Tritium in foods

The qualities of selected scintillation systems for the measurement of very low tritium content in water samples from foods were investigated in the liquid scintillation spectrometer. The influence of the parameters of the measuring method on the detection limit was defined by figures of merit. Optimum values were obtained with an emulsion system, which consists of PPO, bis-MSB, p-xylene and Triton N-101, and which takes up 40% water. 0.16 to 0.18 pCi/ml water are detectable with this system. Reference water, which is poor in tritium, was produced by combustion of propane.     

Study of kinetics,equilibrium and isotope exchange in ion exchanger systems

An automatic, rapid combustion method has been developed for the determination of tritium and¹⁴C in singly or doubly labelled organic materials by liquid scintillation counting. The sample is burned in a stream of oxygen. The water formed and its tritium content are retained from the gas stream in an absorber containing a small amount of diethyleneglycol monoethyl ether. Radioactive carbon dioxide, if included in the combustion products, is transferred into 3-methoxypropylamine. The final solutions ready for counting are obtained in less than three minutes. Quantitative collection recoveries for both tritium and¹⁴C are achieved and no cross-contamination occurs.     

Tritium in Lebensmitteln

In order to test the method of tritium determination and to determine the tritium activity, foods of known origin were investigated. The accuracy of the method over a prolonged period of time is confirmed by the statistical evaluation of the background values and of the counting efficiency. An average value of 600–800 pCi of tritium in one litre of water was found in milk, potatoes and apples. Drinking water contained very different activities of tritium, depending on its origin as ground or surface water. Food samples from the environment of nuclear reactors were not different in their tritium content when compared to those of other origin.     

A fundamental study on testing candidate tritium breeders for fusion reactiors

An apparatus was designed and constructed for investigation of the tritium release rate from neutron-irradiated materials for fusion reactors. The design principles, as well as safe handling of tritium and complete trapping of tritium components released, are described and the tritium release rates obtained with this apparatus are discussed for sintered lithium fluoride pellets.     

Automatic isotope gas analysis of tritium labelled organic materials

An isotope analytical procedure and an automatic instrument developed for the determination of tritium in organic compounds and biological materials by internal gas counting are described. The sample is burnt in a stream of oxygen and the combustion products including water vapour carrying the tritium are led onto a column of molecular sieve-5A heated to 550 °C. Tritium is retained temporarily on the column, then transferred into a stream of hydrogen by isotope exchange. After addition of butane, the tritiated hydrogen is led into an internal detector and enclosed there for radioactivity measurement. The procedure, providing quantitative recovery, is completed in five minutes. It is free of memory effect and suitable for the determination of tritium in a wide range of organic compounds and samples of biological origin.     

Tritium analysis with an ethane-filled proportional counter

An apparatus for natural tritium concentration measurement using an ethane-filled proportional counter with anticoincidence shielding is described. The counter characteristics and the counter calibration with internal tritium and external¹³⁷Cs standards are discussed. Results of tritium analysis of Bratislava rains are presented.     

Enrichment reliability of solid polymer electrolysis for tritium water analysis

We have developed a novel advanced enrichment apparatus for environmental tritium analysis called SPET (Solid Polymer Electrolysis for Tritium Water). It generates no explosive gas, requires no aqueous electrolyte, terminates enrichment rapidly, and the volume reduction is infinite. It has an automatic shutdown system which gives uniform conditions on every run, making the handling and determination of tritium concentrations very easy. The reliability of SPET was studied using environmental concentration standard water and the reproducibility error was found to be within 4%, which is sufficient for environmental measurements.     

Automatic isotope gas analysis of tritium labelled organic materials

An analytical procedure and an automatic apparatus are described for the determination of tritium in organic compounds by gas counting. The sample is pyrolysed in hydrogen atmosphere at 1000°C, then, with hydrogen, the decomposition products are rinsed through a column of molecular sieve-5A heated to 550°C. Tritium in water, hydrogen sulphide, ammonia and hydrogen cyanide is transferred into the hydrogen stream by isotope exchange completed on the column. The inactive water vapor, hydrogen sulphide, ammonia and hydrogen cyanide as well as carbon dioxide are removed from the gas stream by appropriate absorbents, and the radioactive hydrogen together with tritiated methane, carbon monoxide and nitrogen included in the pyrolytic products is led into an internal proportional counter tube for radioactivity measurement. The method provides quantitative recovery, it is free of memory effect and suitable for the rapid assay of a wide variety of organic compounds containing C, H, N, O, S in addition to tritium.     

A method for the determination of tritium distribution in environmental and biological samples

A method for the determination of the tritium distribution in environmental and biological samples is described. Tritium as HTO is removed by freeze-drying and the residue is combusted to obtain organically bound tritium. Each tritium fraction is electrolytically enriched and determined by liquid scintillation spectrometry. Enrichment and large sample sizes are required due to the low environmental tritium levels. During the analyses of more than 600 samples over a two-year period all aspects of the method (freeze-drying, combustion, enrichment and counting) have provided reproducible and precise results.     

