• Nuclear Engineering and Technology
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• 제41권10호
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• pp.1307-1314
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• 2009

The isotope ratio of $^{134}Cs/^{137}Cs$ in a spent PWR fuel sample was obtained with a newly developed gamma/neutron combined measuring system at KAERI. Burnup and Pu/U ratio of the spent fuel sample were determined by using the measured isotope ratio and the burnup-isotope ratio correlation equations calculated from the ORIGEN-ARP computer code. The results were compared and evaluated with the chemically determined burnup and Pu/U ratio. As a result of the comparative evaluation, the nondestructively determined burnup and Pu/U ratio values showed a good agreement with the chemically obtained results to within a 4.5% and 0.8% difference, respectively.

• Mass Spectrometry Letters
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• 제2권4호
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• pp.80-83
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• 2011

Isotope ratio analysis of nuclear materials in individual particles is of great importance for nuclear safeguards. Although secondary ion mass spectrometry (SIMS) and thermal ionization mass spectrometry (TIMS) are utilized for the analysis of individual uranium particles, few studies were conducted for the analysis of individual uranium-plutonium mixed oxide particles. In this study, we applied SIMS and inductively coupled plasma mass spectrometry (ICP-MS) to the isotope ratio analysis of individual U-Pu mixed oxide particles. In the analysis of individual U-Pu particles prepared from mixed solution of uranium and plutonium standard reference materials, accurate $^{235}U/^{238}U$, $^{240}Pu/^{239}Pu$ and $^{242}Pu/^{239}Pu$ isotope ratios were obtained with both methods. However, accurate analysis of $^{241}Pu/^{239}Pu$ isotope ratio was impossible, due to the interference of the $^{241}Am$ peak to the $^{241}Pu$ peak. In addition, it was indicated that the interference of the $^{238}UH$ peak to the $^{239}Pu$ peak has a possibility to prevent accurate analysis of plutonium isotope ratios. These problems would be avoided by a combination of ICP-MS and chemical separation of uranium, plutonium and americium in individual U-Pu particles.

• Journal of Radiation Protection and Research
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• 제35권3호
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• pp.117-123
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• 2010

Pu 동위원소는 기원에 따라 각기 다른 $^{240}Pu/^{239}Pu$ 동위원소비를 나타내는 특성이 있다. 질량분석법은 극미량 장반감기핵종 분석에 매우 유용한 방법으로서 검출기 특성상 낮은 검출한계를 갖고 있으며, 소량의 시료를 이용하여 짧은 시간에 측정을 할 수 있다는 장점을 갖고 있으므로 Pu을 비롯한 장반감기 핵종 분석에 유용하다. 다중검출기유도결합플라즈마질량분석기(Multicollector ICP-MS)는 다중검출시스템을 이용하여 분석하고자 하는 여러 핵종의 동시분석이 가능하며, 특별히 본 연구에서는 극미량 핵종의 검출이 가능한 multiple ion counter (MIC)를 사용하여 Pu 동위원소 분석에 적용하였다. 본 연구방법의 검출한계(detection limit)는 최적화된 조건에서 $^{239}Pu$와 $^{240}Pu$ 각각 $0.10\;fg\;ml^{-1}$ ($0.24\;{\mu}Bq\;ml^{-1}$), $0.12\;fg\;ml^{-1}$ ($0.97\;{\mu}Bq\;ml^{-1}$)이었으며, 240Pu 기준으로 약 200 cps 정도의 매우 낮은 농도수준에서 1%이하의 $^{240}Pu/^{239}Pu$ 동위원소비 계측편차를 나타내었다. 본 연구방법은 표준용액 및 다양한 매트릭스의 표준물질 분석에 적용함으로써 검증 확인하였다.

• Nuclear Engineering and Technology
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• 제42권1호
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• pp.79-88
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• 2010

Spent $UO_2$ nuclear fuel discharged from a nuclear power plant (NPP) contains fission products, U, Pu, and other actinides. Due to neutron capture by $^{238}U$ in the rim region and a temperature gradient between the center and the rim of a fuel pellet, a considerable increase in the concentration of fission products, Pu, and other actinides are expected in the pellet periphery of high burnup fuel. The characterization of the radial profiles of the various isotopic concentrations is our main concern. For an analysis, spent nuclear fuels originating from the Yeonggwang-2 pressurized water reactor (PWR) were chosen as the test specimens. In this work, the distributions of some actinide isotopes were measured from center to rim of the spent fuel specimens by a radiation shielded laser ablation inductively coupled plasma mass spectrometer (LA-ICP-MS) system. Sampling was performed along the diameter of the specimen by reducing the sampling intervals from 500 ${\mu}m$ in the center to 100 ${\mu}m$ in the pellet periphery region. It was observed that the isotopic concentration ratios for minor actinides in the center of the specimen remain almost constant and increase near the pellet periphery due to the rim effect apart from the $^{236}U$ to $^{235}U$ ratio, which remains approximately constant. In addition, the distributions of local burnup were derived from the measured isotope ratios by applying the relationship between burnup and isotopic ratio for plutonium and minor actinides calculated by the ORIGEN2 code.