『Abstract
This study explores the dynamics of porosity and reactive surface
area changes during porous limestone dissolution by CO2-rich
water. The Sr and Ca concentrations in both the rock and the outlet
solution are used to evaluate the reactive surface area changes
of the two rock-forming calcites, i.e. micrite grains and sparite
crystals, which have different trace element signatures. The geometric
surface area measured with X-ray microtomography decreases slightly
whereas the reactive surface area increases continuously with
increasing porosity from 20.3 to 30.2%. Surprisingly, changes
in reactive surface areas are very different between the two calcites.
The reactive surface area changes in the micrite are parabolic
while the reactive surface area of sparite increases greatly.
The numerical model HYTEC is used to model the change in reactive
surface areas during the experiment. Different geometrical models
are tested. The model based on spherical-grain dissolution and
spherical-pore growth fails to reproduce the experimental results,
while the sugar-lump model provides reasonable agreement with
the experiment.
Keywords: Reactive surface area; Reactive transport; Modelling;
Carbon dioxide; Dissolution; Limestone』
1. Introduction
1.1. Surface areas of rocks
2. Materials and methods
2.1. Rock sample
2.2. Flow-through experiment
2.3. X-ray microtomography
2.4. Analysis of 3D geometry with X-ray microtomography
2.5. Measurement of major and minor element by ICP-AES and ICP-MS
2.6. Secondary ion mass spectroscopy and ion microprobe analysis
3. Results
3.1. Minor and trace element chemistry of the rock sample
3.2. Porosity and permeability changes
3.3. Solution chemistry
3.4. Surface area changes
3.4.1. Geometric surface area
3.4.2. Reactive surface area
5. Discussion
6. Conclusion
Acknowledgments
References