Mihok S, Wilk M, Lapp A, St-Amant N, Kwamena N-O A, Clark I D
Canadian Nuclear Safety Commission, 280 Slater Street, P.O. Box 1046, Station B, Ottawa, Ontario K1P 5S9, Canada.
Department of Earth Sciences, 140 Louis-Pasteur, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada.
J Environ Radioact. 2016 Mar;153:176-187. doi: 10.1016/j.jenvrad.2015.12.025. Epub 2016 Jan 12.
The dynamics of tritium released from nuclear facilities as tritiated water (HTO) have been studied extensively with results incorporated into regulatory assessment models. These models typically estimate organically bound tritium (OBT) for calculating public dose as OBT itself is rarely measured. Higher than expected OBT/HTO ratios in plants and soils are an emerging issue that is not well understood. To support the improvement of models, an experimental garden was set up in 2012 at a tritium processing facility in Pembroke, Ontario to characterize the circumstances under which high OBT/HTO ratios may arise. Soils and plants were sampled weekly to coincide with detailed air and stack monitoring. The design included a plot of native grass/soil, contrasted with sod and vegetables grown in barrels with commercial topsoil under natural rain and either low or high tritium irrigation water. Air monitoring indicated that the plume was present infrequently at concentrations of up to about 100 Bq/m(3) (the garden was not in a major wind sector). Mean air concentrations during the day on workdays (HTO 10.3 Bq/m(3), HT 5.8 Bq/m(3)) were higher than at other times (0.7-2.6 Bq/m(3)). Mean Tissue Free Water Tritium (TFWT) in plants and soils and OBT/HTO ratios were only very weakly or not at all correlated with releases on a weekly basis. TFWT was equal in soils and plants and in above and below ground parts of vegetables. OBT/HTO ratios in above ground parts of vegetables were above one when the main source of tritium was from high tritium irrigation water (1.5-1.8). Ratios were below one in below ground parts of vegetables when irrigated with high tritium water (0.4-0.6) and above one in vegetables rain-fed or irrigated with low tritium water (1.3-2.8). In contrast, OBT/HTO ratios were very high (9.0-13.5) when the source of tritium was mainly from the atmosphere. TFWT varied considerably through time as a result of SRBT's operations; OBT/HTO ratios showed no clear temporal pattern in above or below ground plant parts. Native soil after ∼20 years of operations at SRBT had high initial OBT that persisted through the growing season; little OBT formed in garden plot soil during experiments. High OBT in native soil appeared to be a signature of higher past releases at SRBT. This phenomenon was confirmed in soils obtained at another processing facility in Canada with a similar history. The insights into variation in OBT/HTO ratios found here are of regulatory interest and should be incorporated in assessment models to aid in the design of relevant environmental monitoring programs for OBT.
作为氚化水(HTO)从核设施释放的氚的动态变化已得到广泛研究,其结果已纳入监管评估模型。这些模型通常会估算有机结合氚(OBT)以计算公众剂量,因为OBT本身很少被测量。植物和土壤中OBT/HTO比值高于预期是一个新出现的问题,目前尚未得到很好的理解。为支持模型的改进,2012年在安大略省彭布罗克的一个氚处理设施设立了一个实验园,以表征可能出现高OBT/HTO比值的情况。每周对土壤和植物进行采样,同时进行详细的空气和烟囱监测。设计包括一块原生草皮/土壤区域,与在装有商业表土的桶中种植的草皮和蔬菜形成对比,这些植物处于自然降雨以及低氚或高氚灌溉水条件下。空气监测表明,羽流很少出现,浓度高达约100 Bq/m³(实验园不在主要风区)。工作日白天的平均空气浓度(HTO为10.3 Bq/m³,HT为5.8 Bq/m³)高于其他时间(0.7 - 2.6 Bq/m³)。植物和土壤中的平均组织游离水氚(TFWT)以及OBT/HTO比值与每周的释放量之间仅存在非常微弱的相关性或根本没有相关性。土壤和植物中的TFWT相等,蔬菜地上部分和地下部分的TFWT也相等。当氚的主要来源是高氚灌溉水时,蔬菜地上部分OBT/HTO比值高于1(1.5 - 1.8)。用高氚水灌溉时,蔬菜地下部分的比值低于1(0.4 - 0.6),而靠雨水灌溉或用低氚水灌溉的蔬菜OBT/HTO比值高于1(1.3 - 2.8)。相比之下,当氚的来源主要是大气时,OBT/HTO比值非常高(9.0 - 13.5)。由于SRBT的运行,TFWT随时间有很大变化;地上或地下植物部分的OBT/HTO比值没有明显的时间模式。在SRBT运行约20年后,原生土壤初始OBT含量很高,且在整个生长季节持续存在;实验期间,园圃土壤中几乎没有形成OBT。原生土壤中高OBT似乎是SRBT过去较高释放量的一个特征。在加拿大另一个有类似历史的处理设施获取的土壤中也证实了这一现象。此处发现的关于OBT/HTO比值变化的见解具有监管意义,应纳入评估模型,以协助设计相关的OBT环境监测计划。