• 분석과학
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• 제16권2호
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• pp.110-116
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• 2003

사용 후 핵연료의 화학특성 연구를 위하여 요오드의 분리와 정량에 관한 연구를 수행하였다. 사용 후 핵연료를 용해시키는 과정에서 핵연료 중에 CsI로 존재하는 요오드가 $I_2$로 산화되어 휘발되지 않도록 질산과 염산의 혼합산 (80:20 mol%)을 이용하여 비휘발성 ${IO_3}^-$­로 안정화시켰다. 2.5 M $HNO_3$ 매질에서 $NH_2OH{\cdot}HCl$을 이용하여 $I_2$로 환원시킨 후 사염화탄소로 추출하여 우라늄과 핵분열생성물로부터 분리, 회수하였다. 0.1 M $NaHSO_3$을 사용하여 요오드를 역추출하였으며 수용액층으로 회수된 요오드를 이온 크로마토그래피로 정량하였다. 방사성 물질 분석에 적합한 이온 크로마토그래피/차폐 시스템을 구성하였으며 42,000~44,000 MWd/MtU 의 연소도를 갖는 사용후핵연료를 대상으로 요오드를 분석한 결과 Origin 2 연소도 전산코드에 의한 계산결과인 $324.5{\sim}343.6{\mu}g/g$와는 -8.3~-0.5%의 편차를 나타내었다.

• 한국방사성폐기물학회:학술대회논문집
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• 한국방사성폐기물학회 2004년도 Proceedings of the 4th Korea-China Joint Workshop on Nuclear Waste Management
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• pp.245-256
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• 2004

The extraction of three kinds of amido podands, N,N,N'N'-tetrabutyl-3-oxa-pentanedi- amide (TBDGA), N,N,N'N'-tetra-isobutyl-3-oxa-pentanediamide(TiBDGA) and N,N,N'N'-tetra- butyl-3,6-dioxa-oct-anediam- ide(TBDOODA) on U(VI),Pu(IV), Am(III), Eu(III) and other metal ions is studied in nitric acid solutions. 40%octanol-kerosene is chosen as diluents to eliminate third phase and emulsion. TBDGA and TiBDGA show extraction selectivity to An(III) and Ln(III) much higher than to U(VI) and Pu(IV). Fe, Ru and Mo is poorly extracted by the three kinds of amid podands in 2~3mol/L $HNO_3$ solutions. Aiming to eliminate interface crude when using simulated HLLW solution in the system of 0.2mol/L TBDGA/Octanol＋kerosene, acetohydroxyamic acid was adapted. Distribution ratio of zirconium was decreased when adding acetohydroxyamic acid in aqueous solution, and interface crude disappeared as mixing extractant with HLLW. The counter-current extraction test is carried out in a set of miniature mixer-settler, with 0.2mol/L TBDGA/ 40% octanol-kerosene as extractant to separate U(VI), Pu(IV), Am(III) and Eu(III) from simulated high level liquid waste(HLLW) solution. In battery A, lanthanides and actinides are coextracted into organic phase with the recovery of 99.98% for U(Ⅵ), >99.99% for Pu(IV), and >99.99% for Am(III) and Eu(III) respectively. In battery R1, 99.99% U, 86.2% Pu and a part of Am or Eu are stripped into aqueous phase by 0.2mol/L acetohydroxyamic acid (AHA) in 0.01mol/L $HNO_3$ solution. In battery $R_2$, Am, Eu and remained Pu are completely back-extracted by 0.2mol/L AHA. This separation process contains no salt reagent, and it is not necessary to dilute HLLW feed.

• 대한화학회지
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• 제39권5호
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• pp.399-407
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• 1995

