Microwave-Assisted Sample Treatment in a Fully Automated Flow-Based Instrument:  Oxidation of Reduced Technetium Species in the Analysis of Total Technetium-99 in Caustic Aged Nuclear Waste Samples

Egorov, Oleg B.; O’Hara, Matthew J.; Grate, Jay W.

doi:10.1021/ac0497196

Cited by 24 publications

(32 citation statements)

References 43 publications

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“…Trace/matrix separation, which is performed off-line or on-line, is used more and more frequently for isotope ratio measurements of long-lived radionuclides in order to avoid possible isobaric interferences, matrix effects and to reduce the detection limits. For example, Egorov et al [44] developed fully automated flow-based equipment for the microwave-assisted treatment of liquid samples for the oxidation (using peroxydisulfate) of reduced technetium species to pertechnetate in the analysis of 99 Tc by ICP-MS in nuclear waste samples from the Hanford site.…”

Section: Introductionmentioning

confidence: 99%

Inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS for isotope analysis of long-lived radionuclides

Becker

2005

International Journal of Mass Spectrometry

113

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Section: Introductionmentioning

confidence: 99%

Inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS for isotope analysis of long-lived radionuclides

Becker

2005

International Journal of Mass Spectrometry

113

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“…Step 6 involves performing an exhaustive oxidation of the system to convert any soluble n-Tc to pertechnetate. The method of exhaustive oxidation consists of microwave digestion of an acidified solution in the presence of sodium persulfate as described by Egorov et al (2004Egorov et al ( , 2012.…”

Section: Approach/discussionmentioning

confidence: 99%

Protocol for Identifying the Presence of and Understanding the Nature of Soluble, Non-pertechnetate Technetium in Hanford Tank Supernatants

Rapko¹

2014

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Executive SummaryThe purpose of this report is twofold: first, to propose a test protocol for identifying the presence of soluble, non-pertechnetate Tc (n-Tc) in alkaline, high ionic strength, Hanford tank supernatants, and second, to evaluate various methods of obtaining information about the nature of the identified, non-pertechnetate species.The proposed protocol addresses three questions: 1) is n-Tc present and what fraction of the total soluble Tc is present in this form, 2) is there an interference at m/e 99 in the inductively coupled plasma mass spectrometry (ICP-MS) that gives false positives in a test for n-Tc, and 3) is there another isotope that could act as an interference in a test for n-Tc by liquid scintillation counting.For ALARA (as low as reasonably achievable) reasons, the protocol involves an initial Cs decontamination by contact with the Cs selective IE-911 ion exchanger. It is recommended that the Cs-depleted supernatant be spiked with a non-Tc-99 source (likely Tc-99m) of pertechnetate to allow an independent assessment of pertechnetate and total technetium behaviors during the test. The solution is then passed through a column containing a pertechnetate getter. Because of its extensive use with Hanford tank waste supernatants, SuperLig® 639 is recommended as the pertechnetate getter. The resulting effluent is sampled for analysis by gamma energy analysis, liquid scintillation counting for beta activity, and ICP-MS for its mass 99 concentration.Should there be a significant difference in pertechnetate versus total technetium behavior, the effluent is exhaustively oxidized by a persulfate/microwave digestion, adjusted as needed in composition, passed again through an appropriate pertechnetate getter, and resampled. From analysis of these sample results, the questions posed above can be addressed.The report concludes with an evaluation of a variety of spectroscopic methods that might be used either to identify n-Tc spectroscopically in Hanford tank waste supernatant or to gain insight into the chemical structure of n-Tc. It is concluded that most methods evaluated either are unsuitable, sufficiently insensitive to preclude use at the technetium concentrations present in Hanford tank waste supernatant, or would require significant methods development before they might be effective in n-Tc species analysis. The two methods currently available that can supply useful speciation information are X-ray absorption spectroscopy (of various types) and Tc-99 nuclear magnetic resonance spectroscopy.

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“…Regarding to the online connectivity of the detectors, LSCs [20,21] together with its modified versions for radionuclide sensors [22e24] and ICP-MS [25e27] have been successfully coupled to flow-based methods.…”

Section: Detection Of Radionuclidesmentioning

confidence: 99%

“…As an example of a fully automated system for radionuclide determination, there is a method based on SIA technique developed for 99 Tc determination, including microwave assisted treatment, solid phase extraction (SPE) and online detection (Figure 8.6) [21]. An oxidation procedure using peroxydisulfate in acidic solution was online performed to convert reduced technetium species into pertechnetate in samples with high content of reducing organics.…”

Section: Online Detectionmentioning

confidence: 99%

Automating Radiochemical Analysis

Cerdà

Ferrer²,

Avivar³

et al. 2014

Flow Analysis

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Microwave-Assisted Sample Treatment in a Fully Automated Flow-Based Instrument: Oxidation of Reduced Technetium Species in the Analysis of Total Technetium-99 in Caustic Aged Nuclear Waste Samples

Cited by 24 publications

References 43 publications

Inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS for isotope analysis of long-lived radionuclides

Inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS for isotope analysis of long-lived radionuclides

Protocol for Identifying the Presence of and Understanding the Nature of Soluble, Non-pertechnetate Technetium in Hanford Tank Supernatants

Automating Radiochemical Analysis

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