Specific surface area determinations on intact drillcores and evaluation of extrapolation methods for rock matrix surfaces

摘要

Permanent storage of spent nuclear fuel in crystalline bedrock is investigated in several countries. For this storage scenario, the host rock is the third and final barrier for radionuclide migration. Sorption reactions in the crystalline rock matrix have strong retardative effects on the transport of radionuclides. To assess the barrier properties of the host rock it is important to have sorption data representative of the undisturbed host rock conditions. Sorption data is in the majority of reported cases determined using crushed rock. Crushing has been shown to increase a rock samples sorption capacity by creating additional surfaces. There are several problems with such an extrapolation. In studies where this problem is addressed, simple models relating the specific surface area to the particle size are used to extrapolate experimental data to a value representative of the host rock conditions. In this article, we report and compare surface area data of five size fractions of crushed granite and of 100 mm long drillcores as determined by the Brunauer Emmet Teller (BET)-method using N_2-gas. Special sample holders that could hold large specimen were developed for the BET measurements. Surface area data on rock samples as large as the drillcore has not previously been published. An analysis of this data show that the extrapolated value for intact rock obtained from measurements on crushed material was larger than the determined specific surface area of the drillcores, in some cases with more than 1000%. Our results show that the use of data from crushed material and current models to extrapolate specific surface areas for host rock conditions can lead to over estimation interpretations of sorption ability. The shortcomings of the extrapolation model are discussed and possible explanations for the deviation from experimental data are proposed.