회토류와 악티늄족 원소의 현장분석을 목적으로 휴대용 극미량 분석용 원자 분광계인 Electrothermal-Hollow Cathode Glow Discharge Spectrometry(Et-HCGDS)가 제작되었다.본 분광계의 기본 구조는 전기열과 글로우 방전에 기초를 두고 있으며 본 분광계가 미량의 원소분석에도 유용함을 실험적으로 살펴보았다. 본 연구는 새로이 제작된 Et-HCGDS라는 글로우방전 시스템을 사용하여 공기의 저온 플라스마를 만들고 여기서 얻은 공기의 방출 스펙스럼에 관하여 연구하였다. 본 연구를 통하여 Et-HCGDS를 사용할시에 공기가 흐름가스로 유용하며 이 경우 대기의 분석도 쉽게 이루어질 수 있음을 알았다. 글로우 방전을 이용하여 관찰한 공기의 방출 스펙트럼의 분석을 통하여 볼 때 거의 질소에 의한 방출이 전 자외선과 가시광선 영역에서 골고루 나타남을 살펴보았다. 공기를 흐름가스로 사용할 시에도 여러파장 영역에서 미량 분석이 가능함을 알았다. 이 결과는 앞으로 Et-HCGDS를 사용하여 현장에서 공기만을 사용하여 분석을 수행할 경우에 필요한 기초 자료로 활용될 수 있으리라 본다. 본 연구에서 수행한 공기 방출 스펙트럼의 분석은 대기 분석 및 물질 분석에도 중요한 기초자료로 쓰이게 되리라 기대하며 이와 더불어 방출을 이용한 분광분석에서 공기로 인한 간섭 스펙트럼등을 이해하는 경우에도 중요한 참고자료로 활용되리라 본다.

• Nuclear Engineering and Technology
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• 제34권5호
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• pp.517-531
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• 2002

The speciation and solubility of Am, Np, Pu and U have been analyzed by means of the geochemical code MUGREM, under the chemical conditions of domestic deep groundwater, in order to support the preliminary safety assessment for a Korean HLW disposal concept. Under the conditions of groundwaters studied, the stable solid phase is AmOHC $O_3$(s) or Am(OH)$_3$(s), soddyite((U $O_2$)$_2$ $SiO_2$.2$H_2O$) or N $a_2$ $U_2$ $O_{7}$ (c), Np(OH)$_4$(am), and Pu(OH)$_4$(am) for Am, U, Np, and Pu, respectively. The dominating aqueous species are as follows: the complexes of Am(III), Am(OH)$_2$$^{+}$ and Am(C $O_3$)$_2$$^{[-10]}$ , the complexes of U(VI), U $O_2$(OH)$_3$$^{[-10]}$ and U $O_2$(C $O_3$)$_3$$^{4-}$, the complexes of Np(IV), Np(OH)$_4$(aq) and Np(OH)$_3$C $O_3$, and the complexes of Pu(IV), Pu(OH)$_4$(aq) and Pu(OH)$_3$C $O_3$$^{[-10]}$ . The calculated solubilities exist between 1.9E-10 and 1.3E-9 mol/L for Am, between 5.6E-6 and 1.2E-4 mol/L for U, between 3.1E-9 and 1.3E-8 mol/L for Np, and between 6.6E-10 and 2.4E-10 mol/L for Pu, depending on groundwater conditions. The present solubilities of each actinide agree well with the results of other studies obtained under similar conditions.s.

• Nuclear Engineering and Technology
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• 제47권3호
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• pp.380-387
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• 2015

A lead slowing-down spectrometer (LSDS) system is a promising nondestructive assay technique that enables a quantitative measurement of the isotopic contents of major fissile isotopes in spent nuclear fuel and its pyroprocessing counterparts, such as $^{235}U$, $^{239}Pu$, $^{241}Pu$, and, potentially, minor actinides. The LSDS system currently under development at the Korea Atomic Energy Research Institute (Daejeon, Korea) is planned to utilize a high-flux ($>10^{12}n/cm^2{\cdot}s$) neutron source comprised of a high-energy (30 MeV)/high-current (~2 A) electron beam and a heavy metal target, which results in a very intense and complex radiation field for the facility, thus demanding structural shielding to guarantee the safety. Optimization of the structural shielding design was conducted using MCNPX for neutron dose rate evaluation of several representative hypothetical designs. In order to satisfy the construction cost and neutron attenuation capability of the facility, while simultaneously achieving the aimed dose rate limit (< $0.06{\mu}Sv/h$), a few shielding materials [high-density polyethylene (HDPE)eBorax, $B_4C$, and $Li_2CO_3$] were considered for the main neutron absorber layer, which is encapsulated within the double-sided concrete wall. The MCNP simulation indicated that HDPE-Borax is the most efficient among the aforementioned candidate materials, and the combined thickness of the shielding layers should exceed 100 cm to satisfy the dose limit on the outside surface of the shielding wall of the facility when limiting the thickness of the HDPE-Borax intermediate layer to below 5 cm. However, the shielding wall must include the instrumentation and installation holes for the LSDS system. The radiation leakage through the holes was substantially mitigated by adopting a zigzag-shape with concrete covers on both sides. The suggested optimized design of the shielding structure satisfies the dose rate limit and can be used for the construction of a facility in the near future.

