DOE OSTI2013
The objective of this suite of experiments was to develop a useful kinetic dissolution expression for chlorite that would be applicable over a wide range of solution pH and temperature conditions representative of subsurface conditions in natural and/or engineering geothermal reservoirs. The resulting rate equation is dependent on both pH and temperature and utilizes two specific dissolution mechanisms (an “acid” and a “neutral” mechanism). Rate parameters were derived from data collected at LLNL and available published data from Lowson et al. (2007). The form of this rate equation (Equation 1) should be easy to incorporate into most existing reactive transport codes for use in prediction of rock-water interactions in EGS systems. Specifically, we find that the dissolution of chlorite, a sheet-silicate, is relatively slow at elevated temperatures (100-275 °C), compared to other framework silicate minerals for which higher temperature kinetic data are available (e.g., quartz and feldspars; see Palandri and Kharaka, 2004). This finding is in conflict with previously reported high activation energies for chlorite based on extrapolation of low-temperature experimental data to higher temperatures. Additionally, we note that the dissolution of chlorite does not increase under alkaline conditions, as has been noted for other minerals, but rather remains at the same level as that noted for neutral conditions, with only a weak dependence on temperature. Future work includes similar rate measurements and the derivation of useful rate equations for illite, smectite, and biotite from pH 3 to 10 and 100 to 275 °C. Geochemical alteration, changing stress fields, mass transport and heat transfer incorporated into computational models are needed to optimize geothermal energy production for EGS systems. The resulting mineral rate equations from this work can be directly incorporated in modeling efforts to fully assess the impacts of geochemical alteration on long-term fracture permeability for EGS systems across the Geothermal Program. Chlorite rate equations and data have been submitted to the Geothermal Data Repository.