5}$Z $r_2$F $e_3$ $O_{12}$ 및 $Ca_2$CeZrFeF $e_3$ $O_{12}$인 조성을 가진 석류석을 합성하여 이들의 상평형 관계 및 특성을 연구하였다. 혼합된 시료는 200∼400 kg/$\textrm{cm}^2$의 압력으로 성형한 후, 1100∼140$0^{\circ}C$ 범위에서 온도 및 분위기를 변화시키면서 소결하였으며 합성된 시료는 XRD, SEM/EDS를 사용하여 상분석과 정량분석을 실시하였다. 실험결과, 이들 조성을 가진 석류석들은 130$0^{\circ}C$로 가열하였을 때, 최적 합성상을 얻을 수 있었지만 소량의 페롭스카이트 등 부수상이 공존하였다. $Ca_{2,5}$C $e_{0.5}$Z $r_2$F $e_3$ $O_{12}$ 및 $Ca_2$CeZrFeF $e_3$ $O_{12}$인 조성으로부터 합성된 Fe­석류석의 조성이 각각 $Ca_{2.5­3.2}$C $e_{0.3­0.7}$Z $r_{1.8­2.8}$F $e_{1.9­3.2}$ $O_{12}$ 및 $Ca_{2.2­2.5}$C $e_{0.8­1.0}$Z $r_{1.3­1.6}$F $e_{0.4­.07}$ F $e_{3­3.2}$ $O_{12}$였다. 특히 화학양론적 조성과 비교시, 합성된 석류석의 8배위 자리를 점하고 있는 Ca이 초과된 양상을 보였고, Ce의 함량은 초과 또는 결핍된 양상을 보였다. 이는 8배위 자리에서의 Ca과 Ce의 이온반경의 상대적인 차이 및 전하보상적 차원에서 비롯된 것으로 해석된다.에서 비롯된 것으로 해석된다.

• 공업화학
• /
• 제8권6호
• /
• pp.1006-1013
• /
• 1997

방사성 폐액에 존재하는 악티늄족과 란탄족의 대표원소로 Am과 Eu을 각각 선정하여 Zr을 함유한 di-(2-ethylhexyl) phosphoric acid 추출제를 사용하여 회분식으로 이들 원소의 상호분리에 대한 분리특성을 고찰하였다. 0.5M $HNO_3$에서 Zr을 함유한 1M DEHPA/n-dodecane(Zr 농도:$8.7g/{\ell}$)에 의한 Am 및 Eu의 추출율은 각각 92.3%와 99.1%이었으며, 추출제 1M DEHPA/n-dodecane에 함유된 Zr 농도에 비례하여 Am과 Eu의 추출율이 증가하는 상승효과를 보였다. 그리고 pH가 3.0으로 조정된 0.05M DTPA와 1M lactic acid의 혼합용액에 의한 제 1단계 역추출에서는 유기상으로 추출된 Am과 Eu의 38.1% 및 3%가 각각 역추출되었으며, 이때 Am 과 Eu의 분배계수로부터 구한 상호 분리 계수는 14.2였다. 또한 6M $HNO_3$용액에 의한 제2단계 역추출에서는 제1단계 역추출에서 역추출되지 않고 유기상에 남아 있는 Eu의 94.4%가 역추출되었다.

• 자원환경지질
• /
• 제38권2호
• /
• pp.187-196
• /
• 2005

석류석 구조에서, 양이온이 점할 수 있는 구조적 위치는 사면체, 팔면체 및 이들과 능을 공유하고 있는 배위다면체의 중심 등이다. 이들 중, 사면체의 자리를 차지하는 양이온의 크기는 석류석의 단위포의 크기와 밀접한 관계를 가진다. 따라서 4-배위 자리에 비교적 이온반경이 큰 철을 함유하고 있는 석류석은 방사성 폐기물 내에 함유된 비교적 이온반경이 큰 악티나이드 원소를 고정시키기 위한 유망한 매트릭스로써 고려될 수 있다. 따라서 본 연구에서는 $Ca_{1.5}GdCe_{0.5}ZrFeFe_3O_{12}$인 조성을 가진 석류석을 합성하여 이들의 상평형 관계 및 특성을 연구하였다. 혼합된 시료는 $200{\~}400{\cal}kg/{\cal}cm^2$의 압력으로 성형한 후, $1100{\~}1400^{\circ}C$ 범위에서 온도 및 분위기를 변화시키면서 소결하였으며, 합성된 시료는 XRD 및 SEM/EDS를 사용하여 상분석과 정량분석을 실시하였다. 실험결과, 석류석은 소결온도 $1300^{\circ}C$에서 최적의 합성상을 얻을 수 있었지만, 미량의 페로브스카이트 및 미지의 상이 공존하였다. 석류석과 페로브스카이트의 화학조성은 각각 $[Ca_{l.2-1.8}Gd_{0.9-1.4}Ce_{0.3-0.5}]^{VIII}[Zr_{0.8-1.3}Fe_{0.7-1.2}]^{VI}[Fe_{2.9-3.1}]^{IV}O_{12}$ 및 $Ca_{0.1-0.5}Gd_{0.0-0.8}Ce_{0.1-0.5}\;Zr_{0.0-0.2}Fe_{0.9-1.1}O_3$ 이었다. 특히 화학양론적 조성과 비교 시, 합성된 석류석의 8-배위 자리를 점하고 있는 Ca의 초과 및 Ce의 결핍된 양상을 보였다. 이는 6-배위 자리에서의 Zr 및 Fe의 화학조성과 밀접한 관계를 지닌다.