• Nuclear Engineering and Technology
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• 제47권1호
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• pp.47-58
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• 2015

Four recycling scenarios involving pyroprocessing of spent fuel (SF) have been investigated for a 600-MWe transmutation sodium-cooled fast reactor (SFR), KALIMER. Performance evaluation was done with code system REBUS connected with TRANSX and TWODANT. Scenario Number 1 is the pyroprocessing of Canada deuterium uranium (CANDU) SF. Because the recycling of CANDU SF does not have any safety problems, the CANDU-Pyro-SFR system will be possible if the pyroprocessing capacity is large enough. Scenario Number 2 is a feasibility test of feed SF from a pressurized water reactor PWR. Thefsensitivity of cooling time before prior to pyro-processing was studied. As the cooling time sensitivity of cooling time before prior to pyro-processing was studied. As the cooling time increases, excess reactivity at the beginning of the equilibrium cycle (BOEC) decreases, thereby creating advantageous reactivity control and improving the transmutation performance of minor actinides. Scenario Number 3 is a case study for various levels of recovery factors of transuranic isotopes (TRUs). If long-lived fission products can be separated during pyroprocessing, the waste that is not recovered is classified as low- and intermediate-level waste, and it is sufficient to be disposed of in an underground site due to very low-heat-generation rate when the waste cooling time becomes >300 years at a TRU recovery factor of 99.9%. Scenario Number 4 is a case study for the recovery factor of rare earth (RE) isotopes. The RE isotope recovery factor should be lowered to ${\leq}20%$ in order to make sodium void reactivity less than <7$, which is the design limit of a metal fuel.

• Nuclear Engineering and Technology
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• 제40권7호
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• pp.593-606
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• 2008

In this study, data on radionuclide migration and retardation processes in the engineered and natural barriers of High-Level Radioactive Waste (HLW) repository have been reviewed and compiled for use in the performance assessment of a HLW disposal system in Korea. The status of the database on radionuclide migration and retardation that is being developed in Korea is investigated and summarized in this study. The solubilities of major actinides such as D, Th, Am, Np, and Pu both in Korean bentonite porewater and in deep Korean groundwater are calculated by using the geochemical code PHREEQC (Ver. 2.0) based on the KAERI-TDB(Korea Atomic Energy Research Institute-Thermochemical Database), which is under development. Databases for the diffusion coefficients ($D^b_e$ values) and distribution coefficients ($K^b_d$ values) of some radionuclides in the compacted Korean Ca-bentonite are developed based upon domestic experimental results. Databases for the rock matrix diffusion coefficients ($D^r_e$ values) and distribution coefficients ($K^r_d$ values) of some radionuclides for Korean granite rock and deep groundwater are also developed based upon domestic experimental results. Finally, data related to colloids such as the characteristics of natural groundwater colloids and the pseudo-colloid formation constants ($K_{pc}$ values) are provided for the consideration of colloid effects in the performance assessment.

• Nuclear Engineering and Technology
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• 제42권1호
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• pp.17-36
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• 2010

In this study, we compare the mass release rates of radionuclides(1) from waste forms arising from the KIEP-21 pyroprocessing system with (2) those from the directly-disposed pressurized-water reactor spent fuel, to investigate the potential radiological and environmental impacts. In both cases, most actinides and their daughters have been observed to remain in the vicinity of waste packages as precipitates because of their low solubility. The effects of the waste-form alteration rate on the release of radionuclides from the engineered-barrier boundary have been found to be significant, especially for congruently released radionuclides. the total mass release rate of radionuclides from direct disposal concept is similar to those from the pyroprocessing disposal concept. While the mass release rates for most radionuclides would decrease to negligible levels due to radioactive decay while in the engineered barriers and the surrounding host rock in both cases even without assuming any dilution or dispersal mechanisms during their transport, significant mass release rates for three fission-product radionuclides, $^{129}I$, $^{79}Se$, and $^{36}Cl$, are observed at the 1,000-m location in the host rock. For these three radionuclides, we need to account for dilution/dispersal in the geosphere and the biosphere to confirm finally that the repository would achieve sufficient level of radiological safety. This can be done only after we have known where the repository site would by sited. the footprint of repository for the KIEP-21 system is about one tenth of those for the direct disposal.

