Massic Activity Research Articles

Development of a high precision electrostatic force balance for measuring quantity of dispensed fluid as a new calibration standard for the becquerel

The 2019 redefinition of the kilogram not only changes the way mass is defined but also broadens the horizon for a direct realization of other standards. The true becquerel project at the national institute of standards and technology is creating a new paradigm for realization and dissemination of radionuclide activity. Standard reference materials for radioactivity are supplied as aqueous solutions of specific radionuclides which are characterized by massic activity in the units becquerel per gram of solution, Bq/g. The new method requires measuring the mass of a few milligrams of dispensed radionuclide liquid solution. An electrostatic force balance is used, due to its suitability for a milligram mass range. The goal is to measure the mass of dispensed fluid of 1 mg–5 mg with a relative uncertainty of less than 0.05%. A description of the balance operation is presented. Results of preliminary measurements with a reference mass indicate relative standard deviations less than 0.5% for tens of tests and differ 0.54% or less from an independent measurement of the reference mass.

Digital coincidence counting with 4πβ(PPC)-γ for the standardization of 60Co

A 4πβ(PPC)-γ coincidence system has been made at KRISS based on a digital DAQ. 60Co sources were measured to verify the system. The maximum detection efficiency for beta particles was estimated to be 96.7 %. Massic activities for sample sources had 0.005 % of the sample variability error, which was well within the expanded standard uncertainty of 0.54 % (k = 2).

A comparison of different approaches for the analysis of 36Cl in graphite samples

This study compares different approaches for the quantification of the massic activity of 36Cl in graphite samples. All approaches consisted of a combustion step in combination with a trapping solution to collect the volatile elements. Two different resins were used to separate 36Cl from the matrix (CL resin and PS resin). Liquid scintillation counting (LSC), scintillation counting (SC) and tandem inductively coupled plasma mass spectrometry (ICP-MS/MS) were used to quantify 36Cl activity. The chemical yield in all approaches was determined by means of ion chromatography (IC). In addition, the methods were applied to a real activated graphite sample.

Development of metal radioactive liquid reference material for proficiency test

This study developed liquid reference materials containing various metals, to be used for quality assurance of radiation measurements of the most common metallic wastes generated during the operation or decommissioning of nuclear power plants. The liquid reference materials were prepared by assuming the dissolution of stainless-steel using acid and melting of the major metals present in the stainless steel, namely Fe, Ni, Cr, and Mn, along with the standard sources (134Cs, 137Cs, 60Co, 90Sr). The theoretical massic activity of the standard sources added to the samples and the measured reference values of the gamma and beta emitters in the samples were compared, and they showed good agreement within a one-sigma confidence interval (k = 1). Using the developed reference materials, a proficiency test was conducted on three domestic labs, and the results were evaluated using Z-score. While the evaluation results showed good agreement between the reference values and the reported values for 137Cs and 60Co, all participating labs reported lower values than the reference value for 134Cs. For 90Sr, two out of the three labs reported significantly higher values than the reference value. Based on the results of this study, the developed metal radioactive liquid reference material is expected to be registered as certified reference material (CRM) in the future. They will be used as the CRM for measuring and ensuring the quality of radioactive metal waste.

Anaerobic digestion: A promising technology of utilizing radioactively contaminated plant biomass

Anaerobic digestion (AD) is a widely used technology that allows for the reprocessing and reduction of waste biomass. A study was conducted to see if the AD technology might be used to process radioactively polluted agricultural biomass. For this purpose, laboratory tests were carried out with a 20-liter model biogas plant (BGP) with the radionuclide 134Cs and operational tests with the South Bohemian commercial biogas plant monitoring the radionuclide 137Cs. The activities of 134Cs in inputs, contaminated grass or maize silage and in emerging fractions were investigated in the model fermenter. The activity of 134Cs in the dry matter during the fermentation process increased by 46% on average, which corresponds to a reduction of dry matter by 43% due to the production of biogas. 137Cs activities were measured in commercial BGP maize, grass, and whole plant silage, wheat, digestate, biogas, and aerosol samples. The commercial BGP fermentation process was more efficient, with an 80% reduction in dry mass weight. Dry biomass (1.37 Bq/kg) had a 137Cs massic activity that was 4.4 times lower than the activity of dry digestate mass (6.01 Bq/kg). The activity of the 137Cs in biogas aerosol was 1.1 × 10−7 Bq/m3 or less, and the decontamination factor was 6.9 × 106 or greater. Most Cs remain in the digestate. No other ways of radioactivity leakage have been identified.

