Experimental investigation of D2 conversion to DHO in soil near the Cernavoda nuclear power plant site in Romania.

The current Canadian and Romanian model predictions for tritium dose following an atmospheric tritiated hydrogen gas (HT) release is based on a default Canadian Standards Association (CSA) conversion factor of HT to tritiated water (HTO) of 4.3%. The determination of an empirical site specific value for the conversion factor was essential for the CANDU Cernavoda Nuclear Power Plant (NPP) in Romania to verify if the CSA value is appropriate for use at this site. Given the role of soil characteristics on the conversion of HT to HTO, on-site experiments would provide the best evaluation of the conversion factor. The objective of the study was to define the soil HT to HTO conversion parameters specific to the Cernavoda NPP site. In June 2016, a series of experiments were conducted to meet this objective. First, the in situ deposition velocity of D2 gas, as a surrogate for HT gas, was obtained using an exposure chamber. Diffusion of D2 into the soil was then evaluated based on the measurements of DHO concentrations in the exposed soil. As soil microbes play a role in the conversion of HT to HTO, this work included a microbiological characterization of the soil, which targeted total soil bacteria (cultivable and gene-based) and hydrogen oxidizing bacteria (cultivable and gene-based). The fraction of hydrogen oxidizing cultivable soil bacteria represented 14-20% of the total cultivable bacteria population estimated as 2.8-29.2 × 105 cfu/g of soil. The empirically derived HT to HTO conversion factor was lower than the default value (4.3%). It fell between 0.9% and 2.0%. The default value is therefore more conservative than the Cernavoda site-specific derived value obtained from the study.

Organically bound tritium (OBT) activity concentrations in surface soil at the Chalk River Laboratories, Canada.

Canadian Nuclear Laboratories (CNL)'s Chalk River Laboratories (CRL) site is home to a large nuclear research complex in Canada. CRL's air tritium releases amount to about 1015 Bq/year. The objective of the study was to characterize the spatial footprint of the 60 years of tritium atmospheric releases in surface soil by measurement of organically bound tritium (OBT). Soil OBT activity concentrations were of particular interest because soil represents a long-term tritium reservoir that can act as a historical record of tritium releases into the environment. Soil samples to a 5 cm depth were collected within the CRL site from 2012 to 2014. Each sample was analyzed for tritiated water (HTO) and OBT activity concentrations. The highest HTO and OBT measurements obtained during this study were 154.0 ±â€¯7.8 Bq/L and 180.9 ±â€¯37.3 Bq/L, respectively. A developed OBT map indicated that retained tritium in soil was not related to the distance of sources-term but it was related to the prevailing wind direction.

OBT/HTO ratio in agricultural produce subject to routine atmospheric releases of tritium.

The mean expected value of the OBT/HTO ratio (i.e. generic ratio) is derived in this study on the joint basis of a long-term study conducted at Atomic Energy of Canada Limited (AECL)'s Chalk River Laboratories (CRL), model simulations targeted at filling gaps in a yet incomplete timeline of CRL measurements and a reference dataset comprised of numerous experiments reported in the literature. Cultivar variability and disparity in site-specific settings are covered by the reference dataset. Dynamical variability caused by meteorology has been a specific target of the long-term experimental campaign at CRL, where the former two types of variability were eliminated. The distribution of OBT/HTO ratios observed at CRL appears to be a fairly good match to the distribution of OBT/HTO ratios from the literature. This implies that dynamical variability appears important in both cases. Dynamics of atmospheric HTO at CRL is comprised of a sequence of episodes of atmospheric HTO uptake and re-emission of plant HTO. The OBT/HTO ratio appears sensitive to the proportion of the duration of these two episodes: the lesser the frequency (and duration) of plume arrivals, the higher the expected mean OBT/HTO ratio. With the plume arrival frequency defined by the typical wind rose, one would encounter a mean OBT/HTO ratio close to 2. It is important to note that this number is seen both in the reference dataset, and in the continuous timeline of HTO and OBT reconstructed from CRL observations by dynamical interpolation (modelling). Many datasets (including that of CRL) targeted at the OBT/HTO ratio are biased high compared to the suggested number. This could be explained by scarce measurements of the low OBT/HTO ratios in the short phase of uptake of atmospheric HTO by the plant.

Relation between the tritium in continuous atmospheric release and the tritium contents of fruits and tubers.

Concentrations of organically bound tritium (OBT) and tissue-free water tritium (TFWT, also referred to as HTO) in fruits and tubers were measured at a garden plot in the vicinity of the source of chronic airborne tritium emissions during the 2008, 2010, and 2011 growing seasons. A continuous record of HTO concentration in the air moisture was reconstructed from the continuous record of Ar-41 ambient gamma radiation, as well as from frequent measurements of air HTO by active samplers at the garden plot and Ar-41 and air HTO monitoring data from the same sector. Performed measurements were used for testing the modified Specific Activity (SA) model based on the assumption that the average air HTO during the pod-filling period provides an appropriate basis for estimating the levels of OBT present in pods, fruits and tubers. It is established that the relationship between the OBT of fruits and tubers and the average air HTO from a 15-20 day wide window centred at the peak of the pod-filling period is consistent throughout the three analysed years, and could be expressed by the fruit or tuber's OBT to air-HTO ratio of 0.93 ± 0.21. For all three years, the concentration of HTO in fruits and tubers was found to be related to levels of HTO in the air, as averaged within a 3-day pre-harvest window. The variability in the ratio of plant HTO to air HTO appears to be three times greater than that for the OBT of the fruits and tubers. It is concluded that the OBT of fruits and tubers adequately follows an empirical relationship based on the average level of air HTO from the pod-filling window, and therefore is clearly in line with the modified SA approach.

HTO and OBT activity concentrations in soil at the historical atmospheric HT release site (Chalk River Laboratories).

Tritium is routinely released by the Chalk River Laboratories (CRL) nuclear facilities. Three International HT release experiments have been conducted at the CRL site in the past. The site has not been disturbed since the last historical atmospheric testing in 1994 and presents an opportunity to assess the retention of tritium in soil. This study is devoted to the measurement of HTO and OBT activity concentration profiles in the subsurface 25 cm of soil. In terms of soil HTO, there is no evidence from the past HT release experiments that HTO was retained. The HTO activity concentration in the soil pore water appears similar to concentrations found in background areas in Ontario. In contrast, OBT activity concentrations in soil at the same site were significantly higher than HTO activity concentrations in soil. Elevated OBT appears to reside in the top layer of the soil (0-5 cm). In addition, OBT activity concentrations in the top soil layer did not fluctuate much with season, again, quite in contrast with soil HTO. This result suggests that OBT activity concentrations retained the signature of the historical tritium releases.