Ultra-trace determination of the <sup>135</sup>Cs/<sup>137</sup>Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples

Bu, Wenting; Tang, Lei; Liu, Xuemei; Wang, Zhongtang; Fukuda, Makoto; Zheng, Jian; Aono, Tatsuo; Hu, Sheng; Wang, Xiaolin

doi:10.1039/c8ja00380g

Cited by 25 publications

(47 citation statements)

References 34 publications

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“…The overall decontamination factors of 4 × 10 7 for Ba, 4 × 10 6 for Li, 4 × 10 5 for Mo, 3 × 10 5 for Sn, and 2 × 10 5 for Sb were achieved, which are better or comparable compared to the reported values using combined chromatographic purification (AMP-PAN, AGMP-1 M, and AG 50W-X8). 14,18 In consideration of all steps including ICP-MS measurement, the entire analysis of a batch of 8 samples can be completed within 3 days. The overall chemical yields of 135 Cs were measured by counting the 137 Cs in the original samples and the final separated cesium solution by gamma spectrometry to be more than 85% for soils from Sweden and Ukraine.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Determination of Ultralow Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

2020

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An analytical method was developed for the determination of ultralow level 135 Cs in environmental samples by chromatographic separation of cesium with AMP-PAN and AG50W-X8 columns and sensitive measurement of cesium isotopes with triple quadrupole inductively coupled plasma mass spectrometry (ICP-MS/MS). Cesium was simply released by acid leaching using aqua regia from environmental solid samples and preconcentrated on AMP-PAN column. The cesium adsorbed on the column was effectively eluted with NH 4 Cl solution without dissolving the AMP. The excessive amount of NH 4 Cl in the eluate was removed by sublimation in the presence of small amount of LiCl. The remaining barium and other interfering elements such as Mo, Sn, Sb, and Li were efficiently removed using cation exchange chromatography (AG50W-X8). The decontamination factors of this procedure are above 4 × 10 7 for barium and 4 × 10 5 for molybdenum; the chemical yields of cesium are more than 85% for samples of less than 10 g. This method enables to separate cesium from large size of samples for the determination of ultralow level 135 Cs, avoiding the problem of removal of a huge amount of Mo in the dissolved AMP. Intrinsic 137 Cs in the environmental samples measured by gamma spectrometry before and after separation was used as internal isotope dilution standard for quantitative determination of 135 Cs without complete release and recover of radiocesium. The interference of barium ( 135 Ba and 137 Ba) to the ICP-MS measurement of 135 Cs and 137 Cs was further suppressed to 8 × 10 −5 by using N 2 O as the reaction gas in ICP-MS/MS at a flow rate of 0.7 mL/min, so a total suppression of 2 × 10 −12 for Ba was achieved, making the isobaric interference of Ba isotopes to the measurement of 135 Cs and 137 Cs in environmental samples negligible. A detection limit of 9.1 × 10 −17 g/g for 135 Cs and 137 Cs was achieved for 60 g samples. The developed method was validated by analysis of standard reference materials and successfully applied for the determination of 135 Cs concentrations and 135 Cs/ 137 Cs ratios in soil samples collected from Denmark, Sweden, and Ukraine. The 135 Cs/ 137 Cs isotopic ratios in Danish soil (2.08−2.68) were significantly higher than that from Sweden and Ukraine (0.65−0.71), indicating different sources of radiocesium. This work demonstrated the application of 135 Cs/ 137 Cs as a unique fingerprint for discriminating the sources of radioactive contamination and estimating their contribution to the total inventory, which will be useful for nuclear forensics and environmental tracer studies.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Determination of Ultralow Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

2020

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“…Sector field inductively coupled plasmamass spectrometry (SF-ICP-MS), 20,21 electrothermal vaporization-inductively coupled plasma-mass spectrometry (ETV-ICP-MS), 22 triple quadrupole inductively coupled plasma-mass spectrometry (ICP-QQQ-MS), 6,9,10 resonance ionization mass spectrometry (RIMS), 23 and thermal ionization mass spectrometry (TIMS) 7,24−29 have been used for this purpose. Due to the serious isobaric interference of 135 16 O + ), high decontamination factors for Ba and other interfering elements are needed prior to the spectrometric measurement. Due to the high elimination of Ba using a dynamic reaction cell and significant improvement of abundance sensitivity, ICP-QQQ-MS has been successfully applied for measurement of 135 Cs/ 137 Cs ratios in various environmental samples.…”

mentioning

confidence: 99%

Determination of Ultratrace Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Small Volume Seawater by Chemical Separation and Thermal Ionization Mass Spectrometry

Zhu

Hou

et al. 2020

Anal. Chem.

