Hellevang Helge, Aagaard Per, Oelkers Eric H, Kvamme Bjørn
Department of Physics and Technology, University of Bergen, Allégt. 55, 5009 Bergen, Norway.
Environ Sci Technol. 2005 Nov 1;39(21):8281-7. doi: 10.1021/es0504791.
Thermodynamic calculations indicate that although dawsonite (NaAlCO3(OH)2) is favored to form at the high CO2 pressures associated with carbon dioxide injection into sandstone reservoirs, this mineral will become unstable as CO2 pressure decreases following injection. To assess the degree to which dawsonite will persist following its formation in sandstone reservoirs, its dissolution rates have been measured at 80 +/- 3 degrees C as a function of pH from 3 to 10. Measured dawsonite dissolution rates normalized to their BET surface area are found to be nearly independent of pH over the range of 3.5 < pH < 8.6 at 1.58 x 10(-9) mol/(m2 x s). Use of these dissolution rates in reactive transport calculations indicate that dawsonite rapidly dissolves following the decrease of CO2 pressure out of its stability field, leading mainly to the precipitation of secondary kaolinite. This result indicates that dawsonite will provide a permanent mineral storage host only in systems that maintain high CO2 pressures, whereas dawsonite may be an ephemeral phase in dynamic settings and dissolve once high CO2 pressure dissipates either through dispersion or leakage.
热力学计算表明,虽然片钠铝石(NaAlCO3(OH)2)在与向砂岩储层注入二氧化碳相关的高二氧化碳压力下易于形成,但随着注入后二氧化碳压力降低,这种矿物将变得不稳定。为了评估片钠铝石在砂岩储层中形成后持续存在的程度,已在80±3℃下测量了其溶解速率,该速率是pH值从3到10的函数。在1.58×10−9 mol/(m2·s)的条件下,将测量得到的片钠铝石溶解速率归一化为其BET表面积后,发现在3.5<pH<8.6范围内,其溶解速率几乎与pH值无关。在反应输运计算中使用这些溶解速率表明,当二氧化碳压力降低到其稳定范围之外时,片钠铝石会迅速溶解,主要导致次生高岭石沉淀。这一结果表明,片钠铝石仅在维持高二氧化碳压力的系统中才会提供永久性的矿物储存载体,而在动态环境中,片钠铝石可能是一个短暂的相,一旦高二氧化碳压力通过扩散或泄漏消散,它就会溶解。