Automation of the gas analysis of14C-labelled compounds utilizing a piston-type counter tube

In this paper an automatic apparatus designed for the radioactivity measurement of¹⁴C-labelled organic compounds in the gaseous phase is described. The labelled organic compounds are combusted in a mixture of argon and oxygen. After combustion the oxygen content of the gas is eliminated by passing it through a copper packing. The water and heteroelements present are also removed and the radioactive carbon dioxide gas is swept by argon carrier gas into a piston-type counter tube. In the counter tube the piston forming a dividing wall moves forward in accordance with the rate of combustion and sweeping, and thus sucks the gases leaving the combustion tube into the effective tube volume. The anode wire is carried by a reel located in the piston and a spring device ensures its stretched state. At the end of the sweeping period methane is fed into the counter tube and the activity of the argon—methane—carbon dioxide mixture is measured in the limited proportional region. Manual and automatic operation is possible. The piston-type counter tube provides possibility for strandardization by means of extrapolation and for measurement of absolute activities.     

Determination of surface hydroxyl concentration on glass and fused silica capillary columns

Summary The concentration of surface hydroxyl groups on three types of capillary columns was determined by exchanging the hydroxyl protons with tritium. The tritium was quantified by combustion to tritiated water followed by scintillation counting. The number of hydroxyl groups on a leached and presumably hydroxylated Pyrex glass capillary column was found to be about 2.8 groups per square nanometer. This value was slightly less than the 4.6 groups per square nanometer that is generally accepted for a fully hydroxylated porous silica. Dehydroxylation of the same glass by heating at 600°C left only 0.4 groups per square nanometer while an untreated fused silica had only 0.2 groups per square nanometer.Dedicated to Dr. Leslie S. Ettre for his 60th birthday.     

Levels of tritium concentration in the environmental samples around JAERI TOKAI

By the operation of research reactors, tritium-handling facilities, nuclear power plants, and a reprocessing facility around JAERI TOKAI, tritium is released into the environment in compliance with the regulatory standards.To investigate the levels of tritium concentration in environmental samples around JAERI, rain, air (vapor and hydrogen gas), and tissue-free water of pine needles were measured and analyzed from 1984 to 1993. Sampling locations were determined by taking into consideration wind direction, distance from nuclear facilities, and population distribution. The NAKA site (about 6 km west-northwest from the TOKAI site) was also selected as a reference point.Rain and tissue-free water of pine needles were sampled monthly. For air samples, sampling was carried out for two weeks by using the continuous tritium sampler. After the pretreatment of samples, tritium concentrations were measured by a low background liquid scintillation counter (detection limit is 0.8 Bq/l).Annual mean tritium concentrations in rain observed at six points for 10 years was 0.8 to 8.9 Bq/l, which decreased with distance from the nuclear facilities. Tritium concentrations in rain obtained at Chiba City were around 0.8 Bq/l (1987–1988) and those at the NAKA site were 0.8 to 3.8 Bq/l.Annual mean HTO concentrations in air at three points for 10 years were 9.2×10^–2 to 1.1 Bq/m³, although HT concentrations in air, ranging from 1.7×10^–2 to 5.8×10^–2 Bq/m³, were not influenced by the operation of the nuclear facilities.Annual mean tritium concentrations in tissue-free water of pine needles at four points for 10 years were 1.4 to 31 Bq/l. Those at the NAKA site ranging from 1.4 to 6.2 Bq/l were in good agreement with the reported value by Takashima of 0.78 to 3.0 Bq/l at twenty-one locations in Japan.Monthly mean HTO concentrations in air for 10 years showed a good correlation with absolute humidity, while other samples showed no seasonal variation.Higher level tritium concentrations in rain, in air (vapor), and in tissue-free water of pine needles at the TOKAI site were caused by the tritium released from the nuclear facilities.The committed effective dose equivalent to the member of general public, estimated using the maximum tritium concentration in air (1.1 Bq/m³), was 0.23 Sv, which was about 1/4000 of dose limit for general public.     

Liebig's alkaloid analyses: the uncertain route from content to molecular formulae

Liebig's 1831 paper that describes a new apparatus for the analysis of organic compounds and the results of several analyses using the apparatus is a justly famous contribution to the evolution of modern chemistry. In this paper, I look at the three separate components of Liebig's combustion apparatus that collect the water, carbon dioxide and nitrogen released by the combustion of six alkaloids. Gravimetric data included in the paper reveal that very accurate results could be obtained for water by absorption in a calcium chloride tube, and even better results for carbon dioxide resulted from use of the Kaliapparat. Volumetric measurement of nitrogen gave very poor results despite Liebig's efforts to improve it. Inaccuracies in nitrogen measurement made consistent construction of accurate molecular formulae for nitrogenous substances impossible, and only fortuitous decisions intended to bring molecular formulae into agreement with measured combining weights gave formulae in agreement with modern ones, as in the case for quinine.     

