Tritium Measurements Research Articles

A device to generate multi-concentration tritiated water vapor

Access to a gas tritium source with controlled concentrations is the key to calibrating tritium measurement instruments. In this study, a method of generating multi-concentration tritiated water vapor based on a closed circulation loop is outlined. The method produces tritiated water vapor by a bubbling process, the operational parameters for achieving the saturated bubbling process were determined through simulation. The temperature dependence of the isotope fractionation coefficient has been established through experimental tests. In order to avoid leakage of tritium and contamination of laboratory environment, tritiated water vapor generator was plugged into a closed loop and tested. Two tritiated water standard samples with known concentrations were used to produce 20 tritiated water vapor samples at 10 different temperatures, where the experimental results were in good agreement with the empirical formula. Based on the experimental results, the model for a non-closed loop tritiated water vapor generation has been modified, and the formula for multi-concentration tritiated water vapor generation based on a closed loop is established.

Measurement Techniques for Low-Concentration Tritium Radiation in Water: Review and Prospects.

Tritium (3H) is one of the most critical nuclides for environmental monitoring, yet it is challenging to measure. Its high natural mobility and its potential to enter the human body through the food chain underscore the importance of not overlooking the radiation safety risks associated with tritium. The need for the online measurement of tritium at low concentrations is becoming increasingly apparent. This review examines the two principal stages of current measurement methodologies: sample preparation and radiation signal detection. It provides a summary of the tritium sample preparation and detection techniques, highlighting advances in the research with potential applications in online monitoring. The review concludes with an analysis of the issues inherent in the current techniques and offers perspectives on possible technological enhancements and future trajectories for the development of online monitoring systems for trace tritium levels.

Nitrate trend reversal in Dutch dual-permeability chalk springs, evaluated by tritium-based groundwater travel time distributions

Historical use of fertilizer and manure on farmlands is known to have a lasting impact on ecosystems and water resources, but few studies assess the legacy of nitrate pollution on groundwater and surface water after farming applications were reduced. We studied the response of nitrate in spring water to a reduction of nitrogen fertilizer applications in agriculture realized since the mid-1980s. We assessed the travel time distribution of groundwater based on a time series of tritium measurements for 90 springs and small brooks that drain a dual porosity chalk aquifer. The travel time distributions were constrained using the tritium data in combination with time series of nitrate concentrations, applying a shape-free travel time distribution model. A clear trend reversal of nitrate concentrations was observed and simulated for springs with a large fraction of young water (< 30 years old) whereas the nitrate response in springs with relatively older water was attenuated and delayed. We conclude that obtaining a time series of tritium data helps to constrain age distributions of water that is discharged from dual permeability aquifers. The fraction of water aged <30 years was a meaningful parameter to distinguish between different types of springs. Nitrate trends in springs that drain large fractions of young water (> 0.6) show higher peak concentrations, shorter lag-time between leaching and outflow peaks and steeper declines after trend reversal, relative to trends in springs which are dominantly fed by older groundwater. The study thus shows that the nitrate legacy of groundwater systems is strongly determined by the range of their travel time distributions, and trend reversal in receiving springs and surface waters may appear within 10 to 15 years after measures to reduce nitrate losses from farming.

Short high-accuracy tritium data time series for assessing groundwater mean transit times in the vadose and saturated zones of the Luxembourg Sandstone aquifer

