Blood tritium level as an estimate of soft tissue dose

To test the blood tritium level as an estimate of free water tritium (FWT) and organically bound tritium (OBT) in human soft tissues, a tritiated amino acid mixture (TAA) and tritiated water (HTO) were injected or orally administered to mice. Relatively high tritium retention in the blood was found after TAA injection. This observation was explained by a low rate of clearance of non-volatile tritium components. The dose estimated for the soft tissues after TAA injection was larger than that estimated on the basis of tritium concentration in urine by a factor of 1.8-2.3. In both HTO and TAA injections, the blood tritium level gave a conservative estimate of the dose to soft tissues including active bone marrow. The accumulated dose to soft tissues after oral administration tended to be lower than that for intraperitoneal injection.     

Dose reconstruction for an occupational cohort at the Savannah River nuclear facility: evaluation of a hybrid method

The Savannah River Site (SRS) is the only nuclear facility in the United States that produces tritium, a radioactive isotope of hydrogen. The purpose of the study was to derive annual tritium dose estimates for SRS employees through the development of a job-exposure matrix. The proposed method is unique in that along with qualitative information on job, area and time of employment, it utilises recorded annual whole-body dose measures, when available, in order to estimate doses from tritium intakes of the monitored workers. Using information from 75 253 dose measures for the period 1954-1978, the average proportion of the whole-body dose that was due to tritium intake was calculated; these proportions were allowed to vary by job, area and time period. This information was used to assign tritium dose levels for 43 590 employment-years. The collective estimated tritium dose was 4319 mSv compared with the total known tritium dose of 17 382 mSv. The correlation (R2) of estimated tritium dose with known tritium dose was 0.68.     

Tritium Sorption by Modified Natural Aluminosilicates

In connection with problems of interaction of tritium-containing underground waters with clay geological barriers and tritium water treatment, the sorption of tritium by natural and synthetic clays modified with organic compounds was studied. The mechanism of tritium sorption by aluminosilicates, involving the isotope exchange of hydrogen atoms in organic and inorganic compounds, was proposed. Modification of clays with organic compounds shows promise as a way to improve the sorption capacity of clays with respect to tritium.     

Distribution of tritium in water vapour and precipitation around Wolsung nuclear power plant

The distribution of tritium in water vapour and precipitation with discharge of tritiated water vapour and meteorological factors was studied around the Wolsung nuclear power plant (NPP) site during the period 2004-2008. The tritium concentrations in atmospheric water vapour and precipitation had a temporal variation with relatively high values in the early summer. Spatial distribution of tritium concentrations was affected by various factors such as distance from the NPP site, wind direction, tritium discharge into the atmosphere and atmospheric dispersion factor. The annual mean concentrations of atmospheric HTO and precipitation were correlated with the amount of gaseous tritium released from the Wolsung NPP. The tritium concentrations in precipitation decrease exponentially with an increase of the distance from the Wolsung NPP site.     

Influence of Tritium Spillover on the Efficiency of Labeling of Organic Compounds

Various mechanisms of hydrogen spillover are discussed. A number of evidences are given that tritium incorporation by isotope exchange occurs with the participation of both tritium cations and atomic tritium. The molar radioactivity of the labeled products prepared at temperatures of up to 180°C is, apparently, mainly determined by reactions of the organic compound with tritium cations, and the degree of isotope exchange depends chiefly on the efficiency of tritium spillover to the bulk of the organic substance supported on the catalyst.     

Isotope Exchange of Azidothymidine with Tritium

The following modes of isotope exchange of azidothymidine (3'-azido-3'-deoxythymidine) with tritium were studied: solid- and liquid-phase isotope exchange with gaseous tritium and isotope exchange in solution with tritium water. Catalytic reactions of azidothymidine with gaseous tritium in solution result in virtually complete reduction of the azido group to amino group. This reduction also occurs in the course of solid-phase catalytic hydrogenation; the yield of 3'-amino-3'-deoxythymidine ranges from 20 to 70%. The molar radioactivity of tritium-labeled azidothymidine prepared by solid-phase catalytic isotope exchange with gaseous tritium and by isotope exchange in solution with tritium water does not exceed 0.5 Ci mmol^{- 1}.     