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“…It has to be noted that presently, there are no certified reference materials for the 135 Cs/ 133 Cs nor for the 135 Cs/ 137 Cs isotopic ratio available. However, the 135 Cs/ 137 Cs was already measured in various IAEA and NIST reference materials by various groups (Snow et al, 2015;Snow and Snyder, 2016;Bu et al, 2018Bu et al, , 2019Zhu et al, 2020b) and their consensus values now are commonly used for method development and validation. An important validation step in the development of 135 Cs measurement is to reproduce the given values for the 137 Cs concentration.…”

Section: Fission Products With Stable Isobaric Backgroundmentioning

confidence: 99%

Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers

et al. 2022

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Recent major advances in Accelerator Mass Spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) regarding detection efficiency and isobar suppression have opened possibilities for the analysis of additional long-lived radionuclides at ultra-low environmental concentrations. These radionuclides, including 233U, 135Cs, 99Tc, and 90Sr, will become important for oceanographic tracer application due to their generally conservative behavior in ocean water. In particular, the isotope ratios 233U/236U and 137Cs/135Cs have proven to be powerful fingerprints for emission source identification as they are not affected by elemental fractionation. Improved detection efficiencies allowed us to analyze all major long-lived actinides, i.e., 236U, 237Np, 239,240Pu, 241Am as well as the very rare 233U, in the same 10 L water samples of a depth profile from the northwest Pacific Ocean. For this purpose, a simplified and very flexible chemical purification procedure based on extraction chromatography (a single UTEVA® column) was implemented which can be extended by a DGA® column for Am purification. The procedure was validated with the reference materials IAEA-381/385. With the additional increase in ionization efficiency expected for the extraction of actinides as fluoride molecules from the AMS ion source, a further reduction of chemical processing may become possible. This method was successfully applied to an exemplary set of air filter samples. In order to determine the quantitative 237Np concentration reliably, a 236Np spike material is being developed in collaboration with the University of Tsukuba, Japan. Ion-Laser Interaction Mass Spectrometry (ILIAMS), a novel technique for the efficient suppression of stable isobaric background, has been developed at VERA and provides unprecedented detection sensitivity for the fission fragments 135Cs, 99Tc, and 90Sr. The corresponding setup is fully operational now and the isobar suppression factors of >105 achieved, in principle, allow for the detection of the mentioned radionuclides in the environment. Especially for 90Sr analysis, this new approach has already been validated for selected reference materials (e.g., IAEA-A-12) and is ready for application in oceanographic studies. We estimate that a sample volume of only (1–3) L ocean water is sufficient for 90Sr as well as for 135Cs analysis, respectively.

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Ultra-trace determination of the ¹³⁵Cs/¹³⁷Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples

Abstract: A new method was developed for determination of the 135Cs/137Cs isotopic ratio at the femtogram level in environmental samples.

Cited by 25 publications

References 34 publications

Determination of Ultralow Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

Determination of Ultralow Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

Determination of Ultratrace Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Small Volume Seawater by Chemical Separation and Thermal Ionization Mass Spectrometry

Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers

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Ultra-trace determination of the 135Cs/137Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples

Abstract: A new method was developed for determination of the 135Cs/137Cs isotopic ratio at the femtogram level in environmental samples.

Cited by 25 publications

References 34 publications

Determination of Ultralow Level 135Cs and 135Cs/137Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

Determination of Ultralow Level 135Cs and 135Cs/137Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

Determination of Ultratrace Level 135Cs and 135Cs/137Cs Ratio in Small Volume Seawater by Chemical Separation and Thermal Ionization Mass Spectrometry

Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers

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Ultra-trace determination of the ¹³⁵Cs/¹³⁷Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples

Determination of Ultralow Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

Determination of Ultralow Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Environmental Samples by Chemical Separation and Triple Quadrupole ICP-MS

Determination of Ultratrace Level ¹³⁵Cs and ¹³⁵Cs/¹³⁷Cs Ratio in Small Volume Seawater by Chemical Separation and Thermal Ionization Mass Spectrometry