Determination Of Total And Specific Radon-Exhalation Rates From Porous Materials

INTRODUCTION The occurrence of the radioactive element radium, [2gg~a], often in trace amounts, in the crust of the earth gives rise to a flux of the daughter product radon, ['ii~n], across the earth-air interface. This so-called exhalation process has been studied by many investigators [KO 45, Kra 64, Pe 66, Wi 741] over several decades. In the earlier investigations the exhalation process was studied in a purely geophysical context, but over the last 20 years it has been realized, that under certain conditions the exhalation may be intense enough to also have radiological implications. This is for example the case where relatively radium-rich wastes or by-products, like uranium mill tailings and phospho-gypsum, are stored in larger quantities. In order to be able to predict the radiological impact on the environnent it is necessary to know the rate of exhalation of radon from the surface of the exhaling material. Usually the determination of these exhalation rates has been done by measurements in situ directly upon the accumulated material [~le 74, Ha 791. Although such field measurements have the obvious merit of dealing directly with the full scale problem, the results are often lacking in generality, making predictions for other situations difficult or even impossible. The present paper describes some results of an investigation where it is attempted from laboratory measurements on samples of limited size to obtain material parameters, which are suited for extrapolating and predicting the radiational behaviour of larger accumulations of the material. THEORY Let us consider a sample of a radon exhaling material enclosed in a container with a dead space volume, Vd, and initially containing radon free air. If the total exhalation rate (number of atoms per unit time) is c, the radon concentration (number of atoms per unit volume) N will initially grow with the time t according to the equation [ ] where [R] is the decay constant of radon. As the concentration (or activity) in the container grows, the net exhalation rate will slow down because of back diffusion, and, furthermore, radon atoms may be removed from the container, not only by radioactive decay, but also by diffusion leakage [JO 81 ]. If, however,only the initial. part of the activity growth curve is considered, the total exhalation rate, c, is given by [c = r•Vd(2) where r is the initial activity growth rate in the container. Let the container be cylindrical with an inner cross-section S and filled to a height L with a radon exhaling material with the specific mass p, the porosity E, the radon pore production rate f and the diffusion length i. When the container is left open,i.e. the radon exhalation takes place into a virtually radon free room, the radon area exhalation rate, E, can be written [Jo 80] E = Ef?t tanh L.R (3) assuming the exhalation only takes place in one direction, towards the surface of the material. It appears that for values of L > 2•ithe area exhalation rate becomes E a = Efi (4) independently of the sample dimensions and the total exhalation rate c is then c = E •S (5) For L ;~ 0.5•i, tanh P _ k and equation (3) may be written E ~ EfL (6) then c = EfL•S = p•m= Em •m (7) where m is the mass of the sample and Em = P (8) is the mass exhalation rate. It thus appears that the radon exhalation rate from a given amount of material may often be conveniently expressed by c = E •Sfor L z 2•I (5) a orc = Em •mfor L0.5•i (7) where S is the total exhaling area and m the total exhaling mass, E and E the area and mass exhalation rates respectively defined by equations (4) and (8).]