A Comparative Study of the Reactions of Thermally Activated Tritium with Sugars and Diazines and of Solid-Phase Catalytic Hydrogenation of These Compounds with Tritium

The feasibility of the labeling procedure involving thermal activation (TA) of tritium was examined with the substrates that are commonly labeled by solid-phase catalytic hydrogenation (SCH) with tritium. Comparative characteristics of SCH and TA as procedures for tritium labeling of sugars and diazines were obtained. These two methods ensure comparable rates of tritium incorporation into purine and pyrimidine bases. The SCH allows preparation of tritium-labeled compounds with the maximum possible molar radioactivity. The molar radioactivity of the same compounds labeled using TA did not exceed 37 TBq mol⁻¹, because only a small fraction of the substrate could react with atomic tritium. Longer reaction times and increased amounts of tritium taken into the reaction resulted in stronger degradation of the substrates. On the assumption that the reactive tritium atoms penetrate into the target to a depth of 0.5 nm, the actual specific radioactivity of the labeled compound in the zone accessible for atomic tritium reaches 0.2–2 PBq mol⁻¹. Ways are suggested to increase the molar radioactivity of compounds labeled using thermal activation of tritium.__________Translated from Radiokhimiya, Vol. 47, No. 3, 2005, pp. 284–288.Original Russian Text Copyright © 2005 by Sidorov, Badun, Baitova, Baitov, Platoshina, Myasoedov, Fedoseev.     

高气密性芯片级原子气室的制备研究

氚是涉氚场所中辐射防护监测的重点核素，对涉氚场所中的气态氚浓度进行有效监测具有重要的意义。根据GB/T 7165.5-2008第5部分要求，氚活度监测校准应使用与被测对象成分一致的参考源，即标准氚气。解决该难题需要研究并建立标准氚气的制备方法和定值方法，确保氚气活度量值源头的有效性。基于稀释法研制了气载氚标准源，通过长度补偿法进行氚活度浓度定值，并进行了不确定度的分析和评定。氚气标准源的研制填补了国内该领域的空白，为氚监测仪的量值溯源提供了重要支撑。     

Quick management of accidental tritium exposure cases

Removal half-life (RHL) of tritium is one of the best means for optimising medical treatment, reduction of committed effective dose (CED) and quick/easy handling of a large group of workers for medical treatment reference. The removal of tritium from the body depends on age, temperature, relative humidity and daily rainfall; so tritium removal rate, its follow-up and proper data analysis and recording are the best techniques for management of accidental acute tritium exposed cases. The decision of referring for medical treatment or medical intervention (MI) would be based on workers' tritium RHL history taken from their bodies at the facilities. The workers with tritium intake up to 1 ALI shall not be considered for medical treatment as it is a derived limit of annual total effective dose. The short-term MI may be considered for tritium intake of 1-10 ALI; however, if the results show intake ≥100 ALI, extended strong medical/therapeutic intervention may be recommended based on the severity of exposure for maximum CED reduction requirements and annual total effective dose limit. The methodology is very useful for pressurized heavy water reactors (PHWRs) which are mainly operated by Canada and India and future fusion reactor technologies. Proper management will optimise the cases for medical treatment and enhance public acceptance of nuclear fission and fusion reactor technologies.     

Dosimetric implications of atmospheric dispersal of tritium near a heavy-water research reactor facility

An estimate of the tritium dose to the public in the vicinity of the heavy water research reactor facility at AECL-Chalk River Laboratories, Ontario, Canada, has largely been accomplished from analyses on regularly-collected samples of air, precipitation, drinking water and foodstuffs (pasture, fruit, vegetables and milk) and environmental dose models. To increase the confidence with which public doses are calculated, tritium doses were estimated directly from the ratio of tritiated species in urine samples from members of the general public. Single cumulative 24 h urine samples from a few adults living in the vicinity of the heavy-water research reactor facility at Chalk River Laboratories, Canada were collected and analysed for tritiated water and organically bound tritium. The participants were from Ottawa (200 km east), Deep River (10 km west) and Chalk River Laboratories. Tritiated water concentrations in urine ranged from 6.5 Bq.l-1 for the Ottawa resident to 15.9 Bq.l-1 for the Deep River resident, and were comparable to the ambient levels of tritium-in-precipitation at their locations. The ultra-low levels of organically bound tritium in urine from these same individuals were measured by 3He-ingrowth mass spectrometry and were 0.06 Bq.l-1 (Ottawa) and 0.29 Bq.l-1 (Deep River). For Chalk River Laboratories workers, tritiated water concentrations in urine ranged from 32 Bq.l-1 to 9.2 x 10(4) Bq.l-1, depending on the ambient levels of tritium in their workplace. The organically bound tritium concentrations in urine from the same workers were between 0.08 Bq.l-1 and 350 Bq.l-1. With a model based on the ratio of tritiated water to organically bound tritium in urine, the estimated dose arising from organically bound tritium in the body for the Ottawa and Deep River residents was about 26% and 50%, respectively, of the body water tritium dose. The workers in a reactor building at Chalk River Laboratories had less than 10% dose contribution from organically bound tritium, but had higher overall tritium dose due to frequent intakes of tritiated water vapour in the workplace. The results of this study suggest that most of the tritium dose to workers at Chalk River and general population near Chalk River is the result of tritiated water intakes and not due to dietary intake of organically bound tritium.     

