Abstract
The completion of the radiological inventory of a nuclear facility is hindered by some radionuclides that cannot be easily detected because of hardly measurable gamma lines or low abundance. 135Cs is a long-lived hard-to-measure radionuclide that needs chemical and radiochemical treatments to be measured. A preliminary separation approach to be combined with a non-radiometric assay is being proposed to quantify 135Cs by measuring 135Cs/137Cs isotopic ratio. To exploit this powerful tool, the removal of matrix contaminants, especially 135,137Ba isobaric interferences, remains paramount and challenging. The combined effect of co-precipitation followed by chromatographic separations is being explored in this work.
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07 January 2023
A Correction to this paper has been published: https://doi.org/10.1007/s10967-022-08730-2
References
INTERNATIONAL ATOMIC ENERGY AGENCY (1998) Radiological Characterization of Shut Down Nuclear Reactors for Decommissioning Purposes. Technical Reports Series No. 389, IAEA, Vienna
OECD (2013) Radiological Characterisation for Decommissioning of Nuclear Installations.Nucl Energy Agency72
Hou X (2007) Radiochemical analysis of radionuclides difficult to measure for waste characterization in decommissioning of nuclear facilities. J Radioanal Nucl Chem 273:43–48. https://doi.org/10.1007/s10967-007-0708-x
Mommaert C, Andrieu C, Desnoyers Y et al (2017) Radiological characterisation from a Waste and materials end-state perspective: Practices and Experience. OECD NEA 7373:100
Heinitz S, Kajan I, Schumann D (2022) How accurate are half-life data of long-lived radionuclides? Radiochim Acta. https://doi.org/10.1515/ract-2021-1135
Ling H, Chen L, Chen WM, Yun L (2019) The study of migration velocity of Cs-135 and Se-79 in intact rock. IOP Conf Ser Mater Sci Eng 592. https://doi.org/10.1088/1757-899X/592/1/012049
Helmer RG, Chechev VP (2007) 137Cs. Table de Radionuclides 0015:1–8
Nagy P, Vajda N, Sziklai-László I et al (2014) Determination of 135Cs in nuclear power plant wastes by ICP-MS and k0-NAA. J Radioanal Nucl Chem 300:615–627. https://doi.org/10.1007/s10967-013-2875-2
Chao JH, Tseng CL (1996) Determination of 135Cs by neutron activation analysis. Nucl Instruments Methods Phys Res sect A Accel Spectrometers. Detect Assoc Equip 372:275–279. https://doi.org/10.1016/0168-9002(95)01296-6
Snyder DC, Delmore JE, Tranter T et al (2012) Radioactive cesium isotope ratios as a tool for determining dispersal and re-dispersal mechanisms downwind from the Nevada Nuclear Security Site. J Environ Radioact 110:46–52. https://doi.org/10.1016/j.jenvrad.2012.01.019
Russell BC, Croudace IW, Warwick PE (2015) Determination of 135Cs and 137Cs in environmental samples: a review. Anal Chim Acta 890:7–20. https://doi.org/10.1016/j.aca.2015.06.037
Taylor VF, Evans RD, Cornett RJ (2008) Preliminary evaluation of 135Cs/137Cs as a forensic tool for identifying source of radioactive contamination. J Environ Radioact 99:109–118. https://doi.org/10.1016/j.jenvrad.2007.07.006
Delmore JE, Snyder DC, Tranter T, Mann NR (2011) Cesium isotope ratios as indicators of nuclear power plant operations. J Environ Radioact 102:1008–1011. https://doi.org/10.1016/j.jenvrad.2011.06.013
Croudace IW, Russell BC, Warwick PW (2017) Plasma source mass spectrometry for radioactive waste characterisation in support of nuclear decommissioning: a review. J Anal At Spectrom 32:494–526. https://doi.org/10.1039/c6ja00334f
Balaram V, Rahaman W, Roy P (2022) Recent advances in MC-ICP-MS applications in Earth and environmental sciences: Challenges and solutions. Geosyst Geoenvironment 1:100019. https://doi.org/10.1016/j.geogeo.2021.100019
Yamasaki SI, Akira T, Nanzyo M et al (2001) Background levels of trace and ultra-trace elements in soils of Japan. Soil Sci Plant Nutr 47:755–765. https://doi.org/10.1080/00380768.2001.10408440
