• Nuclear Engineering and Technology
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• 제38권6호
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• pp.459-482
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• 2006

A geochemical approach to the long-term safety of waste disposal is discussed in connection with the significance of actinides, which shall deliver the major radioactivity inventory subsequent to the relatively short-term decay of fission products. Every power reactor generates transuranic (TRU) elements: plutonium and minor actinides (Np, Am, Cm), which consist chiefly of long-lived nuclides emitting alpha radiation. The amount of TRU actinides generated in a fuel life period is found to be relatively small (about 1 wt% or less in spent fuel) but their radioactivity persists many hundred thousands years. Geological confinement of waste containing TRU actinides demands, as a result, fundamental knowledge on the geochemical behavior of actinides in the repository environment for a long period of time. Appraisal of the scientific progress in this subject area is the main objective of the present paper. Following the introductory discussion on natural radioactivities, the nuclear fuel cycle is briefly brought up with reference to actinide generation and waste disposal. As the long-term disposal safety concerns inevitably with actinides, the significance of the aquatic actinide chemistry is summarized in two parts: the fundamental properties relevant to their aquatic behavior and the geochemical reactions in nanoscopic scale. The constrained space of writing allows discussion on some examples only, for which topics of the primary concern are selected, e.g. apparent solubility and colloid generation, colloid-facilitated migration, notable speciation of such processes, etc. Discussion is summed up to end with how to make a geochemical approach available for the long-term disposal safety of nuclear waste or for the performance assessment (PA) as known generally.

• 공업화학
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• 제10권7호
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• pp.996-1002
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• 1999

알칼리 및 알칼리토금속(Cs, Rb, Ba, Sr), 전이금속(Zr, Fe, Mo, Ni, Pd, Rh), 란탄족(La, Y, Nd, Ce, Eu) 및 악티늄족(Np, Am) 등 17개 원소로 구성된 질산매질의 모의 방사성용액에서 옥살산에 의한 란탄족과 악티늄족 원소의 공침전 연구를 수행하였다. 옥살산 농도 0.5 M에서 질산농도의 영향과 아스코빅산 첨가에 따른 원소들의 침전율이 조사되었다. 각 원소들의 침전율은 질산농도에 따라 약간 감소하였으나 란탄족과 악티늄족은 99% 이상 침전되었다. 옥살산 침전시 아스코빅산이 첨가되는 경우 Pd이 금속으로 환원 침전되었고, 이때 Mo, Fe, Ni, Ba의 경우는 침전율이 약 10~20% 감소하는 것으로 나타났으나, 기타 원소들에 대해서는 영향이 나타나지 않았다. Pd(II) 이온은 질산농도 1.0 M 미만의 모의용액에서 아스코빅산 첨가시 Pd 금속으로의 환원침전이 일어났으며, 아스코빅산 농도가 0.01~0.02 M 부근에서 가장 크게 나타났다. 하이드라진이 아스코빅산과 같이 첨가될 때 Pd의 환원침전을 억제하는 것으로 나타났다.

• 한국광물학회지
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• 제15권1호
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• pp.78-84
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• 2002

New pyrochlore-type phases($A_2$$B_2$$O_{7}$) were synthesized in the systems: CaO-C$eO_2$-T$iO_2$, CaO-$UO_2$(T$hO_2$)-Z$rO_2$, CaO-$UO_2$(T$hO_2$)-$Gd_2$$O_3$-T$iO_2$-Z$rO_2$, 및 CaO-T$hO_2$-S$nO_2$. The starting materials were pressed with the pressure of 200~400 MPa and sintered at 1500~ 155$0^{\circ}C$ for 4~8 hours in air and at 1300~ 135$0^{\circ}C$ for 5 ~50 hours under oxygen atmosphere. The products were characterized using XRD, SEM/EDS and TEM. In the bulk compositions of CaCe$Ti_2$$O_{7}$, CaTh$Zr_2$$O_{7}$,($Ca_{0.5}$ Gd$Th_{0.5}$)(ZrTi)$O_{7}$) ($Ca_{0.5}$Gd$Th_{0.5}$)(ZrTi)$O_{7}$, ($Ca_{0.5}$G$dU_{0.5}$)(ZrTi)$O_{7}$ and CaTh$Sn_2$$O_{7}$ , pyrochlore was the major phase, together with other oxide phase $of_2$$O_{7}$ fluorite structure. In the samples with target compositions CaU$Zr_2$$O_2$및 $Ca_{0.5}$ G$dU_{0.5}$)$Zr_2$T$iO_{7}$ pyrochlore was not identified, but a fluorite-structured phase was detected. The formation factor as the stable phase depended on crystal chemical characteristics of the actinide and lanthanide elements of the system concerned.