Reassessment of tritium dose coefficients for the general public

Concerns of increased risk from tritium intake by humans have been claimed in the past. The arguments concerning the radiobiological effectiveness of tritium, its longer retention in the human body and the presence of tritium in the DNA hydration shell are analysed in this paper. A biokinetic model for tritiated water and organically bound tritium retention in the human body is used, based on a common approach for mammals using energy and hydrogen metabolism and tested separately with animal experiments. Extension to this model to humans considers the increased role of the brain, food quality and unique growth patterns of humans. Various ages and genders for Caucasians are considered. For an intake of tritium in organic forms in the diet, the retention for the female is of about a factor 2 compared with ICRP recommendations. Effective dose coefficients are estimated to be about a factor of 2 to 3 higher than those of the ICRP.     

Probability of the reaction at the first collision with polyethylene of tritium atoms generated by thermal activation

The influence of the experimental conditions on the probability of the reaction of tritium atoms generated in the gas phase by thermal dissociation of tritium on a tungsten filament (thermal activation) with hydrocarbons in a solid target was examined. Experiments were performed with polyethylene films placed in a special case with a calibrated slit in the center of the top lid. For tritium atoms reaching the target without energy loss, the probability of the reaction at the first collision with the hydrocarbon matrix cooled to 77 K decreases from 18 to 2.5% with a decrease in the atomizer temperature from 2000 to 1660 K. For tritium atoms preliminarily thermalized in the gas phase to 77 K, the probability of the reaction at the first collision is so low that it cannot be measured with our experimental technique. Nevertheless, even at 77 K tritium atoms can react with the target, yielding the compound labeled at the C-H bonds.     

Synthesis of [3H]Sulfobromophthalein and Related Problems of Tritium Labeling by Solid-Phase Isotope Exchange

Tritium-labeled sulfobromophthalein with a molar radioactivity of 0.5-0.6 PBq mol^-1 was prepared. Various aspects of tritium labeling of organic compounds by solid-phase catalytic isotope exchange are considered. A number of arguments are given in favor of the hypothesis that the degree of isotope exchange mainly depends on the efficiency of tritium spillover in the bulk of the organic substances applied onto the catalyst surface. At present, it can be considered as a reliably proved fact that at temperatures up to 180-200°C the solid-phase isotope exchange mainly occurs via reaction with tritium cations. Apparently, the contribution of the reactions with atomic tritium to labeling is significant only if there is no spillover of tritium cations to the bulk of the organic compound and the substrate withstands heating to 280-300°C.     

Interaction of tritium atoms with solid composite targets: Adsorption layers of nonionic surfactants on hydrophobic supports

The capability of tritium atoms to penetrate deep into solids was used for revealing nonuniformity of coating of polymeric [polyethylene, poly(ethylene terephthalate)] supports by adsorption layers of a nonionic surfactant Brij-35, formed by adsorption from aqueous solutions. The permeability to atomic tritium of Brij-35 adsorption layers on polyethylene appeared to be close to that obtained for hydrocarbon fragments of cationic surfactants in adsorption layers on the water/air boundary. A decrease in the coefficients of attenuation of the tritium atom flow at formation of adsorption polylayers was revealed. This decrease suggests less ordered structure of the polylayers relative to the monolayer. The developed approach involving preparation of adsorption coatings of tritium-labeled surfactants, their treatment with tritium atoms, and subsequent removal of the surfactant from the support, with the autoradiographic detection of tritium distribution on the plate in all the steps of the work, can be used for studying the structure of surfactant adsorption layers on flat solid surfaces.     

