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Nuclear Instruments and Methods in Physics Research A 527 (2004) 657659

Measurement of

Letter to the Editor 85 133

Kr and Xe in air by absorption in Makrofol

Dobromir S. Pressyanova,*, Krasimir K. Miteva, Vladimir H. Stefanovb

a

Department of Atomic Physics, Faculty of Physics, St. Kliment Ohridski University of Soa, 5 James Bourchier Blvd., 1164 Soa, Bulgaria b AEGIS SP, 12 Liuliakova gradina str., 1113 Soa, Bulgaria Received 12 December 2003; received in revised form 8 March 2004; accepted 20 March 2004

Abstract In this letter we show that the high absorption ability of Makrofol to noble gases could be successfully used for measurements of 85 Kr and 133 Xe in air. r 2004 Elsevier B.V. All rights reserved.
PACS: 29.40.Wk; 28.41.Te; 89.60.Ec Keywords:
85

Kr;

133

Xe; Makrofol

Krypton-85 (half-life of 10:71 y) and 133 Xe (half-life of 5.244 days) are radioactive noble gases produced by ssion of the nuclear fuel. A small amount of these radionuclides is leaking from the fuel elements of nuclear reactors. The releases of 85 Kr and 133 Xe into the atmosphere from nuclear power plants (NPPs) are an important indicator for their technological and safety status. High activity of 85 Kr is released also from the spent fuel reprocessing plants [1]. Normally, the releases of radioactive noble gases are evaluated by means of continuous or grab sampling measurements in the exhausted air stream.

*Corresponding author. Tel.: +359-2-8687009. E-mail address: pressyan@phys.uni-soa.bg (D.S. Pressyanov).

Widely used grab sampling methods are based on the adsorption of noble gases on activated charcoal. The exposure time of these methods is limited by the adverse effect of humidity on adsorption [2]. Recently, plastics equivalent to Makrofol (Makrofols DE 1-4, commercial product of Bayer AG, Leverkusen, Germany) were found to have a remarkably high radon absorption ability compared to other studied plastics [3]. This high radon absorption ability of Makrofol has been successfully used to measure 222 Rn [4,5]. As shown in Ref. [5] the effect of the humidity for this method is weakwithin 10% at even 100% relative humidity. New experiments were initiated to study whether the absorption in Makrofol could be used for measurement of 85 Kr and 133 Xe in air. In this letter we show the pilot results which demonstrate the feasibility of this approach.

0168-9002/$ - see front matter r 2004 Elsevier B.V. All rights reserved. doi:10.1016/j.nima.2004.03.198

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658 D.S. Pressyanov et al. / Nuclear Instruments and Methods in Physics Research A 527 (2004) 657659

To test this approach samples made of Makrofol were exposed to known concentrations of 85 Kr: A 85 Kr source with certied volumic activity (219 MBq m3 STP72:5%) was used (produced by LEA Radioctive Standards Laboratory, CERCA division, FRAMATOME ANP). Different activity concentrations were prepared by mixing known volumes of the source gas and air, using a specially constructed gas dosage system. The prepared gas mixture was transferred to a 10 l hermetic laboratory vessel in which the specimens of Makrofol foils (square pieces with thickness 0.3 and 0:5 mm; each of 25 cm2 area) were placed. After a controlled exposure time of 18:5 h the foils were removed from the vessel and each foil was measured by gross beta counting for 100 s; using a system with end window GM detector. The correlation between the determined net counting rate and the volumic activity of 85 Kr is almost perfect, as can be seen in Fig. 1. In this experiment relatively high concentrations of 85 Kr (33.6 85 MBq m3 ) were used, but the observed counting rates were several orders of magnitude higher than the background of typical low beta-counting systems. To estimate the sensitivity of the method the approach of Currie [6] was employed. These estimates are dependent on the background counting rate of the beta counting system, the

160 Net area counting rate (cps) 140 120 100 80 60 40 20 0 0 50 100 150 200 250 300 350 400 450 Time after exposure (min)
Fig. 2. Net area counting rate of the 81 keV full-energy peak of 133 Xe in the rst 7 h after the end of exposure, for foils of thickness 0:3 mm (), 0:5 mm () and 0:8 mm (~). The live counting time for each measurement was 200 s: The error bars indicate the overall estimated uncertainties.

