• Mass Spectrometry Letters
• /
• 제2권4호
• /
• pp.80-83
• /
• 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
• /
• 제35권3호
• /
• pp.117-123
• /
• 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
• /
• 제50권1호
• /
• pp.140-144
• /
• 2018

Isotopic analyses of plutonium and low-enriched uranium mixtures with particle sizes of $0.6-3.3{\mu}m$ were performed using thermal ionization mass spectrometry with a continuous heating method to verify its effectiveness for the accurate analysis of minor isotopes without sample pretreatment. The mixed particles used in this study were prepared from a mixed solution of plutonium (SRM 947) and uranium (U010, $^{235}U$ 1% enriched) reference materials. The isotope ratios for plutonium in the individual mixed particles, including $^{238}Pu/^{239}Pu$, $^{241}Pu/^{239}Pu$ as well as $^{240}Pu/^{239}Pu$, and $^{242}Pu/^{239}Pu$, were in good agreement with the certified values despite the isobaric interference of $^{238}U$ and $^{241}Am$. The isotope ratios for uranium in the mixed particles also agreed well with the certified values within the range of error. However, the isotope ratios for minor isotopes, such as $^{234}U$ and $^{236}U$, in the particles with diameters of less than approximately $1.8{\mu}m$ could not be measured because numbers of $^{234}U$ and $^{236}U$ atoms in analyzed particles are too low. These results indicate that thermal ionization mass spectrometry with a continuous heating method is applicable for the analysis of trace amounts of plutonium isotopes, including $^{238}Pu$ and $^{241}Pu$, despite the presence of the respective isobars $^{238}U$ and $^{241}Am$ in the microsamples.

• 한국원자력학회:학술대회논문집
• /
• 한국원자력학회 1998년도 춘계학술발표회논문집(2)
• /
• pp.551-556
• /
• 1998

The correlation of isotope composition of Zr with the turnup and some heavy isotopes in PWR uranium dioxide fuel has been investigated. The total and partial ($^{235}$ U) burnup were determined by $^{148Nd}$ and by U and Pu mass spectrometric method, respectively. After separating Zr from the fuel samples, its isotope composition was measured by mass spectrometry. In addition, the quantities of the U and Pu in the spent fuel were determined by isotope di lution mass spectrometric method using $^{233}$ U and $^{242}$ Pu as spikes. The content of some heavy isotopes, $^{235}$ U, $^{239}$ Pu and $^{241}$ Pu, and the Pu Contribution to total turnup were expressed by the correlation with Zr isotope ratios, $^{91}$ Zr/$^{96}$ Zr and $^{93}$ Zr/$^{96}$ Zr The correlations by isotope compositions measured were compared wi th those calculated from ORIGEN2 code.

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

• Nuclear Engineering and Technology
• /
• 제29권4호
• /
• pp.327-335
• /
• 1997

The correlation of isotope composition of uranium, plutonium and neodymium with the burnup in M uranium dioxide fuel has been investigated experimentally. The total and fractional($^{235}$ U) burnup were determined by Nd-148 and, U and Pu mass spectrometric method respectively. The isotope compositions of these elements, after their separation from the fuel samples were measured by mass spectrometric. The content of the elements in the irradiated fuel ore determined by isotope dilution mass spectrometric method using $^{233}$ U, $^{242}$ Pu and $^{150}$ Nd as spikes. The content of plutonium in the irradiated fuel was expressed by the correlation with uranium isotopes. The correlations between isotope compositions themselves and the total and fractional burnup ore compared with those calculated from ORIGEN2 code.

• Nuclear Engineering and Technology
• /
• 제21권4호
• /
• pp.277-286
• /
• 1989

PWR 핵연료의 연소도측정은 삼중스파이크(U-233. Pu-242, Nd-150)를 사용한 동위원소 희석 질량분석법으로 U, PU, Nd-148 및 Nd-(145+146)을 정량하여 수행하였다. 이 방법은 먼저 두개의 연속적 이온교환수지 분리과정을 거친다. Pu는 첫번째 음이온 교환수지 분리관(Dowex AG 1 X 8)으로부터 12 M HCl-0.1 M HI 혼합용액으로 분리하고 이어서 0.1 M HCl로 U을 분리하였다. Nd은 질산-메탄올 용리액으로 두번째 음이온 교환수지분리관(Dowex AG 1 X 4) 상에서 분리하였다. 각 부분을 열이온화질량분석법으로 각각의 동위원소비를 측정하였다. Nd-148과 Nd-(145+146) 방법 사이의 차이는 평균 2.07%로 나타났다. 이 결과를 U과 Pu동위원소를 이용한 무거운 원소방법 및 Cs-137의 파괴 감마분광측정법과 비교하였다. 연소도에 대한 U과 Pu의 동위원소 조성의존도와 동위원소사이의 상관관계를 그래프로서 설명하였다.