等离子喷涂碳化硼/钼涂层氚的滞留性能研究

为了保证核能源的使用安全, 对氚在第一壁材料表面的滞留数量以及深度进行定量表征非常重要。在本研究中, 制备了一系列潜在的第一壁材料B₄C/Mo 涂层, 并采用成像板(IP)和β射线激发X射线(BIXS)法对其表面的氚滞留情况进行了测定。IP 图像表明, 涂层表面吸附的氚含量遵循以下顺序: B₄C>BM15>BM5>Mo。而BIXS结果进一步表明, 对于B₄C涂层, 大部分氚扩散到了涂层内部; 而对于其他三种涂层, 氚仅在其表面发生吸附。扫描电镜(SEM)结果显示, B₄C涂层气孔率最高, 而其他三种涂层尽管气孔率较低, 但其截面仍能观察到大量气孔和微裂纹的存在。涂层中的这些缺陷为氚的吸收和扩散提供了通道, 而气孔与微裂纹的尺寸最终决定了氚在涂层表面的吸附数量。实验结果还表明, 涂层杂质成分Ti的存在也对氚的滞留产生了一定影响。     

Tritium-Labeled Compounds V. Radioassay of Both Carbon–14 and Tritium in Films,With a Proportional Counter

A convenient procedure is described for the radioassay of both carbon-14 and tritium in water-soluble, nonvolatile compounds by means of a windowless, gas-flow, proportional counter. The materials are counted in uniform films of sodium O-(carboxymethyl) cellulose that are “infinitely thick” to the radiation of tritium but not to the radiation of carbon-14. Films of uniform thickness are obtained by new techniques which are described in detail.If only carbon-14 is present, its absolute activity can be calculated conveniently by means of an empirically established curve for the counting-efficiency. If both carbon-14 and tritium are present, the films are counted in the proportional counter and are then recounted in the presence of a screen that stops all radiation from tritium but only a portion of that from carbon-14. From a film with a thickness of 0.8 mg/cm², approximately 43 percent of the radiation of carbon-14 is counted. Of this emerging radiation, approximately 50 percent passes through a screen of ¼-mil double-aluminized “Mylar.” By use of suitable calibration curves for counting-efficiency, carbon-14 and tritium in the same sample can be calculated from the counts with, and without, the screen.Satisfactory analyses can be made with samples containing less than 0.001 microcurie of carbon-14 and 0.005 microcurie of tritium. The method is suitable for the radioassay of a wide variety of labeled materials.     

Monitoring a Flow of “Hot” Tritium Atoms in the Course of Thermal Activation

The possibility of measuring a flow of reactive tritium atoms falling on a target during thermal activation using polyethylene (PE) films was studied. Procedures were developed for pretreatment of PE films before experiment, their subsequent treatment, and radioactivity measurements. The distribution of the flow of tritium atoms in a common reactor as influenced by various modes of atomizer arrangement and different experimental conditions was studied with PE films. The rate of formation of the labeled compound was maximal when the product of the tritium pressure in the system (Pa) by the distance from the atomizer to the target (cm) was 2.     

Expectation of LET∞ for a tritium beta particle

The expectation of LET_∞ (unrestricted linear energy transfer) for a tritium beta particle around its parent nucleus in water has been calculated by the use of the energy-range relation of electrons. The amount of energy deposited by a beta particle with a certain initial energy over the interval of one micron at a definite position is obtained from the relation by the calculus of difference, and the probability that the event takes place per decay of tritium is estimated from the energy spectrum of tritium beta particles. The calculated values of expectations of LET_∞ are higher at positions close to the parent nucleus.     

Radiation quality of tritium

Tritium occurs from both natural and manufactured processes. In the environment, tritium can exist in the form of tritiated water (HTO) and in an organic form known as organically-bound tritium (OBT). Although, the concentrations of environmental OBT are relatively low, there is concern that current risk factors may underestimate the risk from OBT. Because tritium poses an internal hazard at cellular levels, microdosimetric techniques provide suitable tools for the study of radiation quality of tritium. In this study, microdosimetric simulations are performed for tritium uniformly distributed in a medium, and for tritium bound to biologically critical sites of dimensions from 10 nm to 2 microm. Results of local energy density are different for these two cases in microscopic regions. Based on the spatial distribution of energy deposition, dose mean lineal energies are calculated for tritium in forms of HTO and OBT. The dose mean lineal energies of OBT are about a factor of 1.7 higher than those of HTO in a wide range of target dimensions of biological interest. The results are consistent with radiobiological findings that OBT is about twice as effective as that of HTO.     

Atomic tritium as a surface nanoprobe in a structural investigation of molecular assemblies

Possibilities of atomic tritium application as surface nanoprobe for structural investigations of adsorption layers on the liquid–air interface have been demonstrated. Frozen aqueous solutions of a series of amino acids and their mixtures and one well-known surface-active substance (cetyltrimethylammonium bromide, CTAB) were exposed to bombardment by tritium atoms generated on hot tungsten wire in a special vacuum device. This procedure resulted in substitution of hydrogen atoms by radioactive tritium in the thin surface layer of investigated samples. Curves of radioactivity changes depending on bombardment time and solution concentration for applied compounds were obtained and analyzed.