Abstract. Among the manifold of environmental tracers at hand, tritium is the only one that can give information on groundwater age within the timescale of 100 years for the entire flow system, i.e., unsaturated and saturated. However, while in the Southern Hemisphere, a single water sample is sufficient for tritium-based young groundwater dating, several tritium measurements spanning multiple years are still needed in the Northern Hemisphere to disentangle the natural cosmogenic tritium input from that caused by the atmospheric thermonuclear weapons tests mainly carried out in the early 1960s. Although it is advised to focus tritium dating on sites where long chronicles of tritium data are available, in this study we tested the potential for short high-accuracy tritium data series (∼4 years) to date groundwater from 35 springs draining the Luxembourg Sandstone aquifer (central western Europe). We determined groundwater mean transit times using the lumped-parameter model approach in a Monte Carlo uncertainty estimation framework to provide uncertainty ranges inherent to the low number of tritium data at hand and their related analytical errors. Our results show that unambiguous groundwater mean transit time assessments cannot be determined solely based on such recent short tritium time series, given that several ranges of mean transit times appeared theoretically possible. Nonetheless we succeeded in discriminating groundwater mean transit times in the vadose and saturated zones of the aquifer through a stepwise decision process guided with several supplementary data. The mean transit time required for water to cross the vadose zone was estimated to be between 0.5±0.5 and 8.1±1.2 years depending on the spring, while for water to flow through the saturated zone, it varied from 5.7±2.4 to 18.9±4.6 years (median ± half of the 5–95 percentile range). Our findings are consistent with both the tritium measurements of individual springs and the hydrogeological context of the study area. We specifically corroborated the dating results using the known hydrogeological properties of the Luxembourg Sandstone aquifer, the hydrochemistry of the studied springs, and their discharge dynamics. When translated into water velocities (which average ∼12 and ∼170 m yr−1 for the vadose and the saturated zones, respectively), the tritium dating results mirrored the horizontal–vertical anisotropy of the aquifer's hydraulic properties caused by the bedded character of the Luxembourg Sandstone. In addition to improving our understanding of water transit times in the Luxembourg Sandstone aquifer, this study demonstrates how it is currently possible to use short tritium time series to date young groundwater bodies at new sites in central Europe.

Feasibility Analysis of Tritium Measurement in the Aqueous Medium Based on a Plastic Scintillating Fiber Array

Tritium causes internal dose hazards to humans. Currently, tritium in the environment mainly comes from nuclear power plants, and tritiated water (HTO) is the main form of liquid emission. Therefore, online monitoring activity of tritium in the aqueous medium is vital for protecting human health, and it can warn of the operation status of nuclear power plants. In this paper, we present an improved structure of plastic scintillating fiber (PSF) and a PSF array design, and the detection parameters of PSF arrays with different radii and lengths under different radius detection chambers are simulated using Geant4. Based on the simulation results, the detector is designed, and the minimum detectable activity concentration (MDAC) of the detector is calculated. With calculated MDACs down to 3.09 Bq/L, the proposed design can meet the Chinese requirements for HTO release of inland nuclear power plants of <100 Bq∙L−1. Therefore, the detector designed with a PSF array can be applied to online monitoring of tritium in the aqueous medium.

Interlaboratory comparison exercises for organically-bound tritium in the development of reference materials of environmental samples

The complex behavior of tritium and the probability of increasing tritium concentrations released in the environment were the promotors for the research and development of laboratory methods that enable to accurately determine the various forms of tritium including organically-bound tritium (OBT) for public and regulatory assurance. The measurement of tritium is a key step for dose and risk assessment. The Cernavoda Nuclear Power Plant (NPP) in Romania improved preparation methods and tested environmental matrices for OBT analysis through intercomparison exercises. This paper describes the international Organically-Bound Tritium (OBT) intercomparison exercise, organized by the Cernavoda Nuclear Power Plant (NPP) in 2019–2020, using fruit sample (quince) from Cernavoda town. Evaluation of the results from the participating laboratories was performed using both robust analysis (Algorithm A) method described in the ISO 13528:2015 standard and ANOVA method. The results obtained are encouraging as an increased number of participating laboratories did not change the observed dispersion of the results for activity concentration level around 50 Bq/L of combustion water. The stability of the remaining sample will be checked in time to investigate its use as a reference material for OBT analysis at the environmental levels.

