László Palcsu

Diffusion of 3H, 99Tc, 125I, 36Cl and 85Sr in granite, concrete and bentonite

Understanding the characteristics of diffusion is essential in the assessment of radionuclide release through the backfill of waste repository. The diffusion behavior of 3H, 99Tc, 125I, 36Cl and 85Sr in granite, concrete and bentonite was studied in a specially designed diffusion cell. Diffusion coefficients (D, Da) and time-lag (ta) were measured, break-trough curves were plotted and experimental data were interpreted to predict diffusion rates. The results showed that tritium, iodine and chlorine could be considered as non-sorbing tracers, while technetium was weakly and strontium was strongly sorbed (no break-through was observed during the period of the experiments).

Experimental investigation and modelling of tritium washout by precipitation in the area of the nuclear power plant of Paks, Hungary.

Tritium occurs in nature in trace amounts, but its concentration is changing due to natural and artificial sources. Studies focusing on natural tritium have to take into account the effect of artificial sources. Also, the impact of tritium is an important issue in environmental protection, e.g. in connection with the emissions from nuclear power plants. The present work focuses on the rain washout of tritium emitted from the Paks nuclear power plant in Hungary. Rainwater collectors were placed around the plant and after a period of precipitation, rainwater was collected and analysed for tritium content. Samples were analysed using low-level liquid scintillation counting, with some also subject to the more accurate (3)He ingrowth method. The results clearly show the trace of the tritium plume emitted from the plant; however, values are only about one order of magnitude higher than environmental background levels. A washout model was devised to estimate the distribution of tritium around the plant. The model gives slightly higher concentrations than those measured in the field, but in general the agreement is satisfactory. The modelled values demonstrate that the effect of the plant on rainwater tritium levels is negligible over a distance of some kilometres.

Monitoring of tritium, 60Co and 137Cs in the vicinity of the warm water outlet of the Paks Nuclear Power Plant, Hungary.

Danube water, sediment and various aquatic organisms (snail, mussel, predatory and omnivorous fish) were collected upstream (at a background site) and downstream of the outlet of the warm water channel of Paks Nuclear Power Plant. Gamma emitters, tissue free-water tritium (TFWT) and total organically-bound tritium (T-OBT) measurements were performed. A slight contribution of the power plant to the natural tritium background concentration was measured in water samples from the Danube section downstream of the warm water channel. Sediment samples also contained elevated tritium concentrations, along with a detectable amount of (60)Co. In the case of biota samples, TFWT exhibited only a very slight difference compared to the tritium concentration of the Danube water, however, the OBT was higher than the tritium concentration in the Danube, independent of the origin of the samples. The elevated OBT concentration in the mollusc samples downstream of the warm water channel may be attributed to the excess emission from the nuclear power plant. The whole data set obtained was used for dose rate calculations and will be contributed to the development of the ERICA database.

Dating of total soil organic matter used in kurgan studies

We investigated Csipo-halom, one of the kurgans that served as a burial place in the Hortobagy area of the Hungarian Great Plain. For pedological description and other studies of the protected mound and its surroundings, only a few monitoring drillings were permitted to get soil samples. On the basis of morphological and visual studies, the structure and layers of the mound were reconstructed. The Laboratory of Environmental Studies of the Institute of Nuclear Research at the Hungarian Academy of Sciences (INR/HAS) performed radiocarbon measurements of soil samples, applying a bulk combustion pretreatment method. The measured (super 14) C ages of soil samples from reference points, such as the top layer of the mound, the center of mound body, the base layer of the mound, the near surroundings, and the distant surroundings, are in good agreement with the preliminary archaeological concept for this field and give substantial information about the rate of soil generation processes in this area.

A mass spectrometric line for tritium analysis of water and noble gas measurements from different water amounts in the range of microlitres and millilitres

This paper describes the procedure followed for noble gas measurements for litres, millilitres and microlitres of water samples in our laboratory, including sample preparation, mass spectrometric measurement procedure, and the complete calibrations. The preparation line extracts dissolved gases from water samples of volumes of 0.2 μ l to 3 l and it separates them as noble and other chemically active gases. Our compact system handles the following measurements: (i) determination of tritium concentration of environmental water samples by the 3He ingrowth method; (ii) noble gas measurements from surface water and groundwater; and (iii) noble gas measurements from fluid inclusions of solid geological archives (e.g. speleothems). As a result, the tritium measurements have a detection limit of 0.012 TU, and the expectation value (between 1 and 20 TU) is within 0.2 % of the real concentrations with a standard deviation of 2.4 %. The reproducibility of noble gas measurements for water samples of 20–40 ml allows us to determine solubility temperatures by an uncertainty better than 0.5 °C. Moreover, noble gas measurements for tiny water amounts (in the microlitre range) show that the results of the performed calibration measurements for most noble gas isotopes occur with a deviation of less than 2 %. Theoretically, these precisions for noble gas concentrations obtained from measurements of waters samples of a few microlitres allow us to determine noble gas temperatures by an uncertainty of less than 1 °C. Here, we present the first noble gas measurements of tiny amounts of artificial water samples prepared under laboratory conditions.

