Water–rock interactions in the Bruchsal geothermal system by U–Th series radionuclides

Abstract

Uranium and thorium decay series disequilibria in deep geothermal brines are a result of water–rock interaction processes. The migratory behavior of radionuclides provides valuable site-specific information and can therefore be an important tool for reservoir characterization and sustainable management of geothermal sites. In this study, we present data from long-term monitoring of naturally occurring 238U, 232Th and 235U series radionuclides analyzed in brine samples collected from the Permo-Triassic sedimentary reservoir rock at the Bruchsal geothermal site (SW Germany). The results show that radionuclides of the elements radium (226Ra, 228Ra, 224Ra, 223Ra), radon (222Rn), and lead (210Pb, 212Pb) are rather soluble in brine, while isotopes of uranium (238U, 234U, 235U), thorium (232Th, 228Th, 230Th), polonium (210Po), and actinium (227Ac, 228Ac) have low solubilities and are mostly immobile. Activities of radium isotopes in the geothermal brine exceed those of their thorium progenitors (average 226Ra = 29.9 Bq kg−1, about 103 times that of its 230Th parent). Modelling the observed disequilibria allows the following conclusion on water–rock interaction processes: (1) supply from alpha-recoil depends on isotope half-life because it is limited by the rate of diffusion through microfractures causing isotopic fractionation. (2) Radium retardation due to adsorption is low (226Ra/222Rn = 1.3) resulting in adsorption–desorption rate constants in the order of 10−10 s−1 for k1 and 10−9 for k2. (3) Scavenging of 226Ra from brine can best be explained by co-precipitation with barite resulting in an observed 226Ra anomaly in the solids of the reservoir section. The precipitation rate constant amounts to ca. 3.4 × 10−8 s−1 corresponding to a mean removal time of radium from brine by mineral precipitation to approximately 1 year.