Natural and anthropogenic radionuclides in karstic coastal area (Kaštela Bay, Adriatic Sea, Croatia) exposed to anthropogenic activities: distribution, sources, and influencing factors

Abstract 40K, 226Ra, 232Th, 238U, and 137Cs massic activities were determined by gamma-spectrometry in limestones, marls, stream sediments, and soils of Kaštela Bay (Adriatic Sea, Croatia) coastal area. Their distribution, sources and potential influencing factors were studied. The lowest 40K, 226Ra, 232Th, and 238U massic activities were determined in limestones and the highest in soils, with the following median values, respectively: 7.2, 14, 0.8, and 5.3 Bq/kg in limestones and 518, 72, 71, and 31 Bq/kg in soils. All four radionuclides were of natural origin and reflected background values of the karstic area influenced by flysch/marl and terra rossa soil. Local TENORM disposal site did not influence the study area, but it will be needed to study its potential influence on marine sediments. Strong disequilibrium between 226Ra and 238U was found in limestones s.l. and soils, but not in marls and only moderately in stream sediments. This implies that limestones are more susceptible to selective 238U leaching than marls, and soils more than stream sediments. 137Cs was the only radionuclide of anthropogenic origin, with a global source only. It was detected in stream sediments and soils with median values of 5.4 and 31 Bq/kg, respectively. 137Cs distribution was more heterogeneous in stream sediments than in soils, but soils generally presented higher activities. Soil is considered the most important reservoir of 137Cs and its potential source.

137Cs Sediment Profiles as a Tracer of Marine Sedimentation Processes in a Semi-Enclosed Bay Affected by Anthropogenic Releases—Example of Kaštela Bay (Adriatic Sea, Croatia)

Kaštela Bay was taken as a model to study sedimentation processes using the vertical sediment profiles of 137Cs massic activities. The aim was to distinguish the sedimentation conditions in different parts of the Bay and to partly determine the pathways of terrigenous input into the Bay. The purpose was to demonstrate that 137Cs profiles are applicable in differentiating sedimentation processes. It was found that mostly continuous, undisturbed sedimentation takes place in the central and south parts of the Bay; the sedimentation conditions in the west part of the Bay are more complicated. The west part is characterised by the extremely slow sedimentation of the coarse-grained sediment or even by erosion and selective resuspension of the fine-grained particles followed by resedimentation in other parts of the Bay. It was also observed that the upper 10 cm of the sediment is the most exposed to homogenisation. The strong influence of the Jadro River and anthropogenic activities in the east part of the Bay are reflected in the higher 137Cs activities, strong sediment mixing, and increased sediment input. This study shows that the 137Cs profiles can provide comprehensive insights for the whole study region when a sophisticated sampling layout is deployed. The results of the study are applicable to other aquatic environments with comparable processes and sedimentary environments.

Response of sedimentation rate to environmental evolution in Da River Reservoir in Southwest China.

Lake sediment records the evolution process of the interaction between human and nature. It is important to master the lacustrine sedimentation rate for the ecological environment assessment of catchment. A 60-cm sediment core was collected in the Da River Reservoir during 2019 to analyze radionuclides (210Pb and 137Cs) massic activities, grain size, total organic carbon (TOC), total nitrogen (TN), total phosphorus (TP), and metals (Mn, Cu, Al, and Pb) mass fractions to reconstruct the response of sedimentation rate to environmental evolution. The environmental changes in the small catchment were classified into the following three stages through cluster analysis (CA) for geochemical parameters in the sediment core: phase I (1881-1985), phase II (1987-1999), and phase III (2000-2018). The average depth sedimentation rates (ADSRs) of the three stages were 0.33, 0.90, and 1.50cm/year, respectively. The sedimentation rates increased from the bottom to the surface layer, indicating that the exogenous inputs into the reservoir have been occurring. The sediment deposition in phase III was strongly disturbed by the environmental changes (such as warmer climate and intensified land use). Therefore, sedimentation rates showed a rapid increase. Both Pearson correlation analysis and redundancy analysis (RDA) showed that sedimentation rates were positively correlated with climatic factors, particle size, nutrients and metals mass fractions, elemental ratios, and socioeconomic parameters. Sedimentation rates show high sensitivity to anthropogenic activities and climatic change, which can be used to reconstruct the environmental evolution process at a small catchment scale.

