Time-lapse 3D imaging of calcite precipitation in a microporous column

• Published in: Geochimica et cosmochimica acta Vol. 222; pp. 156 - 170
• Main Authors: Godinho, Jose R.A., Withers, Philip J.
• Format: Journal Article
• Language: English
• Published: Elsevier Ltd 01.02.2018
• Subjects: Calcite; Growth rate; Helical CT; Permeability; Porous media; Precipitation; Porous media; Helical CT; Precipitation; Permeability; Growth rate; Calcite
• ISSN: 0016-7037; 1872-9533
• DOI: 10.1016/j.gca.2017.10.024

Time-lapse X-ray computed tomography is used to image the evolution of calcite precipitation during flow through microporous quartz over the course of 400 h. The growth rate decreases by more than seven times, which is linked to the clogging of flow paths that restricts flow to some regions of the column. Fewer precipitates are observed as a function of column depth, which is found to be related to a differential nucleation density along the sample. A higher nucleation density closer to the inlet implies more crystal volume increase per unit of time without affecting the rate if normalized to the surface area of crystals. Our overall growth rates measured in porous media are orders of magnitude slower than growth rates derived from traditional precipitation experiments on free surfaces. Based on our time-lapse results we hypothesize a scenario where the evolving distribution of precipitates within a pore structure during precipitation progressively modifies the local transport through the pores. Within less permeable regions the saturation index may be lower than along the main flow paths. Therefore, the reactive crystal surfaces within those regions grow at a slower rate than that expected from the bulk fluid composition. Since the amount of reactive surface area within these less permeable regions increases over time, the overall growth rate decreases without a necessary significant change of the bulk fluid composition along more permeable flow paths. In conclusion, the overall growth rates in an evolving porous media expected from bulk fluid compositions alone can be overestimated due to the development of stagnant sub-regions where the reactive surface area is bath by a solution with lower saturation index. In this context we highlight the value of time-lapse 3D studies for understanding the dynamics of mineral precipitation in porous media.