Deep learning based event reconstruction for cyclotron radiation emission spectroscopy

The objective of the cyclotron radiation emission spectroscopy (CRES) technology is to build precise particle energy spectra. This is achieved by identifying the start frequencies of charged particle trajectories which, when exposed to an external magnetic field, leave semi-linear profiles (called tracks) in the time–frequency plane. Due to the need for excellent instrumental energy resolution in application, highly efficient and accurate track reconstruction methods are desired. Deep learning convolutional neural networks (CNNs) - particularly suited to deal with information-sparse data and which offer precise foreground localization—may be utilized to extract track properties from measured CRES signals (called events) with relative computational ease. In this work, we develop a novel machine learning based model which operates a CNN and a support vector machine in tandem to perform this reconstruction. A primary application of our method is shown on simulated CRES signals which mimic those of the Project 8 experiment—a novel effort to extract the unknown absolute neutrino mass value from a precise measurement of tritium β −-decay energy spectrum. When compared to a point-clustering based technique used as a baseline, we show a relative gain of 24.1% in event reconstruction efficiency and comparable performance in accuracy of track parameter reconstruction.

Groundwater vulnerability to pollution in Africa’s Sahel region

Protection of groundwater resources is essential to ensure quality and sustainable use. However, predicting vulnerability to anthropogenic pollution can be difficult where data are limited. This is particularly true in the Sahel region of Africa, which has a rapidly growing population and increasing water demands. Here we use groundwater measurements of tritium (3H) with machine learning to create an aquifer vulnerability map (of the western Sahel), which forms an important basis for sustainable groundwater management. Modelling shows that arid areas with greater precipitation seasonality, higher permeability and deeper wells or water table generally have older groundwater and less vulnerability to pollution. About half of the modelled area was classified as vulnerable. Groundwater vulnerability is based on recent recharge, implying a sensitivity also to a changing climate, for example, through altered precipitation or evapotranspiration. This study showcases the efficacy of using tritium to assess aquifer vulnerability and the value of tritium analyses in groundwater, particularly towards improving the spatial and temporal resolution.

Thermal simulations on a spinning rotor gauge to improve systematic uncertainties for viscosity measurements

Experimental values for the viscosity of the radioactive hydrogen isotope tritium (T2) are currently unavailable in literature. The value of this material property over a wide temperature range is of interest for applications in the field of fusion, neutrino physics, as well as to test ab initio calculations. To measure the viscosity of tritium, a measurement setup has been built utilizing a spinning rotor gauge inside a Dewar. Temperature control is of high importance to produce accurate and precise values. To ensure high quality measurement results, prior to the tritium measurements, thermal simulations are done on measurements with protium and deuterium inside the sample gas volume of the spinning rotor gauge.

3D benchmark experiments of tritium in tungsten for tritium measurements by detecting β-ray induced X-rays

Tungsten is one of the most promising materials for plasma facing components (PFCs), and β-ray induced X-ray spectrometry (BIXS) is an important non-destructive method to obtain tritium depth profile and retention information for the development of PFCs, recovery of fuel and control of tritium safety in a fusion reactor. In this article, benchmark experiments to obtain tritium 3D profile in tungsten have been firstly performed using layer-by-layer chemical etching (LLCE) and imaging plate (IP) techniques. BIXS spectra have been detected at each layer. The average layer thickness of each erosion was controlled to be around 150 nm and 8 layers (the total thickness was 1.21 μm) were eroded, and the maximum uncertainty of tritium activity was 7.91 % in the LLCE experiments. Monte-Carlo simulations of BIXS spectra with Geant 4 code and four kinds of physical packages (Penelope, Livermore, EmStd. Opt1 and EmStd. Opt4) have been benchmarked against to the experimental results. Results show that all the four physical packages are not suitable to calculate the intensity of the BIXS spectra, and the current mode or cross sections should be improved to simulate the interaction between low electron/photon and tungsten accurately. However, the relative intensity of W-Mα peak and W-Lα can be simulated well using current physical packages such as EmStd. Opt4 and Livermore, which is a good indicator for tritium depth profile in tungsten.