• Nuclear Engineering and Technology
• /
• 제47권7호
• /
• pp.924-933
• /
• 2015

The correlation of the isotopic composition of uranium, plutonium, neodymium, and cesium with the burnup for high burnup pressurized water reactor fuels irradiated in nuclear power reactors has been experimentally investigated. The total burnup was determined by Nd-148 and the fractional $^{235}U$ burnup was determined by U and Pu mass spectrometric methods. The isotopic compositions of U, Pu, Nd, and Cs after their separation from the irradiated fuel samples were measured using thermal ionization mass spectrometry. The contents of these elements in the irradiated fuel were determined through an isotope dilution mass spectrometric method using $^{233}U$, $^{242}Pu$, $^{150}Nd$, and $^{133}Cs$ as spikes. The activity ratios of Cs isotopes in the fuel samples were determined using gamma-ray spectrometry. The content of each element and its isotopic compositions in the irradiated fuel were expressed by their correlation with the total and fractional burnup, burnup parameters, and the isotopic compositions of different elements. The results obtained from the experimental methods were compared with those calculated using the ORIGEN-S code.

• Nuclear Engineering and Technology
• /
• 제33권4호
• /
• pp.375-385
• /
• 2001

The total burnup in the spent U$_3$Si/Al fuel samples from Hanaro reactor was determined by destructive methods using $^{148}$ Nd, the sum of $^{143}$ Nd and $^{144}$ Nd, the sum of $^{145}$ Nd and $^{146}$ Nd, and the sum of total Nd isotopes($^{143}$ Nd, $^{144}$ Nd, $^{145}$ Nd, $^{146}$ Nd, $^{148}$ Nd and $^{150}$ Nd) monitors. The fractional($^{235}$ U) turnup in the spent fuel samples was also determined by U and Pu mass spectrometric method. The samples were dissolved in a mixture of 4 M HCI and 10 M HNO$_3$ without any catalyst. The separation of U, Pu and Nd from the spiked and unspiked sample solutions was achieved by two sequential anion exchange separation methods. The isotope compositions of these elements, after their separation from the fuel samples were measured by mass spectrometry. The contents of the elements in the spent fuel samples were determined by isotope dilution mass spectrometric method(IDMS) using $^{233}$ U, $^{242}$ Pu and $^{150}$ Nd as spikes. The effective fission yield was calculated from the weighted fission yields averaged over the irradiation period. The difference between total turnup values determined by various Nd monitors were in the range of 1.8%.

• Nuclear Engineering and Technology
• /
• 제38권3호
• /
• pp.301-310
• /
• 2006

Destructive methods were used for the burnup determination of U-Zr alloy nuclear fuel irradiated in the High-flux Advanced Neutron Application Reactor (HANARO) at KAERI. The dissolution rate of unirradiated U-Zr alloy fuel in $HNO_3$/HF mixtures was investigated for the experimental conditions of a different temperature, and initial concentrations of HF and $HNO_3$. The irradiated U-Zr alloy fuel specimen was dissolved in a mixed acid condition of 3 M HNO3 and 1 M HF at $90^{\circ}C$ for 8 hours under reflux. The total burnup was determined from measurement of the Nd isotope burnup monitors. The method includes U, Pu, $^{148}Nd,\;^P{145}Nd+^{146}Nd,\;^{144}Nd+^{143}Nd$ and total Nd isotopes determination by the isotope dilution mass spectrometric method (IDMS) using triple spikes $(^{233}U,\;^{242}Pu\;and\;^{150}Nd)$. The effective fission yield was calculated from the weighted fission yields averaged over the irradiation period. The results are compared with that obtained by the destructive -spectrometric measurement of the $^{137}Cs$ monitor.