Radiological risks from 40K, 226Ra and 232Th in urbanised and industrialised karstic coastal area (Kaštela Bay, Croatia).

Radiological risks associated with 40K, 226Ra and 232Th massic activities in limestones, marls, stream sediments and soils of the Kaštela Bay (Croatia) coastal area were assessed by calculating outdoor absorbed dose rates in air (D), annual outdoor effective dose rates (Def), radium equivalent activities (Raeq) and external hazard indices (Hex). Radionuclides relative contributions to D and Hex were determined for all four types of samples as well as their total contribution to Hex in all samples. D, Def, Raeq and Hex were the lowest in limestones and the highest in soils. Maximum Raeq and Hex in soil were below the recommended values of 370Bq/kg and 1.0. No adverse radiological effects were determined in the researched area. The most important contribution to D and Hex in limestones was almost exclusively from 226Ra, in marls from 40K, in stream sediments from 226Ra and in soils from 232Th. The most significant total contribution to Hex in all samples came from 226Ra and 232Th, and the lowest came from 40K. 226Ra showed the largest variability of its total contribution to Hex, with tendency to higher values. Special attention should be given to 226Ra when studying radiological risks in typical karstic areas, irrespectively of other possible influences of geological background.

40K, 226Ra, 232Th, 238U and 137Cs relationships and behaviour in sedimentary rocks and sediments of a karstic coastal area (Kaštela Bay, Croatia) and related rocks and sediments' differentiation.

Natural (40K, 226Ra, 232Th, 238U) and anthropogenic (137Cs) radionuclides in consolidated sedimentary rocks (limestones s.l. and marls) and unconsolidated sediments (stream sediments and soils) of the Kaštela Bay (Adriatic Sea, Croatia) coastal area were studied. Kaštela Bay is a typical karstic environment and it is under strong anthropogenic influence due to industrialisation and urbanisation. Relationships between radionuclides, their behaviour in different types of samples and possible influencing factors were studied. Radionuclides were also studied in relation to selected metals (Al, K, Ca, Fe, Ti, Mn, V, Cr, Co, Ni, Cu, Zn, Ga, Rb, Sr, Y, Pb and As) and distribution in limestones s.l., marls, stream sediments and soils. Radionuclides' massic activities were determined by gamma-spectrometry and metal mass fractions were measured by EDXRF technique. Relationships were studied using statistical tools (principal component analysis, factor analysis). It was found that stream sediments were more similar to source rocks (limestones s.l. and marl) than to soils in terms of natural radionuclides' activities. 40K and 232Th in consolidated rocks were preferentially bound to alumosilicates and associated with the majority of studied metals. However, this was not the case with 226Ra and 238U, which did not show any preferences regarding binding to mineral components or associating with metals. On the other hand, all four natural radionuclides presented the same behaviour in unconsolidated sediments, i.e. they were all preferentially bound to alumosilicates and associated with the majority of metals. 137Cs did not associate with any of the metals or other radionuclides in sediments. The statistical approach applied in this study revealed differences in radionuclides' relationships and behaviour in a karstic environment and implied possible influencing processes or factors. This approach can be applied in other types of environments as well to study preferential radionuclides' binding to certain mineral components that influences radionuclides' mobility and transport to other environmental compartments.