Overview of tritium management in WCLL test blanket system of ITER

A key aspect for the achievement of the fuel self-sufficiency of future fusion power plants is the management of tritium in the different stages of the reactor fuel cycle. In particular, one of the greatest challenges for the success of liquid metal breeder concepts such as the Water-Cooled Lithium-Lead (WCLL) is the extraction of tritium from the liquid LiPb eutectic alloy (15.7 at.%Li), which fulfils the main functions of tritium breeder, tritium carrier and neutron multiplier, and the processing in a form suitable for an accurate tritium accountancy. Within this frame, significant advancements have been carried out in the last years as regards the WCLL Test Blanket System (TBS) of ITER. Tritium is mainly produced inside the LiPb and extracted through the Tritium Extraction Unit (TEU). The reference technology for the TEU of the WCLL-TBS is the Gas-Liquid Contactor (GLC) in the packed-column configuration. Tritium is then concentrated in ZrCo getter beds before being sent to the accountancy system where different technologies for both static and dynamic accountancy are adopted in order to provide precise and reliable tritium measurements, which are an essential need in view of an application to the European DEMO reactor. In this paper, the present status and the design solutions foreseen for tritium management in WCLL-TBS are presented and discussed. The implementation and optimization of the conceptual design of the lithium-lead loop (LLP), the Tritium Extraction System (TES) and the Tritium Accountancy System (TAS) have been performed in order to manage tritium concentration in LiPb and in the ancillary systems.

Low-level tritium measurements in freshwater and seawater samples

The aim of this study was to test two potential tritium determination methods (with and without electrolysis enrichment) suitable for low-level measurements. Both methodologies were applied to water samples from the Baltic Sea and ten Polish rivers providing new data on tritium activity concentration. Optimization steps carried out to the standard method lowered minimum detectable activity concentration (MDC) from 3.1 to 1.8 Bq L–1 (at 95% confidence level) enabling to apply it to environmental water samples. However, electrolytic enrichment method of MDC of 0.20 Bq L–1 provided more accurate results for tritium activity concentration in surface waters.

Application of portable liquid scintillation counter for on-field measurement of tritium in aqueous samples during radiation emergency

Screening of aqueous samples for 3H contamination is required to decide suitability of water intended for human consumption during radiation emergency. BARC, Trombay has recently procured Portable Triathler liquid scintillation counter as a screening tool for on-site response to radiation emergency. For this purpose, parameters like, different available scintillators, scintillator to sample ratio and influence of different capacity scintillation vials were optimized for 3H concentration measurement. The study indicated that for 7 mL vials, the optimized scintillator to sample ratio was 4:1 for Optiphase Hisafe II, Ultima Gold Ultra Low Level Tritium, Aqualight AB and Dioxane based scintillators whereas for Ultima Gold AB and Optiphase Hisafe III scintillators it was 3:1. In case of 20 mL vials, the ratio was optimized to 8:1 for all the above mentioned six scintillators. Additionally, the effect of applying counting efficiency using calibration curves generated using distilled water and that obtained using optimized scintillator to sample ratio in various spiked water samples was also studied. Results in 3H concentration (2000–5700 Bq/mL) indicate about ±10% deviation using both the methods for commercially available scintillators. However, in case of Dioxane based scintillator, the deviation was higher (20%). For analysis of 3H concentration ∼200 Bq/mL using commercially available scintillators results in higher deviation of about 21% due to unreliable quench indicating parameter for count rate less than 4000. The study indicated that calibration curves constructed using optimized parameters are universally applicable for determination of 3H concentration in wide variety of water samples.

Effective methods for monitoring internal contamination among workers handling radioactive materials in various fields

This study aimed to develop effective methods for monitoring internal contamination among workers handling radioactive materials in various fields. A total of 160 workers from nuclear power plants, medical institutions, military units, and educational/research institutions were included in the study. The monitoring methods included urinalysis and whole-body counting (WBC) using a mobile radio bioassay laboratory (MRL). Gamma-emitting radionuclides were monitored using the MRL WBC system, and a separate pretreatment procedure was used for tritium measurement in urine samples. Gross beta-screening was performed using a liquid scintillation counting system. The results were evaluated on the basis of the established screening criteria and compared with the dose limits. Additionally, tritium concentrations in the bodies of workers in the vicinity of a heavy-water reactor was analysed to assess the association between tritium concentration and occupation. The results showed a wide distribution of tritium concentrations. Workers involved in fuel and maintenance tasks demonstrated the maximum exposure. Workers in medical facilities showed low levels of internal contamination, which was primarily related to tasks involving radioactive isotopes. Military personnel involved in equipment repair showed significant tritium contamination due to damage during repairs. Workers in educational and research institutions in general had low levels of internal contamination.

