Earticle

Background: Analysis of enrichment of UO2 is important to verify the information declared by the license-holders. The redundancy methods are required to guarantee the analysis result. Korea Institute of Nuclear Nonproliferation and Control (KINAC) used to analyze it with alpha spectrometry and consign to Korea Basic Science Institute (KBSI) Thermal Ionization Mass Spectrometry (TIMS). This article evaluated the similarity of the results with two methods and derive correlation equation. It could be compared to the results measured by TIMS running by KBSI. Materials and Methods: There are not many certified materials for the uranium enrichment value. Therefore, 34 uranium pellets, which have the wide range of uranium enrichment from 0.21 to 4.69 wt%, were used for the experiments by the alpha spectrometry and the TIMS. Results and Discussion: The study shows there are the tendency of analyzed enrichment by each equipment. It shows uranium enrichment with alpha spectrometry evaluated 17% higher than that with TIMS on average. The regression equations were also derived in case the similarity between the two results with two methods is lower than predicted. Two experiments were designed to compare the effect of number of samples. The R2 was 0.9977 with 34 pellets. It shows the equation is appropriate to predict the enrichment values by TIMS with that of alpha spectrometry. The R2 was 0.9858 with four pellets for ten times. The R2 decreased while the number of samples increased. The discrepancy between the lowest and highest enrichment seems to be one of the reason for it. Conclusion: KINAC expects the first equation with 34 samples is useful to predict the result with TIMS, the redundancy method, based on the alpha spectrometry. The extra samples are necessary to collect if the enrichment value analyzed by TIMS is lower than the value predicted with the equation. Further study would be followed related to the impact of the peak counts for each uranium isotopes, sample amount and number of experiments when TIMS established in KINAC by the end of 2018.

파이로프로세싱 전해환원 공정에서 현재 사용 중인 Pt 양극을 대체하기 위한 소재 개발은 매우 중요하다. 이 연구에서는 전 기화학 반응시 산소를 발생시키는 전도성 세라믹 양극으로서 TiN의 전기화학적 거동을 알아보았다. UO2의 전해환원이 일어 나는 동안 TiN 양극의 적합성과 안정성에 대한 평가를 진행하였다. LiCl-Li2O 용융염에서 TiN 양극을 이용하여 UO2를 전기 화학적으로 금속 U로 변환시킬 수 있었다. 반응 도중 TiN의 산화 반응은 관찰되지 않았다. 하지만 TiN 내부에서 공공이 생 기는 것을 확인하였으며, 이에 따라 소재 수명에 제한이 있을 것으로 판단된다.

Developing novel anode materials to replace the Pt anode currently used in electrolytic reduction is an important issue on pyroprocessing. In this study, the electrochemical behavior of TiN was investigated as the conductive ceramic anode which evolves O2 gas during the reaction. The feasibility and stability of the TiN anode was examined during the electrolytic reduction of UO2. The TiN anode could electrochemically convert UO2 to metallic U in a LiCl–Li2O molten salt electrolyte. No oxidation of TiN was observed during the reaction; however, the formation of voids in the bulk section appeared to limit the lifetime of the TiN anode.

실증용 UO pellet 산화로의 실증을 위한 제한된 핫셀 공간 안에서 사용후 핵 연료를 취급하는 산화로는 소형화 하여야 하고, 사용후 핵 연료 분말은 UO pellet 산화로 장치로부터 비산되지 않아야 한다. 본 연구에서는 분말의 최종속도를 구하기 위하여 Stokes식과 밀도비식을 제안하였다. UO 의 최종속도 SiO 의 최종속도를 사용하여 예측하였고, 비산방지를 할 수 있는 최적유량을 결정하였다. SiO 의 이론 최종속도 식을 검증하고, UO 과 관계식을 예측하기 위하여 아크릴 장치를 만들었다. 목업시설 에 설치 된 산화로에서 제안된 이론최종속도식 인 Stokes식 의 20 L/min과 밀도비식의 14.5 L/min을 적용하여 UO 분말의 필터감지에 의해 검증하였다. 그 결과 밀도비식에 의한 14.5 L/min은 UO 이전혀 검출되지 않았고, Stokes식의 20 L/min에서는 평균 7m 의 입도분말이 검출되었다. 따라서 UO pellet 산화로에서 UO이 비산되지 않는 최적유량은 14.5L/min임을 알 수 있었고, 제안된 밀도비식이 바람직함을 알 수 있었다.

A voloxidizer for a hot cell demonstration, that handles spent fuels of a high radiation level in a limited space should be small and spent fuel powders should not be dispersed out of the equipment involved. In this study a density rate equation as well as the Stokes'equation has been proposed in order to obtain the theoretical terminal velocity of powders. The terminal velocity of UO has been predicted by using the terminal velocity of SiO, and then determination has been the optimum air flow rate which is able to prevent powders from scattering. An equation which has shown a relationship between theoretical terminal velocities of UO and SiO has been derived with the help of the Stokes'equation, and then an experimental verification made for the theoretical Stokes' equation of SiO by means of an experimental device made of acryl. The theoretical terminal velocity based on the proposed density rate equation has been verified by detecting UO powders in a filter installed in the mock-up voloxidizer. As the results, the optimum air flow rates seem to be 20 LPM by the Stokes'equation while they are 14.5 L/min by the density rate equation. At the experiments with the mock-up voloxidizer, a trace amount of UO seems to be detectable at the air flow rate of 14.5 L/min by the density rate equation, but UO powders of 7m diameter seem detectable at the air flow rate of 20 L/min by the Stokes'equation. It is revealed that 14.5 L/min is the optimum air flowe rate which is capable of preventing UO powders from scattering in the UO voloxidizer and the proposed density rate equation is proper to calculate the terminal velocity of UO powders.

