• Title/Summary/Keyword: Isotope ratios

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Attenuation of Background Molecular Ions and Determination of Isotope Ratios by Inductively Coupled Plasma Mass Spectrometry at Cool Plasma Condition

  • 박창준
    • Bulletin of the Korean Chemical Society
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    • v.18 no.7
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    • pp.706-710
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    • 1997
  • Isotope ratios of K, Ca, Cr and Fe are measured at cool plasma condition generated using high carrier flow rate and relatively low RF power of 900 W. Background molecular ions are suppressed to below 100 counts which give isobaric interference to the analytes. The background ions show different attenuation characteristics at increased carrier flow rate and hence for each element different carrier flow rate should be used to measure isotope ratios without isobaric interference. Isotope ratios are measured at both scan and peak-hopping modes and compared with certified or accepted ratios. The measured isotope ratios show some mass discrimination against low mass due to low ion energy induced from a copper shield to eliminate capacitive coupling of plasma with load coil.

Accurate Measurement of Isotope Amount Ratios of Lead in Bronze with Multicollector Inductively Coupled Plasma Mass Spectrometry

  • Lee, Kyoung-Seok;Kim, Jin-Il;Yim, Yong-Hyeon;Hwang, Euijin;Kim, Tae Kyu
    • Mass Spectrometry Letters
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    • v.4 no.4
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    • pp.87-90
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    • 2013
  • Isotope amount ratios of lead in a bronze sample have been successfully determined using multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS). Matrix separation conditions were tested and optimized using ion exchange chromatography with anion-exchange resin, AG1-X8, and sequential elution of the 0.5 M HBr and 7 M $HNO_3$ to separate lead from very high contents of copper and tin in bronze matrix. Mercury was also removed efficiently in the optimized separation condition. The instrumental isotope fractionation of lead in the MC-ICP-MS measurement was corrected by the external standard sample bracketing method using an external standard, NIST SRM 981 lead common isotope ratio standard followed by correction of procedure blank to obtain reliable isotope ratios of lead. The isotope ratios, $^{206}Pb/^{204}Pb$, $^{207}Pb/^{204}Pb$, $^{208}Pb/^{204}Pb$, and $^{208}Pb/^{206}Pb$, of lead were determined as $18.0802{\pm}0.0114$, $15.5799{\pm}0.0099$, $38.0853{\pm}0.0241$, and $2.1065{\pm}0.0004$, respectively, and the determined isotope ratios showed good agreement with the reference values of an international comparison for the same sample within the stated uncertainties

Sensitivity studies on a novel nuclear forensics methodology for source reactor-type discrimination of separated weapons grade plutonium

  • Kitcher, Evans D.;Osborn, Jeremy M.;Chirayath, Sunil S.
    • Nuclear Engineering and Technology
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    • v.51 no.5
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    • pp.1355-1364
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    • 2019
  • A recently published nuclear forensics methodology for source discrimination of separated weapons-grade plutonium utilizes intra-element isotope ratios and a maximum likelihood formulation to identify the most likely source reactor-type, fuel burnup and time since irradiation of unknown material. Sensitivity studies performed here on the effects of random measurement error and the uncertainty in intra-element isotope ratio values show that different intra-element isotope ratios have disproportionate contributions to the determination of the reactor parameters. The methodology is robust to individual errors in measured intra-element isotope ratio values and even more so for uniform systematic errors due to competing effects on the predictions from the selected intra-element isotope ratios suite. For a unique sample-model pair, simulation uncertainties of up to 28% are acceptable without impeding successful source-reactor discrimination. However, for a generic sample with multiple plausible sources within the reactor library, uncertainties of 7% or less may be required. The results confirm the critical role of accurate reactor core physics, fuel burnup simulations and experimental measurements in the proposed methodology where increased simulation uncertainty is found to significantly affect the capability to discriminate between the reactors in the library.