Determination of tritium activity and chemical forms in the exhaust gas from a large fusion test device

A water bubbler system that can distinguish chemical forms of tritium was proposed for long-term tritium monitoring of the exhaust gas of a large fusion test device. The characteristics and performance of the water bubbler system were evaluated under operational conditions and confirmed to be suitable for tritium monitoring. For the tritium measurements, the water bubbler system determined the tritium activity and distinguished the chemical forms of tritium. The tritium activity and chemical forms in the exhaust gas provided helpful information to understand the tritium behavior in the large fusion test device.     

Characteristics of the combustion water of organically bound tritium (OBT) measurements of fish samples

Improving accuracy and precision of measurements of organically bound tritium (OBT) activity concentration in environmental samples has become a key aspect of the study of radiological effects by scientists and regulators. Significant quenching effects are known to occur in the measurement of fish samples for OBT using a liquid scintillation counter. In this study, the quench effects of fish and vegetable samples were investigated, as well as the ionic composition of the samples following combustion, neutralization and distillation processes. Furthermore, revised water equivalent factors of various foodstuffs for OBT measurement were calculated using the Health Canada database.

     

Succinyl chloride as a hydrolytic reagent for the determination of water

Several hydrolytic reagents have been examined for use in the titrimetric determination of water. Succinyl chloride was found to be satisfactory. It reacts more rapidly with water than cinnamoyl chloride. The reagent can be used under varying conditions of flow rate in a combustion apparatus and yields good recoveries of water     

Quality assessment of hydrosphere in the vicinity of Czech nuclear power plants by radioanalytical methods

Summary The paper deals with the impact of nuclear plants and radioactive waste disposal on surface and ground water quality in their vicinity using various radiometric and radioanalytical methods. The impact of nuclear power plant Temelin on activation concentrations and fission products in hydrosphere, including tritium, was detected. The annual average tritium concentrations in Vltava River correspond to the previously calculated estimates for average and minimal quaranteed flow rates. The concentrations histories of ⁹⁰Sr and ¹³⁷Cs in surface water show a decreasing trend. This trend was not influenced by the nuclear power plant pilot operation. In the case of tritium, a concentration increase trend has been already observed since the startup of pilot operation. An attempt has made interpreting the sorption and diffusion data for radionuclides of cesium, strontium and tritium and technetium as representatives of multivalent elements. Sorption and diffusion data of ¹³⁷Cs and ⁹⁰Sr in contact with natural sorbent bentonite lead to the conclusion that both diffusion and batch sorption experiments can be simulated by an exchange model. Sorption of technetium on various bentonites plus additives materials is described. Retention of technetium on these solid phases is driven by sorption of reduced form of technetium Tc(IV).     

Essay Reviews

Abstract

Liebig's 1831 paper that describes a new apparatus for the analysis of organic compounds and the results of several analyses using the apparatus is a justly famous contribution to the evolution of modern chemistry. In this paper, I look at the three separate components of Liebig's combustion apparatus that collect the water, carbon dioxide and nitrogen released by the combustion of six alkaloids. Gravimetric data included in the paper reveal that very accurate results could be obtained for water by absorption in a calcium chloride tube, and even better results for carbon dioxide resulted from use of the Kaliapparat. Volumetric measurement of nitrogen gave very poor results despite Liebig's efforts to improve it. Inaccuracies in nitrogen measurement made consistent construction of accurate molecular formulae for nitrogenous substances impossible, and only fortuitous decisions intended to bring molecular formulae into agreement with measured combining weights gave formulae in agreement with modern ones, as in the case for quinine.     

Concentrations of Tritium in Water Vapor and Precipitation on Mt. Hakkoda

A large reprocessing plant of spent nuclear fuel is now under construction in Rokkasho-village, Aomori Pref. Japan. We carried out the survey of tritium concentration in water vapor and precipitation on the top of Mt. Hakkoda, to grasp the behavior of tritium in the environment of Aomori Pref. The tritium concentration in water vapor and precipitation tended to increase from spring through summer. Deuterium concentration in water vapor is lower than precipitation and the effect of the isotope separation by evaporation was observed. The tritium concentration in water vapor, however, is a little bit higher than precipitation. The tritium concentration in water vapor showed the similar change on the top of Mt. Hakkoda and also the wide region covering Rokkasho-village from Aomori-City. Also, on the top of Mt. Hakkoda the correlation was observed between the tritium concentration in water vapor and ozone concentration.