Validation of measurement comparability of NaI(Tl) scintillation detectors for radioactive cesium in brown rice sample by interlaboratory comparison

The interlaboratory comparison that 148 laboratories participated was performed to understand the validity and variability of measurements with NaI(Tl) scintillation detectors for samples near the standard limit for radioactive cesium in general foods in Japan. Brown rice grains with certified massic activity of radioactive cesium were used as test samples. The medians of the reported massic activities of radioactive cesium, 134Cs, and 137Cs in brown rice grains agreed with the reference values. On the point of view for inspection, more than 92% of the reported values were within the acceptable range.

From radiometry to chronology of a marine sediment core: A 210Pb dating interlaboratory comparison exercise organised by the IAEA

Laboratories from 14 countries (with different levels of expertise in radionuclide measurements and 210Pb dating) participated in an interlaboratory comparison exercise (ILC) related to the application of 210Pb sediment dating technique within the framework of the IAEA Coordinated Research Project.The laboratories were provided with samples from a composite sediment core and were required to provide massic activities of several radionuclides and an age versus depth model from the obtained results, using the most suitable 210Pb dating model. Massic concentrations of Zn and Cu were also determined to be used for chronology validation.The ILC results indicated good analytical performances while the dating results didn't demonstrate the same degree of competence in part due to the different experience in dating of the participant laboratories. The ILC exercise enabled evaluation of the difficulties faced by laboratories implementing 210Pb dating methods and identified some limitations in providing reliable chronologies.

Evaluation of a proficiency test of 131I, 134Cs and 137Cs in maize powder

In 2017, JRC-Geel organised a proficiency test for 120 participants on the massic activity determination of 131I, 134Cs and 137Cs in maize powder. The proficiency test reference material was produced by spiking blank maize powder. The material was characterised for its radioactive content using γ-ray spectrometry. The z scores of the reported massic activity were acceptable in 92% of the results for 131I, and in 94% for both 134Cs and 137Cs. The ζ scores were consistent with the reference value for 66% of the results for 131I, 56% for 134Cs and 68% for 137Cs.

Performance evaluation of a European scale proficiency test on radon-in-water measurements in Europe

In 2018, a Europe wide proficiency test (PT) on measurements of the massic activity of 222Rn in drinking water was organised with the participation of 101 European environmental radioactivity monitoring laboratories. The performance of the participating laboratories was evaluated by comparing submitted results to the reference value using percentage deviation, z-score and zeta-score. It was found that 84% of the participants’ results were within the ±20% reference range. When analysing the zeta-score it was found that 76% of the participants' results were acceptable. The accompanied questionnaire and workshop helped to identify practices that could lead to erroneous results. As it was probably the largest scale PT on radon-in-water ever, the evaluation of results is representative of the quality of radon-in-water monitoring in the EU today.

Evaluation of a radon-in-water pilot-proficiency test

A pilot proficiency test (PT) on measurements of the massic activity of 222Rn in drinking water was organised by JRC-Geel. Fourteen environmental radioactivity monitoring laboratories were invited to participate. The key aim of the study was to test, optimise and stream-line the complete process for conducting such a PT in order to perform a large scale Europe-wide PT in a robust manner. The process involved using all state-of-the art knowledge on sampling, transporting and measuring 222Rn in water. It was found that the majority of the participants’ results (92%) were within the ±15% reference range. The pilot-PT showed that the applied process was suitable and can be used for the large scale European PT planned for the third quarter of 2018.

Correction to: Primary standardization of the massic activity of a 233Pa solution

In the original publication, the value “2.611·104 Bq g−1” in the sentence “The measured massic activity of 233Pa at the reference time was 2.611·104 Bq g−1 with a combined standard uncertainty of 0.93%.” under the heading “HPGe detector activity determination” should be read as “2.632·104 Bq g−1”.

