• Title/Summary/Keyword: Isotopic Analysis

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Geochemical and S isotopic studies of pollutant evolution in groundwater after acid in situ leaching in a uranium mine area in Xinjiang

  • Zhenzhong Liu;Kaixuan Tan;Chunguang Li;Yongmei Li;Chong Zhang;Jing Song;Longcheng Liu
    • Nuclear Engineering and Technology
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    • v.55 no.4
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    • pp.1476-1484
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    • 2023
  • Laboratory experiments and point monitoring of reservoir sediments have proven that stable sulfate reduction (SSR) can lower the concentrations of toxic metals and sulfate in acidic groundwater for a long time. Here, we hypothesize that SSR occurred during in situ leaching after uranium mining, which can impact the fate of acid groundwater in an entire region. To test this, we applied a sulfur isotope fractionation method to analyze the mechanism for natural attenuation of contaminated groundwater produced by acid in situ leaching of uranium (Xinjiang, China). The results showed that δ34S increased over time after the cessation of uranium mining, and natural attenuation caused considerable, area-scale immobilization of sulfur corresponding to retention levels of 5.3%-48.3% while simultaneously decreasing the concentration of uranium. Isotopic evidence for SSR in the area, together with evidence for changes of pollutant concentrations, suggest that area-scale SSR is most likely also important at other acid mining sites for uranium, where retention of acid groundwater may be strengthened through natural attenuation. To recapitulate, the sulfur isotope fractionation method constitutes a relatively accurate tool for quantification of spatiotemporal trends for groundwater during migration and transformation resulting from acid in situ leaching of uranium in northern China.

Determination of the Isotope Ratio for Metal Samples Using a Laser Ablation/Ionization Time-of-flight Mass Spectrometry

  • Song, Kyu-Seok;Cha, Hyung-Ki;Kim, Duk-Hyeon;Min, Ki-Hyun
    • Bulletin of the Korean Chemical Society
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    • v.25 no.1
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    • pp.101-105
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    • 2004
  • The laser ablation/ionization time-of-flight mass spectrometry is applied to the isotopic analysis of solid samples using a home-made instrument. The technique is convenient for solid sample analysis due to the onestep process of vaporization and ionization of the samples. The analyzed samples were lead, cadmium, molybdenum, and ytterbium. To optimize the analytical conditions of the technique, several parameters, such as laser energy, laser wavelength, size of the laser beam on the samples surface, and high voltages applied on the ion source electrodes were varied. Low energy of laser light was necessary to obtain the optimal mass resolution of spectra. The 532 nm light generated mass spectra with the higher signal-to-noise ratio compared with the 355 nm light. The best mass resolution obtained in the present study is ~1,500 for the ytterbium.

Uranium Analysis in Aqueous Samples by Selective Extraction and Photon-Electron Rejecting Alpha Liquid Scintillation $(PERALS^\circledR)$ Spectrometry

  • Shin, Hyun-Sang;Lee, Myung-Ho;Park, Geun-Sik;Lee, Chang-Woo
    • Nuclear Engineering and Technology
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    • v.31 no.5
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    • pp.445-454
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    • 1999
  • This work describes the adaptation of extractive scintillation by URAE $X^{TM}$ with a photon-electron rejecting alpha liquid scintillation (PERAL $S^{)}$ spectrometer to the analysis of uranium in aqueous samples. The extraction efficiency of the system was evaluated under varing chemical conditions including pH, and sample-cocktail volume ratio. Isotopic information from the (PERAL $S^{)}$ spectrum of natural uranium was obtained using a curve fitting routine. Comparisons of the result with that obtained from alpha spectrometry method using ion implanted silicon detector showed good agreement.t.