• Nuclear Engineering and Technology
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• 제43권4호
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• pp.329-334
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• 2011

Two conceptual flowsheets were developed for recycling used nuclear fuel. One flowsheet was developed for recycling used oxide nuclear fuel from light water reactors while the other was developed for recycling used metal fuel from fast spectrum reactors. Both flowsheets were developed from a set of design principles including efficient actinide recovery, nonproliferation, waste minimization and commercial viability. Process chemistry is discussed for each unit operation in the flowsheet.

• 방사성폐기물학회지
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• 제16권3호
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• pp.369-376
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• 2018

The ability to recover the nearly limitless supply of uranium contained within the world's oceans would provide supply security to uranium based fuel cycles. Therefore, in addition to U.S. national laboratories conducting R&D on a system capable of harvesting seawater uranium, a number of collaborative university partners have developed alternative technologies to complement the national laboratory scheme. This works summarizes the systems analysis of such novel uranium recovery technologies along with their potential impacts on seawater uranium recovery. While implementation of some recent developments can reduce the cost of seawater uranium by up to 30%, other researchers have sought to address a weakness while maintaining cost competitiveness.

• Nuclear Engineering and Technology
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• 제53권2호
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• pp.603-610
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• 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
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• 제52권5호
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• pp.1013-1021
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• 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.

• 공업화학
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• 제8권6호
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• pp.1006-1013
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• 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.

• 방사성폐기물학회지
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• 제16권4호
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• pp.397-410
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• 2018

아메리슘(Am)은 사용후핵연료의 장기 방사성 독성에 크게 영향을 주기 때문에 고준위 방사성 폐기물 처분의 장기 안전성 평가에 필수적으로 고려되어야 할 원소이다. 분광학적 방법을 이용한 일부 악티나이드 원소의 화학반응 연구가 활발히 진행되고 있는 반면, 아메리슘에 대한 연구는 아직까지 미비한 상황이다. 이 연구에서는 고순도의 시료를 필요로 하는 화학반응 연구를 위하여 $^{241}Am$ 시료를 정제한 후, 액체섬광계수기와 감마선 및 알파선 스펙트럼을 이용하여 정량과 정성분석을 하였다. 액체 광도파 모세관 셀을 이용한 고감도의 UV-Vis 흡수 분광학과 시간분해 레이저 형광 분광학을 이용하여 Am(III) 가수분해물과 옥살레이트(oxalate, Ox) 착물반응을 조사하였다. 산성조건에서 $Am^{3+}$은 503 nm에서 최대 흡수봉우리를 보이며, 몰흡광계수는 $424{\pm}8cm^{-1}{\cdot}M^{-1}$임을 확인하였다. 중성 이상의 pH 조건에서 형성되는 $Am(OH)_3(s)$ 콜로이드 입자에서는 506-507 nm 파장에서 최대 흡수봉우리가 관측되었다. ${Am(Ox)_3}^{3-}$ 착물은 $Am^{3+}$에 비교하여 흡수 및 발광스펙트럼이 각각 4와 5 nm정도 장파장으로 이동하였고 몰흡광계수와 발광세기도 크게 증가하였다. ${Am(Ox)_3}^{3-}$의 발광수명은 23에서 56ns으로 증가하였고 이는 Am(III)의 내부권에 결합하고 있던 약 여섯 개의 물분자가 옥살레이트의 카르복실기로 치환되었음을 의미한다. 이 결과로부터 ${Am(Ox)_3}^{3-}$은 각 옥살레이트 리간드가 두 자리 결합(bidentate)을 하고 있다는 것을 제안하였다.