• Nuclear Engineering and Technology
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• 제43권2호
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• pp.149-158
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• 2011

Metal waste generated from the pyroprocessing of 10 MtU of spent fuel was classified by comparing the specific activity of a relevant radionuclide with the limit value of the specific activity specified in the Korean acceptance criteria for a lowand intermediate-level waste repository. A Korean Optimized Fuel Assembly design with a 17${\times}$17 array, an initial enrichment of 4.5 weight-percent, discharge burn-up of 55 GWD/MtU, and a 10-year cooling time was considered. Initially, the mass and volume of each structural component of the assembly were calculated in detail, and a source term analysis was subsequently performed using ORIGEN-S for these components. An activation cross-section library generated by the KENO-VI/ORIGEN-S module was utilized for top-end and bottom-end pieces. As a result, an Inconel grid plate, a SUS plenum spring, a SUS guide tube subpart, SUS top-end and bottom-end pieces, and an Inconel top-end leaf spring were determined to be unacceptable for the Gyeongju low- and intermediate-level waste repository, as these waste products exceeded the acceptance criteria. In contrast, a Zircaloy grid plate and guide tube can be placed in the Gyeongju repository. Non-contaminated Zircaloy cladding occupying 76% of the metal waste was found to have a lower level of specific activity than the limit value. However, Zircaloy cladding contaminated by fission products and actinides during the decladding process of pyroprocessing was revealed to have 52 and 2 times higher specific activity levels than the limit values for alpha and $^{90}Sr$, respectively. Finally, it was found that 88.7% of the metal waste from the 17${\times}$17 Korean Optimized Fuel Assembly design should be disposed of in a deep geological repository. Therefore, it can be summarized that separation technology with a higher decontamination factor for transuranics and strontium should be developed for the efficient management of metal waste resulting from pyroprocessing.

• 한국방사성폐기물학회:학술대회논문집
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• 한국방사성폐기물학회 2019년도 춘계학술논문요약집
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• pp.69-69
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• 2019

The distillation of liquid cathode is necessary to separate cadmium from the actinide elements in the pyroprocessing since the actinide deposits are dissolved or precipitated in a liquid cathode. It is very important to avoid a splattering of cadmium during evaporation due to the high vapor pressure. Several methods have been proposed to lower the splattering of cadmium during distillation. One of the important methods is an installation of crucible cover on the distillation crucible. A multi-layer porous round cover was proposed to avoid a cadmium splattering in our previous study. In this study, the effect of crucible cover on the cadmium distillation was examined to develop a splatter shield. Various surrogates were used for the actinides in the cadmium. The surrogates such as bismuth, zirconia, and tungsten don't evaporate at the operational temperature of the Cd distiller due to their low vapor pressures. The distillation experiments were carried out in a crucible equipped with cover and in a crucible without cover. About 40 grams of Cd was distilled at a reduced pressure for two hours at various temperatures. The mixture of the cadmium and the surrogate was heated at $470{\sim}620^{\circ}C$. Most of the bismuth remained in the crucible equipped with cover after distillation under $580^{\circ}C$ for two hours, whereas small amount of bismuth decreased in the crucible without cover above $580^{\circ}C$. The liquid bismuth escaped with liquid cadmium drop from the crucible without cover. It seems that the crucible cover played a role to prevent the splash of the liquid cadmium drop. The effect of the cover was not clear for the tungsten or zirconia surrogate since the surrogates remained as a solid powder at the experimental temperature. From the results of this work, it can be concluded that the crucible cover can be used to minimize the deposit loss by prevention of escape of liquid drop from the crucible during distillation of liquid cathode.