Assessing the variability of tissue-free water tritium and non-exchangeable organically bound tritium in pine needles in Fukushima using atmospheric titrated water vapor

When conducting environmental tritium monitoring at nuclear and fusion facilities, it is important to understand how tritium concentrations vary within the soil-plant-atmosphere continuum. Past measurements of organically bound tritium (OBT) concentrations have been conducted from the standpoint of ascertaining the persistence of tritium in terrestrial vegetation, and it has been reported that OBT concentrations fluctuate depending on the influence of atmospheric sources and meteorological conditions. The present study provides information on the variability of tritium concentrations in vegetation growing close to atmospheric sources of tritiated water (HTO) in Japan. We conducted measurements of tissue-free water tritium (TFWT) and non-exchangeable OBT (NE-OBT) in pine needles collected from locations near the Tokyo Electric Power Company's Fukushima Daiichi Nuclear Power Plant from 2018 to 2021. The results we obtained indicate that TFWT concentrations fluctuate in response to short-term changes in atmospheric HTO vapor concentrations and that NE-OBT concentrations vary primarily in response to the time-averaged TFWT concentration during the pine needle growing season, which is in turn mainly determined by atmospheric HTO vapor concentrations. Although it is difficult to ascertain the time-averaged TFWT concentration during the growing season by measuring plant materials, our results show that the measurement of atmospheric HTO vapor concentrations provides an effective alternative method of doing this. We believe our findings can lead to better understanding of the potential impact on the terrestrial environment associated with the atmospheric discharge of HTO and can contribute to improving the strategy of environmental tritium monitoring.

Influence of tritium distribution in aluminum and iron for shape of the beta-ray induced X-ray spectrum

Beta-ray induced X-ray spectrometry (BIXS) is commonly used for qualitative measurement of tritium in solids. We considered that BIXS could also be used quantitatively to determine the depth of tritium in solids. To determine the change in the shape of the BIX spectrum with tritium depth, spectra in aluminum and iron were calculated using the Monte Carlo simulation code (Galet-BIXS). The spectral shape was determined by the relative fractions of the characteristic X-ray components and bremsstrahlung. It was changed with the tritium depth, even when the number of tritium decay events was held constant in the simulations. Specifically, the spectral shape gave information about the tritium depth. However, the accuracy of the estimated tritium depth depended not only on the elements that interact with the beta particles but also on the tritium depth. In some cases, the tritium depth could not be evaluated from the BIX spectra. For example, the spectral shape for aluminum in helium was kept up to 10 µm deep of the tritium depth. When the atmosphere was replaced from helium to argon, the spectral shape was changed with the tritium depth up to 10 µm. Nevertheless, our method allows quantitative analysis of tritium in solids based on the BIX spectrum in most cases. We believe that the Monte Carlo simulation of the BIX spectrum is crucial to the further development to determine the tritium depth in solids.

Toward an efficient determination of tissue-free water tritium in food.

Tritium in the environment constitutes a radiological concern because it can become part of the hydrogen pool in environmental and biological reservoirs and thereby expose people to radiation. Tissue-free water tritium (TFWT) analysis in food is an important subject of environmental radiation monitoring which plays an important role in the estimation of health risks from environmental tritium exposure. At present, tritium content in food is generally determined by liquid scintillation counter (LSC). To improve the analytical efficiency in tritium determination, we developed a novel method to treat TFWT in food using microporous membranes. The microporous membrane treatment method developed in this study has the following characteristics: It has a wide range of application and can process TFWT samples with conductivity below 5 μS/cm. Sample loss for the microporous membrane treatment is approximately 5%. The average treatment time is only 5 min, significantly shortened compared with the currently used atmospheric distillation treatment method (1.5 h). The results of the comparison and spike experiment show that the samples prepared by microporous membrane treatment provides equally satisfactory tritium measurement results as classic distillation method. The developed microporous membrane method is simple to operate, efficient, and environmentally friendly, and effectively improves the analysis efficiency of TFWT in food.