Zhu L, Hou X, Qiao J (2020) Determination of Ultralow Level 135Cs and 135Cs/137Cs ratio in environmental samples by Chemical separation and Triple Quadrupole ICP-MS. Anal Chem 92:7884–7892. https://doi.org/10.1021/acs.analchem.0c01153
Eichrom T(2014) Strontium-89/90 in Water. https://www.eichrom.com/wp-content/uploads/2018/02/srw01-15_sr-water.pdf
Eichrom Technologies (2014) Analytical Procedure EICHROM’S VACUUM BOX SYSTEM (VBS). 1–3
Nagy S (2012) Chemistry and analysis of radionuclides. J Radioanal Nucl Chem 292:465–466. https://doi.org/10.1007/s10967-011-1433-z
Triskem International (2015) Product Sheet SR Resin. 33:3–6
Bio-Rad (2012) Cation Exchange Resins Instruction Manual. 3–18
Davies CM(2012) Determination of distribution coefficients for cationic exchange resin and optimisation of ion exchange chromatography for chromium separation for geological materials. A thesis submitted to The University of Manchester for the degree of Master of Philosophy in the Faculty of Engineering and Physical Sciences
Harrison JJ, Zawadzki A, Chisari R, Wong HKY (2011) Separation and measurement of thorium, plutonium, americium, uranium and strontium in environmental matrices. J Environ Radioact 102:896–900. https://doi.org/10.1016/j.jenvrad.2010.05.010
Eichrom T(2019) Americium, neptunium, plutonium, thorium, curium, uranium, and strontium in water. https://www.eichrom.com/wp-content/uploads/2018/02/ACW17-13_Am-Pu-U-Np-Th-Sr-Water-VBS.pdf. 12–24
Zhu L, Hou X, Qiao J (2021) Determination of 135Cs concentration and 135Cs/137Cs ratio in waste samples from nuclear decommissioning by chemical separation and ICP-MS/MS. Talanta 221:121637. https://doi.org/10.1016/j.talanta.2020.121637
Russell BC, Croudace IW, Warwick PE, Milton JA (2014) Determination of precise 135Cs/137Cs ratio in environmental samples using sector field inductively coupled plasma mass spectrometry. Anal Chem 86:8719–8726. https://doi.org/10.1021/ac501894a
Zheng J, Cao L, Tagami K, Uchida S (2016) Triple-quadrupole inductively coupled Plasma-Mass Spectrometry with a high-efficiency sample introduction system for Ultratrace determination of 135Cs and 137Cs in environmental samples at Femtogram levels. Anal Chem 88:8772–8779. https://doi.org/10.1021/acs.analchem.6b02150
Bu W, Tang L, Liu X et al (2019) Ultra-trace determination of the 135Cs/137Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples. J Anal At Spectrom 34:301–309. https://doi.org/10.1039/c8ja00380g
Zhu L, Hou X, Qiao J (2021) Determination of low-level 135Cs and 135Cs/137Cs atomic ratios in large volume of seawater by chemical separation coupled with triple-quadrupole inductively coupled plasma mass spectrometry measurement for its oceanographic applications. Talanta 226:122121. https://doi.org/10.1016/j.talanta.2021.122121
INTERNATIONAL ATOMIC ENERGY AGENCY (2004) Predisposal Management of Organic Radioactive Waste. Technical Reports Series No. 427, IAEA, Vienna
INTERNATIONAL ATOMIC ENERGY AGENCY (2002) Application of Ion Exchange Processes for the Treatment of Radioactive Waste and Management of Spent Ion Exchangers. Technical Reports Series No. 408, IAEA, Vienna
INTERNATIONAL ATOMIC ENERGY AGENCY (2020) Underground Disposal Concepts for small inventories of Intermediate and High Level Radioactive Waste. TECDOC-1934. IAEA, Vienna
Acknowledgements
The authors acknowledge the Collaborative Doctoral Partnership between Politecnico di Milano and European Commission’s Joint Research Centre – Ispra site.
This work was presented at the 19th Radiochemical Conference (RadChem 2022) held in Mariánské Lázně, Czech Republic, on 15–20 May 2022.
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Galluccio, F., Bilancia, G., Mossini, E. et al. Preliminary development of a radiochemical separation method to determine 135Cs and 135Cs/137Cs isotopic ratio by a non-radiometric technique. J Radioanal Nucl Chem 332, 1489–1498 (2023). https://doi.org/10.1007/s10967-022-08685-4
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DOI: https://doi.org/10.1007/s10967-022-08685-4