Naturally occurring radioactive material and risk assessment of tailings of polymetallic and Ra/U mines from legacy sites

Old mine tailings from Northern and Central Portugal were studied in order to perform a radiological and chemical characterization. The evaluation of massic activity of natural radionuclides and concentrations in tailings of polymetallic and Ra/U mines was performed by gamma spectrometry and neutron activation analysis. Iron speciation was carried out by Mössbauer spectroscopy. In polymetallic tailings with physical ore processing (Cumieira and Verdes - exploited for Sn, Nb-Ta) higher contents of Th, 228Ra and 226Ra in the coarser materials occur, probably due to their presence in host rock and ore fragments. In finer tailings, washing may explain the lower 226Ra and 210Pb massic activity. In tailings with physical/chemical ore processing (Covas - exploited for W and Sn) high U contents and a tendency for higher 226Ra and 210Pb massic activity in the fine materials is observed, probably due to their incorporation in nano-sized particles of iron oxides. A high variation of the 210Pb/226Ra ratio occurs in polymetallic tailings; a deficit of 210Pb can be observed particularly in deposits of settling tanks drained from dumps of chemically treated ore. In Ervideira-Mestras tailings (Ra/U exploitation) where no ore process in situ was performed, a near equilibrium between 210Pb and 226Ra occurs. Dose risk assessment was carried out by calculating external outdoor Annual Effective Dose Rate; the dose rates in air due to terrestrial gamma radiation are low for the polymetallic tailings (<47 nGy/h), and higher for tailings of Ra/U (up to 4130 nGy/h), in the worst scenario.

PRIMARY STANDARDIZATION OF THE MASSIC ACTIVITY OF A PROTACTINIUM-233 SOLUTION.

Protactinium-233 (233Pa) is used as a tracer for radiochemical analysis and is of particular interest as an isotope dilution mass spectrometry (IDMS) spike for 231Pa/235U radio-chronometry. To this end, we present massic activity determinations by two methods for a 233Pa solution, which was prepared at Lawrence Livermore National Laboratory (LLNL) and is being characterized at multiple labs as part of a 231Pa reference material production project. One activity determination method was 4πβ-γ anti-coincidence counting in a multi-dimensional extrapolation model, with Monte Carlo corrections. An independent massic activity determination was completed by γ-ray spectrometry using 5 HPGe detectors using 5 γ-ray lines. The anti-coincidence and γ-ray spectrometry results agree and have combined standard uncertainties of about 0.33 % and 1.0 % respectively. In addition, the two methods were combined to derive γ-ray emission probabilities from 233Pa decay.

A reference material for evaluation of 137 Cs radiochronometric measurements.

A new nuclear forensic reference material has been characterized as a standard for radiochronometric determination of the model purification date for 137Cs sources. The purification date of a radioactive source is a potentially diagnostic nuclear forensic signature for determining the provenance of a radioactive material. Reference values have been measured for the attributes needed to use the 137Cs/137Ba chronometer: the molality (reported here as nmol g-1) of 137Cs and of the radiogenic portion of 137Ba in the material (hereafter referred to as 137Ba*). All measurement results were decay-corrected to represent the composition of the material on the reference date of July 7, 2011. The molality of 137Cs is (0.7915 ± 0.0073) nmol g-1; this value was calculated from the massic activity of 137Cs, (348.4 ± 3.0) kBq g-1, as measured in the NIST 4π-γ secondary standard ionization chamber (previously calibrated by 4π-(e+x)-γ-coincidence efficiency extrapolation counting) and the evaluated half-life of 137Cs, (30.05 ± 0.08) years. The molality of 137Ba*, (1.546 ± 0.024) nmol g-1, was measured by isotope dilution mass spectrometry using the measured relative proportion of 138Ba in the material to apply a correction for the 137Ba contribution from natural Ba. A model age of (47.04 ± 0.56) years, corresponding to a model purification date of June 22, 1964 with an expanded uncertainty of 200 days is calculated from the reference material values. This age is consistent with the date engraved on the capsule that contained the 137Cs starting material and with a prior independent determination of the model purification date. A full discussion of the uncertainties of the reference material values is included.

New determination of the 229Th half-life.

A new determination of the 229Th half-life was made based on measurements of the 229Th massic activity of a high-purity solution for which the 229Th molality had previously been measured. The 229Th massic activity was measured by direct comparison with SRM 4328C using 4παβ liquid scintillation counting, NaI counting, and standard addition liquid scintillation counting. The massic activity was confirmed by isotope dilution alpha spectrometry measurements. The calculated 229Th half-life is (7825 ± 87) years (k = 2), which is shorter than the three most recent half-life determinations but is consistent with these values within uncertainties.