Quantification of excess Carbon-14 specific activity in terrestrial biota in the off-site locations of the PHWR nuclear power plant at Kaiga, India.

This is the first detailed study on 14C activity in the environment surrounding a nuclear facility in India. Samples of food matrices and wild plants from the off-site locations of the PHWR nuclear power plant (NPP) at Kaiga were analysed by liquid scintillation spectrometry, results were validated by accelerator mass spectrometry, and an extensive database (N = 142) was established. The stable isotope ratio of carbon (δ13C) in terrestrial plants varied from -33.5 to -23.3 ‰. The maximum excess 14C activity recorded in terrestrial biota was 44 Bq kg-1C (19 pMC). About 75 % of the samples exhibited specific activity in the range 228-249 Bq kg-1C (101-110 pMC). Statistical tests on the 14C specific activity dataset for 2.3-5, 5-10, and 10-20 km radial zones confirmed that the impact of the operation of the NPP on the environment beyond 5 km is minimal. The study suggests that the 14C activity released through gaseous effluents from Kaiga NPP is transported to greater distances along the axis of the valley than that predicted by the Gaussian plume model and those reported for other NPP sites worldwide. This is due to the unique topography of the Kaiga valley in which wind flow channelling, strong winds in the valley mouth, and calm wind within the valley due to the blocking effect by hills for the south-westerly wind regime play dominant roles in the transport of gaseous effluents. The 14C specific activity values at upwind monitoring stations located at >5 km distance from the NPP during the south-westerly wind regime were higher than those observed during the north-easterly wind regime when the same monitoring stations were located on the downwind side. The ingestion dose to the population in the 2.3-5 km radius zone, attributable to the release of 14C from the NPP, was 0.75 µSv y-1. This is a negligibly small fraction of the ICRP recommended dose limit of 1000 µSv y-1 for the public from other than natural sources. The dose due to the natural 14C activity in the Kaiga region was 12 µSv y-1, corresponding to the ambient natural activity of 230 Bq kg-1 C.

NE-OBT and TFWT activity concentrations in wild plants in the vicinity of the PHWR nuclear power plant and control regions of the tropical monsoonal climatic region of the Indian subcontinent.

The results of the first detailed study, involving a large number of samples, on water equivalent factor (WEQp), non-exchangeable organically bound tritium (NE-OBT) and tissue free water tritium (TFWT) activity concentrations in predominant plant species of the tropical monsoonal climatic region, are presented. A total of 369 samples from the vicinity of the PHWR nuclear power plant (NPP) at Kaiga, West Coast of India, and 47 samples of the control region (region not affected by local anthropogenic sources) were analysed. The WEQp varied in the range of 0.347-0.666 L kg-1 with an overall mean value of 0.540 ± 0.045 L kg-1. The NE-OBT activity concentration varied in the range of <9.8-60.9 Bq L-1 of combustion water (mean = 24.6 ± 11.5 Bq L-1) and that of TFWT in the range of 9.2-60.5 Bq L-1 (mean = 30.7 ± 10.9 Bq L-1) in the vicinity of the NPP. Rigorous statistical analysis of the data confirmed that (i) the activity concentrations of both forms of tritium decreased with the increase in the distance between the sampling location and NPP, and beyond 10 km, it was similar to that of the control region, (ii) the incorporation of tritium released from the NPP into wild plant leaves is not species-dependent, (iii) the NE-OBT activity concentration in the 5-10 km zone exhibited a dependence on the prevailing wind regime with respect to the NPP, but not in the 2.3-5 km zone which suggests that the transport of tritium, released into the atmosphere as the gaseous effluent, through diffusion is a dominating factor governing its activity concentration in the 2.3-5 km zone. The NE-OBT to TFWT specific activity concentration ratio (R-value) had a mean value of 0.82 ± 0.27 (range: 0.38-1.64) for samples collected from the vicinity of the NPP and 1.93 ± 0.50 (range: 1.35-3.19) for the control region. Recording higher NE-OBT activity concentration and R-value at the control region highlights the necessity of detailed studies to understand the mechanism of NE-OBT partitioning in the terrestrial environment.

Determination of Organically Bound Tritium (OBT) Concentration in Fish by Thermal Oxidation and Liquid Scintillation Counting Method.