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Theoretical study of the Reactions of $H+H_2$ and Its Isotopic Variants Inter- and Intramolecular Isotope effect

  • 성주범
    • Bulletin of the Korean Chemical Society
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    • v.19 no.6
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    • pp.634-641
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    • 1998
  • Quasiclassical trajectory calculations were carried out for the reactions of $H+H_2$ (V=O, J=O) and its isotope variants on the Siegbahn-Liu-Truhlar-Horowitz potential energy surface for the relative energies E between 6 and 150 kcal/mol. The goal of the work was to understand the inter- and intramolecular isotope effects. We examine the relative motion of reactants during the collision using the method of analysis that monitors the intermolecular properties (internuclear distances, geometry of reactants, and final product). As in other works, we find that the heavier the incoming atom is, the greater the reaction cross section is at the same collision energy. Using the method of analysis we prove that the intermolecular isotope effect is contributed mainly by differences in reorientation due to the different reduced masses. We show that above E=30 kcal/mol recrossing also contributes to the intermolecular isotope effect. For the intramolecular isotope effect in the reactions of H+HD and T+HD, we reach the same conclusions as in the systems of $O(^3P)+HD$, F+HD, and Cl+HD. That is, the intramolecular isotope effect below E=150 kcal/mol is contributed by reorientation, recrossing, and knockout type reactions.

Validation of UNIST Monte Carlo code MCS for criticality safety calculations with burnup credit through MOX criticality benchmark problems

  • Ta, Duy Long;Hong, Ser Gi;Lee, Deokjung
    • Nuclear Engineering and Technology
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    • v.53 no.1
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    • pp.19-29
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    • 2021
  • This paper presents the validation of the MCS code for critical safety analysis with burnup credit for the spent fuel casks. The validation process in this work considers five critical benchmark problem sets, which consist of total 80 critical experiments having MOX fuels from the International Criticality Safety Benchmark Evaluation Project (ICSBEP). The similarity analysis with the use of sensitivity and uncertainty tool TSUNAMI in SCALE was used to determine the applicable benchmark experiments corresponding to each spent fuel cask model and then the Upper Safety Limits (USLs) except for the isotopic validation were evaluated following the guidance from NUREG/CR-6698. The validation process in this work was also performed with the MCNP6 for comparison with the results using MCS calculations. The results of this work showed the consistence between MCS and MCNP6 for the MOX fueled criticality benchmarks, thus proving the reliability of the MCS calculations.

Spent fuel characterization analysis using various nuclear data libraries

  • Calic, Dusan;Kromar, Marjan
    • Nuclear Engineering and Technology
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    • v.54 no.9
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    • pp.3260-3271
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    • 2022
  • Experience shows that the solution to waste management in any national programme is lengthy and burdened with uncertainties. There are several uncertainties that contribute to the costs associated with spent fuel management. In this work, we have analysed the impact of the current nuclear data on the isotopic composition of the spent fuel and consequently their influence on the main spent fuel observables such as decay heat, activity, neutron multiplication factor, and neutron and photon source terms. Nuclear libraries based on the most general nuclear data ENDF/B-VII.0, ENDF/B-VII.1, ENDF/B-VIII.0 and JEFF-3.3 are considered. A typical NPP Krško fuel assembly is analysed using the Monte Carlo code Serpent 2. The analysis considers burnup of up to 60 GWd/tU and cooling times of up to 100 years. The comparison of results showed significant differences, which should be taken into account when selecting the library and evaluating the uncertainty in determining the characteristics of the spent fuel.

Speed Improvement of an FTICR Mass Spectra Analysis Program by Simple Modifications

  • Jeon, Sang-Hyun;Chang, Hyeong-Soo;Hur, Man-Hoi;Kwon, Kyung-Hoon;Kim, Hyun-Sik;Yoo, Jong-Shin;Kim, Sung-Hwan;Park, Soo-Jin;Oh, Han-Bin
    • Bulletin of the Korean Chemical Society
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    • v.30 no.9
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    • pp.2061-2065
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    • 2009
  • Two simple algorithm modifications are made to the THRASH data retrieval program with the aim of improving analysis speed for complex Fourier transform ion cyclotron resonance (FTICR) mass spectra. Instead of calculating the least-squares fit for every charge state in the backup charge state determination algorithm, only some charge states are pre-selected based on the plausibility values obtained from the FT/Patterson analysis. Second, a modification is made to skip figure-of-merit (FOM) calculations in the central m/z region between two neighboring peaks in isotopic cluster distributions, in which signal intensities are negligible. These combined modifications result in a significant improvement in the analysis speed, which reduces analysis time as much as 50% for ubiquitin (8.6 kDa, 76 amino acids) FTICR MS and MS/MS spectra at the reliability (RL) value = 0.90 and five pre-selected charge states with minimal decreases in data analysis quality (Table 3).