RADIOCARBON AND TRITIUM MEASUREMENTS AT THE GXNU-AMS FACILITY

ABSTRACT A single-stage accelerator mass spectrometer (GXNU-AMS) developed for radiocarbon and tritium measurements was installed and commissioned at Guangxi Normal University in 2017. After several years of operational and methodological upgrades, its performance has been continuously improved and applied in multidisciplinary fields. Currently, the measurement sensitivity for radiocarbon and tritium is 14C/12C ∼ (3.14 ± 0.05) ×10–15 and 3H/1H ∼ (1.23 ± 0.17)×10–16, respectively, and the measurement accuracy is ∼0.6%, which can meet the measurement requirements in the nuclear, earth, environmental and life science fields. This study presents the performance characteristics of GXNU-AMS and several interesting application studies.

Environmental isotope constraints and hydrogeochemical evolution of groundwater in the semi-arid national capital environs of Delhi, India

Changes in hydrological regimes due to rapid urbanization and increasing anthropogenic stress on hydro-geological system creating an alarming condition for the management of ground water resources. Isotope and hydro-geochemical integrated approach has been used to determine the processes governing chemical composition of groundwater and the mechanism influencing the chemical composition of groundwater in National Capital Region (NCR), Delhi. The chemical evolution of groundwater has studied by using flow direction, hydro-chemical facies, bivariate plots of ionic ratios and saturation index. Stable isotopes and tritium are used to understand the recharge mechanism. Pollution index of groundwater (PIG) is also used to check the level of contamination in the groundwater. In total, 57 water samples were collected for water chemistry, 36 water samples for environmental isotopes and 13 samples for tritium measurement. The dominant water type is Ca-Mg-HCO3 and mixed water type. The dominant cation are Ca2+ > Na+ > Mg2+ > K+ and dominant anions are HCO3− > Cl− > SO42− > NO3−. The bicarbonate type water is dominant in quartzite, implies rapid and direct recharge through fracture and joints. Ionic ratios and saturation indices show that major processes controlling groundwater evolution are silicate hydrolysis and reverse cation exchange in the quartzite. Average values of δ2H and δ18O are −43.66 ‰ and −6.28‰. Stable isotopic ratio of groundwater of alluvium area falling on evaporation line, due to the prevailing semi-arid and arid climatic conditions, evaporation is the predominant factor affecting the chemistry of groundwater. The stable isotope shows that the groundwater in the quartzite is mostly meteoric in origin and acting as a recharge area for the nearby alluvium aquifer. Tritium results reveal that groundwater occurring in quartzite and alluvium aquifer in western parts are older than that of groundwater occurring in alluvium aquifer in the eastern parts.13% of groundwater samples are falling in very high pollution zone mainly occurring in alluvium aquifer that lies in the Eastern parts. It is inferred that alluvium aquifer (low lying) is having greater impact of anthropogenic activity than quartzite aquifer (high land).

Impact of the Fukushima Accident on 3H and 14C Environmental Levels: A Review of Ten Years of Investigation

The investigation of the impact of the Fukushima accident is still going on although more than ten years have passed since the disaster. The main goal of this paper was to summarize the results of tritium and radiocarbon determinations in different environmental samples, possibly connected with the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. A document containing compiled data may serve as a solid basis for further research in the selected fields. To accomplish such effort, we went through dozens of relevant published papers, reporting 3H and 14C activity concentrations in precipitations, groundwater, seawater, river systems, tree rings, and, in some more extraordinary samples, such as herbaceous plants or debris from the damaged reactor buildings. As the referenced results would not be obtainable without adequate analytical techniques, the most common methods for routine measurement of tritium and radiocarbon concentrations are discussed as well. We believe that the correct identification of the affected environmental compartments could help quantify the released 3H and 14C activities and track their following fate, which could be especially important for plans to discharge contaminated water from the FDNPP in the upcoming years.