Effluents containing tritium (H) dispersed into the fresh water or marine environment from nuclear facilities can be taken up by biota. Aquatic and marine organisms are among the important pathways through which tritium can enter into the human body, and hence, assessment of the extent of pollution of these ecosystems is very important for radiation dose assessments. Tritium present in environmental matrices can be classified as tissue-free water tritium (TFWT) and organically bound tritium (OBT). Optimization of a method for the determination of OBT in fish, based on thermal oxidation of the sample, is discussed. Samples were subjected to thermal oxidation in a pyrolyser system, and the water produced from the combustion was analyzed by liquid scintillation spectrometry. Results show that a maximum of ~2 g of processed fish sample can be combusted efficiently in the pyrolyser. Using this method, a recovery of 84% was achieved, and minimum detectable activity (MDA) for the method was determined to be 8.5 Bq kg (sample weight = 2 g, counting time = 30,000 s, and detection efficiency = 20%).

Optimisation of a batch thermal combustion method using a tube furnace oxidation system (pyrolyser) and LSC for carbon-14 determination in environmental matrices.

Accelerator mass spectrometry and benzene synthesis coupled with liquid scintillation spectrometry are often used for accurate measurements of 14C activity in the environmental matrices. Thermal oxidation is one of the methods employed for 14C determination in environmental matrices. In this method, the sample is oxidised at high temperature (600-900 °C) to convert carbon species to CO2 and trapped in an amine-based absorber for determining the activity in a liquid scintillation counting (LSC) system. In this study, the performance of a commercially available tube furnace system (pyrolyser), for batch combustion of samples, was evaluated for the determination of 14C specific activity in terrestrial biota samples. Significant improvements over the manufacturer specified method, which is primarily designed for analysis of samples with activity well above the environmental background level, was implemented to achieve accurate determination of 14C specific activity at ambient background level. In the improved method, the CO2 produced from the combustion of the sample was isolated from the combustion products through cryogenic trapping and then absorbed in the absorber (Carbo-Sorb E) through a simple off-line transfer process. This allowed (i) optimisation of CO2 absorption by the absorber (2.2477 g of CO2/10 mL), (ii) achieving good accuracy and precision in the measurements, and a minimum detectable activity value of 13 Bq kg-1C for a counting time of 300 min (7 Bq kg-1C for 1000 min), (iii) avoiding uncertainty associated with the determination of recovery of 14C in the combustion and trapping process, and (iv) elimination of the need for an independent determination of carbon content (%) for expressing the results in terms of 14C specific activity. The method is capable of yielding accurate results with a deviation of <2.4% from the target value for IAEA C3 quality assurance reference material (with a relative standard deviation of 1.40%, and relative error of 0.34%). The combined uncertainty (1σ) associated with the measurements was computed to be 3.4%. Upon optimisation, the suitability of the method for the determination of 14C specific activity in typical terrestrial biota samples of clean air region (region not affected by local anthropogenic sources) and for the quantification of a small increase in the 14C activity above ambient levels in the vicinity of a nuclear power plant is demonstrated.

A WALK-IN TYPE CALIBRATION CHAMBER FACILITY FOR 222Rn MEASURING DEVICES AND INTER-COMPARISON EXERCISES.

A walk-in type 222Rn calibration chamber of volume 22.7 m3, which has traceability to international standards, is established at the Centre for Advanced Research in Environmental Radioactivity, Mangalore University, India. It has a human-machine interface communication system, a programmable logic controller and sensor feedback circuit for controlling and data acquisition of relative humidity (RH) and temperature (T). An innovative method for the generation of desired 222Rn concentration (a few hundred Bq m-3 up to about 36 kBq m-3) using soil gas as a source was adopted. Leak rates of 222Rn from the chamber for the mixing fan ON and OFF conditions were determined to be 0.0011 and 0.00018 h-1 respectively. With the exhaust system fully turned on, the maximum clearance rate of the chamber was 0.58 ± 0.07 h-1. Excellent spatial uniformity in 222Rn concentration in the chamber was confirmed (with a mean value of relative standard deviation < 12%) through measurements at 23 locations using CR-39 film-based passive devices. Demonstration of calibration applications was performed using charcoal canister and PicoRad vials as the 222Rn adsorption devices. The study shows that gamma spectrometry is a convenient alternative approach to liquid scintillation analysis of PicoRad vials for 222Rn measurement.