Recent Developments in Nuclear Forensic and Nuclear Safeguards Analysis Using Mass Spectrometry

  • Song, Kyuseok;Park, Jong-Ho;Lee, Chi-Gyu;Han, Sun-Ho
    • Mass Spectrometry Letters
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    • v.7 no.2
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    • pp.31-40
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    • 2016
  • The analysis of nuclear materials and environmental samples is an important issue in nuclear safeguards and nuclear forensics. An analysis technique for safeguard samples has been developed for the detection of undeclared nuclear activities and verification of declared nuclear activities, while nuclear forensics has been developed to trace the origins and intended use of illicitly trafficked nuclear or radioactive materials. In these two analytical techniques, mass spectrometry has played an important role in determining the isotope ratio of various nuclides, contents of trace elements, and production dates. These two techniques typically use similar analytical instruments, but the analytical procedure and the interpretation of analytical results differ depending on the analytical purpose. The isotopic ratio of the samples is considered the most important result in an environmental sample analysis, while age dating and impurity analysis may also be important for nuclear forensics. In this review, important aspects of these techniques are compared and the role of mass spectrometry, along with recent progress in related technologies, are discussed.

NEW DEVELOPMENT OF HYPERGAM AND ITS TEST OF PERFORMANCE FOR γ-RAY SPECTRUM ANALYSIS

  • Park, B.G.;Choi, H.D.;Park, C.S.
    • Nuclear Engineering and Technology
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    • v.44 no.7
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    • pp.781-790
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    • 2012
  • The HyperGam program was developed for the analysis of complex HPGe ${\gamma}$-ray spectra. The previous version of HyperGam was mainly limited to the analysis of ${\gamma}$-ray peaks and the manual logging of the result. In this study, it is specifically developed into a tool for the isotopic analysis of spectra. The newly developed features include nuclide identification and activity determination. An algorithm for nuclide identification was developed to identify the peaks in the spectrum by considering the yield, efficiency, energy and peak area for the ${\gamma}$-ray lines emitted from the radionuclide. The detailed performance of nuclide identification and activity determination was accessed using the IAEA 2002 set of test spectra. By analyzing the test spectra, the numbers of radionuclides identified truly (true hit), falsely (false hit) or missed (misses) were counted and compared with the results from the IAEA 2002 tests. The determined activities of the radionuclides were also compared for four test spectra of several samples. The result of the performance test is promising in comparison with those of the well-known software packages for ${\gamma}$-ray spectrum analysis.

Activation analysis of targets and lead in a lead slowing down spectrometer system

  • Lee, Yongdeok;Kim, Jeong Dong;Ahn, Seong Kyu;Park, Chang Je
    • Nuclear Engineering and Technology
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    • v.50 no.1
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    • pp.182-189
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    • 2018
  • A neutron generation system was developed to induce fissile fission in a lead slowing down spectrometer (LSDS) system. The source neutron is one of the key factors for LSDS system work. The LSDS was developed to quantify the isotopic contents of fissile materials in spent nuclear fuel and recycled fuel. The source neutron is produced at a multilayered target by the (e,${\gamma}$)(${\gamma}$,n) reaction and slowed down at the lead medium. Activation analysis of the target materials is necessary to estimate the lifetime, durability, and safety of the target system. The CINDER90 code was used for the activation analysis, and it can involve three-dimensional geometry, position dependent neutron flux, and multigroup cross-section libraries. Several sensitivity calculations for a metal target with different geometries, materials, and coolants were done to achieve a high neutron generation rate and a low activation characteristic. Based on the results of the activation analysis, tantalum was chosen as a target material due to its better activation characteristics, and helium gas was suggested as a coolant. In addition, activation in a lead medium was performed. After a distance of 55 cm from the lead surface to the neutron incidence, the neutron intensity dramatically decreased; this result indicates very low activation.