A new approach for measuring dissolution rates of silicate minerals by using silicon isotopes

Abstract

The two major problems in measuring dissolution rates under close-to-natural conditions in laboratory experiments are: (1) our inability to measure small differences in concentration between solutions with relatively high concentrations and (2) the inherent problem that the change in solution concentration is affected by both the dissolution of the primary mineral and the precipitation of secondary minerals. The present manuscript proposes and tests a novel method, “the isotope ratio method”, for measuring slow dissolution rates of silicate minerals by measuring the change in the ratios between stable isotopes of silicon of a spiked solution.Based on mass balance calculations, two equations that describe the dissolution rate of a silicate mineral in a batch reactor and in a flow-through reactor at steady-state are developed. The precipitation rate of the secondary mineral may be calculated by subtracting the release rate of Si that was calculated using isotope dilution from the rate that was calculated using the proposed isotope ratio method.Numerical simulations of flow-through and batch experiments demonstrate that the “isotope ratio method” is significantly more precise than conventional methods. The analytical uncertainty for the determination of dissolution rates was found to be low for the entire range of reported field-based dissolution rates. The calculation showed that even relatively large isotopic fractionations (up to ε values of 20‰), introduce insignificant uncertainties.Preliminary flow-through experiments support the above conclusion that dissolution rate may be obtained accurately and with small uncertainty using the proposed “isotope ratio method”.