Metal container instead of glass bulb in tritium measurement by helium-3 ingrowth method

ABSTRACT The performance of a mass spectrometric system for measurement of tritium by 3He ingrowth method is described. Preparation and measurement includes three steps. The first step is to pump the dissolved gas from the environmental water samples stored in special glass bulb. The second step is the storage of the degassed water for a few months. In the final step the helium-3 formed from tritium is measured by mass spectrometer. In the course of tritium measurement there were some difficulties with the glass bulbs, such as pre-treatment of the glass, storage of the samples in deep freezer, long storage time, O-ring sealing. To solve these problems metal bulbs were built and applied with volume of six litres. The metal bulb was equipped with a metal valve. Three litres of water can be filled into the metal bulb. The large volume of the bulb causes an increase of degassing time, and a decrease of the storage time. The degassing of three litres of water needs twice one and a half hours in two days. The storage time is only two months in contrast to the half-year storage time of glass bulb. The background, the helium penetration from the air is less than using glass bulbs, because the metal bulb can be fitted to the inlet system via copper gasket instead of elastic O-ring.

13C NMR analysis of cellulose samples from different preparation methods

Alpha-cellulose is a part of the wooden material that preserves isotopic composition during tree-growth, and therefore provides important indirect data for paleoclimatological studies. For this reason, it is exceptionally important to extract the alpha-cellulose component from plants, e.g. from tree rings of wood. Since the cell wall of plant cells consists of multicomponent polysaccharides, the extraction of cellulose from wood is not an obvious task. In this paper, we describe, evaluate and compare nine methods, based on the literature and experimental observations, for obtaining cellulose from tree rings of wood. We show that the distortionless enhancement by polarization transfer (DEPT-135) variant of liquid-state 13C NMR spectroscopy is a powerful analytical method for monitoring the preparation process. Trifluoroacetic acid was applied as solvent for the NMR analysis. We proved that all the preparation methods give pure cellulose samples without hemicellulose and lignin content, and we propose methods resulting in non-fragmented cellulose. 13C and 18O isotope ratio measurements have shown that all the applied extraction methods result in similar isotope ratios, thus they are suitable for paleoclimatological studies.

Application of a noble gas mass spectrometric system in environmental studies

Abstract In environmental research, the measurements and evaluation of the isotope ratios represent an important step in explanation of many processes. There are nuclear processes in the environment where stable noble gas isotopes as well as alpha- and beta-decay or spontaneous fission are generated. Therefore, the isotope ratio and concentration can change to such a pitch that notable explanation about these processes can be given in the course of the evaluation of isotope ratio values. The most often used measurement is the tritium–helium method to determine the tritium concentration of water by 3 He ingrowth. The noble gas isotope ratios can be measured from dissolved gas of groundwater or headspace gases. The measurement is done by a VG5400 noble gas mass spectrometer.

Tritium and radiocarbon in the western North Pacific waters: post-Fukushima situation

Impact of the Fukushima Dai-ichi Nuclear Power Plant (FNPP1) accident on tritium (3H) and radiocarbon (14C) levels in the water column of the western North Pacific Ocean in winter 2012 is evaluated and compared with radiocesium (134,137Cs) data collected for the same region. Tritium concentrations in surface seawater, varying between 0.4 and 2.0 TU (47.2-236 Bq m-3), follow the Fukushima radiocesium trend, however, some differences in the vertical profiles were observed, namely in depths of 50-400u202fm. No correlation was visible in the case of 14C, whose surface Δ14C levels raised from negative values (about -40‰) in the northern part of transect, to positive values (∼68‰) near the equator. Homogenously mixed 14C levels in the subsurface layers were observed at all stations. Sixteen surface (from 30 in total) and 6 water profile (from 7) stations were affected by the Fukushima tritium. Surface and vertical profile data together with the calculated water column inventories indicate that the total amount of the FNPP1-derived tritium deposited to the western North Pacific Ocean was 0.7u202f±u202f0.3 PBq. No clear impact of the Fukushima accident on 14C levels in the western North Pacific was observed.

Modulation of Cosmogenic Tritium in Meteoric Precipitation by the 11-year Cycle of Solar Magnetic Field Activity

The relationship between the atmospheric concentration of cosmogenic isotopes, the change of solar activity and hence secondary neutron flux has already been proven. The temporal atmospheric variation of the most studied cosmogenic isotopes shows a significant anti-correlation with solar cycles. However, since artificial tritium input to the atmosphere due to nuclear-weapon tests masked the expected variations of tritium production rate by three orders of magnitude, the natural variation of tritium in meteoric precipitation has not previously been detected. For the first time, we provide clear evidence of the positive correlation between the tritium concentration of meteoric precipitation and neutron flux modulated by solar magnetic activity. We found trends in tritium time series for numerous locations worldwide which are similar to the variation of secondary neutron flux and sun spot numbers. This variability appears to have similar periodicities to that of solar cycle. Frequency analysis, cross correlation analysis, continuous and cross wavelet analysis provide mathematical evidence that the correlation between solar cycle and meteoric tritium does exist. Our results demonstrate that the response of tritium variation in precipitation to the solar cycle can be used to help us understand its role in the water cycle.