Carbon Stable Isotope Ratios of Phytoplankton and Benthic Diatoms in Lake Katanuma with Reference to Those of Other Lakes

  • Kikuchi, Eisuke;Takagi, Shigeto;Shikano, Shuichi;Hideyuki, Doi
    • Korean Journal of Ecology and Environment
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    • v.38 no.spc
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    • pp.8-11
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    • 2005
  • Carbon stable isotope ratios of producers varied in lake ecosystems. In tile present study, we tried to estimate the seasonal variations of carbon isotope ratios of phytoplankton and benthic diatoms in a strongly acidic lake ecosystem. Lake Katanuma is a volcanic, strongly acidic lake (average pH of 2.2), located in Miyagi, Japan. Only two algal species dominate in Lake Katanuma; Pinnularia acidojaponica as a benthic diatom, and Chlamydomonas acidophila as a green alga. Carbon isotope values of P. acidojaponica varied seasonally, while those of particulate organic matter, which were mainly composed of C. acidophila remained fairly stable. The differences suggested that $CO_2$ gas was more frequently limited for P. acidojaponica than C. acidophila, since high density patches of benthic diatoms were sometimes observed on the lake sediment. Generally, carbon concentration mechanisms (CCMs)of microalgae can fix bicarbonate in lakes, and affect the carbon isotope values of microalgae. While, in Lake Katanuma, CCMs of the microalgae may scarcely function because of high $CO_2$ gas concentration and low pH. This is the reason for low seasonal amplitude of carbon isotope values of phytoplankton relative to those in other lakes.

The Origin and Biogeochemistry of Organic Matter in Surface Sediments of Lake Shihwa and Lake Hwaong

  • Won, Eun-Ji;Cho, Hyen-Goo;Shin, Kyung-Hoon
    • Ocean Science Journal
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    • v.42 no.4
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    • pp.223-230
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    • 2007
  • To understand the origin and biogeochemistry of the organic matter in surface sediments of Lake Shihwa and Lake Hwaong, organic nitrogen, inorganic nitrogen, labile organic carbon, and residual organic carbon contents as well as stable isotope ratios for carbon and nitrogen were determined by KOBr-KOH treatment. Ratios of organic carbon to organic nitrogen $(C_{org}/N_{org})$ (mean = 24) were much higher than ratios of organic carbon to total nitrogen $(C_{org}/N_{tot})$ (mean= 12), indicating the presence of significant amounts of inorganic nitrogen in the surface sediments of both lakes. Stable isotope ratios for organic nitrogen were, on average, $5.2\%_{\circ}$ heavier than ratios of inorganic nitrogen in Lake Shihwa, but those same ratios were comparable in Lake Hwaong. This might be due to differences in the origin or the degree of degradation of sedimentary organic matter between the two lakes. In addition, stable isotope ratios for labile organic carbon were, on average, $1.4\%_{\circ}$ heavier than those for residual organic carbon, reflecting the preferential oxidation of $^{13}C$-enriched organic matter. The present study demonstrates that KOBr-KOH treatment of sedimentary organic matter can provide valuable information for understanding the origin and degradation state of organic matter in marine and brackish sediments. This also suggests that the ratio of $(C_{org}/N_{org})$ and stable isotope ratios for organic nitrogen can be used as indexes of the degree of degradation of organic matter.

Determination of Li by Isotope Dilution Inductively Coupled Plasma Mass Spectrometry

  • Park, Chang J.;Chung, Bag S.
    • Analytical Science and Technology
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    • v.8 no.4
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    • pp.427-434
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    • 1995
  • Inductively coupled plasma mass spectrometry combined with the isotope dilution method is used for the determination of lithium. The isotope dilution method is based on the addition of a known amount of enriched isotope (spike) to a sample. The analyte concentration is obtained by measuring the altered isotope ratio. The spike solution is calibrated through so called reverse isotope dilution with a primary standard. The spike calibration is an important step to minimize error in the determined concentration. It has been found essential to add spike to a sample and the primary standard so that the two isotope ratios should be as dose as possible. Since lithium is neither corrosive nor toxic, lithium is used as a chemical tracer in the nuclear power plants to measure feedwater flow rate. 99.9% $^7Li$ was injected into a feedwater line of an experimental system and sample were taken downstream to be spiked with 95% $^6Li$ for the isotope dilution measurements. Effects of uncertainties in the spike enrichment and isotope ratio measurement error at various spike-to-sample ratios are presented together with the flow rate measurement results in comparison with a vortex flow meter.