10 Net counting rate (cps) 8 6 R2=0.9986 4 2 0 0 20 40 60 80 m-3) 100 Activity concentration (MBq

R2=0.9938

Fig. 1. Correlation between the measured net counting rate and the 85 Kr activity concentration for Makrofol samples of thickness 0:3 mm () and 0:5 mm (). The solid lines represent linear t of the data.

detection efciency, the area of the source and the counting time. Assuming counting time of 10000 s and using the other parameters values that are typical for different available low beta counting systems, the detection limit was evaluated to be within the range 104 105 Bq m3 for exposure time of 18:5 h: The detection limit for 85 Kr of many sophisticated noble gas monitors is about 104 Bq m3 or even higher.1 One experiment with 133 Xe was done with a source produced by the Czech Metrological Institute. In this experiment round samples with thickness of 0.3, 0.5 and 0:8 mm were exposed for 20 h to a mixture of 133 Xe and air with 5 109 Bq m3 volumic activity. After the exposure, series of consequent gamma-spectrometry measurements with HPGe detector (ORTEC, relative efciency of 25% and 0:82 keV resolution (FWHM) for the 122 keV line of 57 Co) were made, using 81 keV gamma-line of 133 Xe: The samples were centered at a distance 1:5 cm above the detector. The results are shown in Fig. 2. The net-area counting rates determined for the 81 keV peak are orders of magnitude higher than the background counting rate in the energy region of the peak (568 counts for 170;000 s background
1

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measurement, that is 3:3 103 cps). This indicates the possibility to measure concentrations by several orders of magnitude lower than that in the present experiment. The reduction of the activity by radioactive decay and outgasing from the sample is within about 20% for the rst 7 h: We consider the results of this experiment as an indication that the absorption in Makrofol-based approach could be successfully used for 133 Xe measurements, too. To conclude, the results from the pilot experiments show that the approach to measure 85 Kr and 133 Xe in air by absorption in Makrofol is feasible. However, to develop a practical method for quantitative measurements substantial further work should be done. This includes studies of the dependence of the response on the exposure time and on the thickness of the samples, the inuence of different environmental factors, detailed study of the time dependence of the processes of absorption and desorption etc. A potential application of such a method could be for the alternative inspection and control of the 85 Kr and 133 Xe releases from NPPs or of the 85 Kr releases from spent fuel reprocessing facilities. The sensitivity of the method can be improved by

increasing the exposure time and using large area foils. Further studies are scheduled to reveal the full potential of the method.

Acknowledgements The authors are indebted to Mr. N. Stanchev and Mrs. V. Stancheva from NPP Kozloduy for their valuable help in a part of the experiments.

References
[1] UNSCEAR, Sources and effects of ionizing radiation, UNSCEAR 2000 Report to the General Assembly, with Scientic Annexes, Vol. I: Sources, U.N. Publications, New York, 2000. [2] S. Scarpitta, N. Harley, Health Phys. 59 (1990) 383. . L.M. Hubbard, Radiat. Prot. Dosimetry 74 (1997) [3] H. More, 85. [4] D. Pressyanov, J. Buysse, A. Pofjn, G. Meesen, A. Van Deynse, Nucl. Instr. and Meth. A 447 (2000) 619. [5] D. Pressyanov, J. Buysse, A. Pofjn, A. Van Deynse, G. Meesen, Nucl. Instr. and Meth. A 516 (2004) 203. [6] L. Currie, Anal. Chem. 40 (1968) 586.