[ ] 펠릿 20 kg HM/batch용 분말화 장치는 차세대관리 공정의 금속전환로 안으로 균질화된 분말을 공급하기 위하여 펠릿을 산화하여 으로 분말화하는 장치이다. 본 연구에는 펠릿 20 kg HM/batch용 분말화 장치 설계모델을 제시하고, 실증용 분말화 장치를 제작하여 검증실험을 수행한다. 분말화 장치 설계모델은 내부구조, 성능, 가열로 위치와 크기 등이 고려된다. 실험 방법은 펠릿 20 kg HM/batch용 분말화 장치 설계 모델에 따라 기존의 3단 메시 분말화 장치를 이용하여 분말의 메시 투과시험과 온도변화 특성 실험을 하여 장치 내부구조를 결정한다. 펠릿 20 kg HM/batch의 산화 반응도 실험과 가열로 위치별 온도 분포를 측정하고 장치의 성능과 가열로의 영 역 위치를 결정한다. 장치 크기를 결정하기 위하여 산화전의 20kg의 펠릿과 산화후의 부피를 측정한다. 이상의 결과를 토대로 실증용 분말화 장치를 설계. 제작하고, 검증을 위하여 산화도, 분말특성 및 분석 등을 수행하였다. 산화반응 실험결과 에서 기존장치에 비하여 분말의 메시 투과율이 향상되었으며, 기존의 3단 메시 장치의 펠릿산화시간이 13시간 소요된 것에 비하여 8시간으로 단축되었다. 분말 특성 분석결과, 평균 입도가 이었다. 제작된 펠릿 20 kg HM/batch용 분말화 장치 성능과 설계모델 예측 값은 대체로 잘 일치되었다.

Vol-oxidizer is a device to convert pellets into powder and to feed a homogeneous powder into a Metal Conversion Reactor in the ACP(Advanced Spent Fuel Conditioning Process). In this paper, we propose a design model of the vol-oxidizer, develop the new vol-oxidizer with a capacity of 20 kg HM/batch in pellets, and conduct a verification for the device. Design considerations include the internal structure, the capacity, the heating position of the device, and the size. The dimensions of the new vol-oxidizer are decided by the design model. We determine a permeability test of the measuring the temperature distribution, and the volume of and . We manufactured the new vol-oxidizer for a 20 kg HM/batch in pellets, and then analyzed the characteristics of the powder for the verification. The experimental results show that the permeability of the throughout mesh enhance more than old vol-oxidizer, the oxidation time takes only 8 hours when compared with the 13 hours of the old device, and the average distribution of particle size is . The capacities of new vol-oxidizer for a 20 kg HM/batch in pellets were agree well with the predictions of design model.

KAERI의 PRIDE 시설에서 공학규모의 전해환원용 원료물질인 UO2 다공성펠렛 제조를 위해 공정과 장치를 최적화시킨 내 용을 다루었다. UO2 분말과 별도로 attrition 밀링된 대용산화물 분말을 출발분말로, 정밀 칭량을 통해 사용후핵연료 조성을 모사하였다(Simfuel). Simfuel 분말은 각각 tumbling mixer로 혼합하여 균질화 하고, rotary press로 성형하여 furnace를 이 용해 소결하였다. 4% H2-Ar 분위기에서 1450℃ 24시간 고온 열처리하여 제조된 소결펠렛은 6.89 g·cm-3의 벌크밀도를 가 지며 이는 후속 전해환원 공정의 요구에 부합한다. 소결된 다공성펠렛의 미세구조 관찰을 통해 다공성 기지상과 함께 산화/ 금속 석출물이 관찰되어 사용후핵연료의 상이 모사됨을 확인하였다. 본 결과는 향후 공학규모 이상의 파이로 연구를 위한 UO2 다공성펠렛 제조에 중요한 기초자료로 활용 될 것이다.

Processing and equipment were tailored for engineering scale fabrication of UO2 porous pellets, a feed material for the electrolytic reduction process in the PRIDE (PyRoprocessing Integrated DEmonstration) facility at KAERI (Korea Atomic Energy Research Institute). The starting materials, UO2 powder and pre-milled surrogate oxide powders, were proportioned to simulate the chemical composition of spent fuel (so-called Simfuel). The Simfuel powders were homogenized by mixing, compacted into a pellet shape, and finally heat treated using a tumbling mixer, rotary press, and sintering furnace. After sintering at 1450℃ for 24 h in 4% H2-Ar, the average bulk density of the UO2 Simfuel pellets was 6.89 g·cm-3, which meets the standard of the following electrolytic reduction process. In addition, the results of a microstructural analysis demonstrated that the sintered Simfuel UO2 porous pellets accurately simulate the properties of spent fuel in terms of the formation of second phases. These results provide essential information for the massive fabrication of UO2 porous pellets for engineering scale pyroprocessing research.