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Experimental validation of a nuclear forensics methodology for source reactor-type discrimination of chemically separated plutonium

  • Osborn, Jeremy M.;Glennon, Kevin J.;Kitcher, Evans D.;Burns, Jonathan D.;Folden, Charles M. III;Chirayath, Sunil S.
    • Nuclear Engineering and Technology
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    • v.51 no.2
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    • pp.384-393
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    • 2019
  • An experimental validation of a nuclear forensics methodology for the source reactor-type discrimination of separated weapons-useable plutonium is presented. The methodology uses measured values of intra-element isotope ratios of plutonium and fission product contaminants. MCNP radiation transport codes were used for various reactor core modeling and fuel burnup simulations. A reactor-dependent library of intra-element isotope ratio values as a function of burnup and time since irradiation was created from the simulation results. The experimental validation of the methodology was achieved by performing two low-burnup experimental irradiations, resulting in distinct fuel samples containing sub-milligram quantities of weapons-useable plutonium. The irradiated samples were subjected to gamma and mass spectrometry to measure several intra-element isotope ratios. For each reactor in the library, a maximum likelihood calculation was utilized to compare the measured and simulated intra-element isotope ratio values, producing a likelihood value which is proportional to the probability of observing the measured ratio values, given a particular reactor in the library. The measured intra-element isotope ratio values of both irradiated samples and its comparison with the simulation predictions using maximum likelihood analyses are presented. The analyses validate the nuclear forensics methodology developed.

Determination of the Origin of Particulate Organic Matter at the Estuary of Youngsan River using Stable Isotope Ratios (${\delta}^{13}C$, ${\delta}^{15}N$) (탄소 및 질소 안정동위원소 비를 이용한 영산강하구역 유기물 기원 추정 연구)

  • Lee, Yeon-Jung;Jeong, Byung-Kwan;Shin, Yong-Sik;Kim, Sung-Hwan;Shin, Kyung-Hoon
    • Korean Journal of Ecology and Environment
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    • v.46 no.2
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    • pp.175-184
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    • 2013
  • Organic carbon and total nitrogen stable isotope ratios of suspended materials were determined at 3 stations (from Mongtan Bridge to Youngsan river estuary barrage) (n=6, each) from November 2008 to August 2009, in order to understand the origin of particulate organic matter at the Estuary of Youngsan River. Allochthonous organic matter, ammonia-N and silicate were increased after heavy rain (in August). Carbon isotope ratios were significantly different between stations in November and August, and it was possible to determine the origin of organic matter. The heavier nitrogen isotope ratios, as well as higher phosphate concentrations, were found in November than other sampling times. Livestock wastewater and farmland input was likely the main causes of these high values. In addition, YS3 station, the nearest site to estuary barrage, appears to be affected by a substantial amount of livestock wastewater and farmland input, considering that nitrogen isotope ratios were heavier than those at the upper sites. These results suggest that the analysis of stable isotope ratios is a simple but useful tool for the determination of organic matter origin in aquatic environments.

Study on the Chemical Composition and Lead Isotope Ratios of Lead Glaze Used on Blue Tiles from Gyeoungbokgung Palace (경복궁 청기와에 사용된 납유의 화학조성과 납동위원소 특성연구)

  • So Jin Kim;Young Do Kim
    • Economic and Environmental Geology
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    • v.57 no.3
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    • pp.343-352
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    • 2024
  • Composition analysis and lead isotope ratio analysis were conducted to determine the coloring machanism on lead glaze used in Gyeongbokgung Palace and the provenance of the lead used as a flux. 31 blue tiles were classified into green, blue, and yellow. The chemical analysis of lead glazes on the blue tiles revealed that Pb, Si, and Cu were the main components, and trace amounts of Fe, Ca, Mg, and Al were detected. The Cu content was high in blue lead glaze, while Cu was not detected in yellow or brown lead glaze which instead had high Fe content. Therefore, it was found that lead was used as a flux and copper oxide as a coloring agent in the production of lead glaze. In addition, the lead isotope ratios of the lead glaze used in the blue tiles of Gyeongbokgung palace were plotted in zone 3 on the distribution map of lead isotope ratios on the Korean Peninsula, which includes Chungcheong-do and Jeolla-do. It is presumed that the flux for the lead glaze was sourced from galena found in these regions. The lead isotope ratios of the green glaze from the Three Kingdoms and Unified Silla period were mostly located outside the Korean Peninsula, showing that the provenance of lead had changed. In particular, the lead isotope ratios of the green glaze from the Three Kingdoms and Unified Silla period suggest exchange with neighboring countries. Also the lead isotope ratios of the green glazes from the same temple are different, so it is believed that they were made at different times or in different workshops.

Accurate determination of minor isotope ratios in individual plutonium-uranium mixed particles by thermal ionization mass spectrometry

  • Lee, Chi-Gyu;Park, Jinkyu;Lim, Sang Ho
    • Nuclear Engineering and Technology
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    • v.50 no.1
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    • pp.140-144
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    • 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.