Time-dependent shapes of a dissolving mineral grain: Comparisons of simulations with microfluidic experiments

Filip Dutka; Vitaliy Starchenko; Florian Osselin; Silvana Magni; Piotr Szymczak; Anthony J.C. Ladd

doi:10.1016/j.chemgeo.2019.119459

Time-dependent shapes of a dissolving mineral grain: Comparisons of simulations with microfluidic experiments

Filip Dutka, Vitaliy Starchenko, Florian Osselin, Silvana Magni, Piotr Szymczak, Anthony J.C. Ladd

Geochemistry & Interfacial Science

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

Experimental observations of the dissolution of calcium sulfate by flowing water have been used to investigate the assumptions underlying pore-scale models of reactive transport. Microfluidic experiments were designed to observe changes in size and shape as cylindrical disks (radius 10 mm) of gypsum dissolved for periods of up to 40 days. The dissolution flux over the whole surface of the sample can be determined by observing the motion of the interface. However, in order to extract surface reaction rates, numerical simulations are required to account for diffusional hindrance across the concentration boundary layer; the geometry is too complex for analytic solutions. We have found that a first-principles simulation of pore-scale flow and transport, with a single value of the surface reaction rate, was able to reproduce the time sequence of sample shapes without any fitting parameters. The value of the rate constant is close to recent experimental measurements but much smaller than some earlier values. The shape evolution is a more stringent test of the validity of the method than average measurements such as effluent concentration, because it requires the correct flux at each point on the sample surface.

Original language	English
Article number	119459
Journal	Chemical Geology
Volume	540
DOIs	https://doi.org/10.1016/j.chemgeo.2019.119459
State	Published - May 5 2020

Funding

We gratefully acknowledge the advice and support from Prof. Piotr Garstecki (Polish Academy of Sciences) in setting up the microfluidic experiments, and for comments on the manuscript. We thank the ASTAT Company (Poznań, Poland) for providing us with the ultrathin double-coated tape used in the experiments). Numerical data was generated with the OpenFOAM Ⓡ toolkit (v1712), http://www.openfoam.com/ . Source codes and sample input files used to produce the numerical data shown in this paper can be found at https://github.com/vitst/dissolFoam/releases/tag/v1712 . Additional output data is available on request. AJCL was funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under Award Number DE-SC0018676 . Research by VS was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U. S. Department of Energy. FD, FO, SM and PS acknowledge the support by the National Science Center (Poland) under research grant no. 2012/07/E/ST3/01734 . We gratefully acknowledge the advice and support from Prof. Piotr Garstecki (Polish Academy of Sciences) in setting up the microfluidic experiments, and for comments on the manuscript. We thank the ASTAT Company (Poznań, Poland) for providing us with the ultrathin double-coated tape used in the experiments). Numerical data was generated with the OpenFOAMⓇ toolkit (v1712), http://www.openfoam.com/. Source codes and sample input files used to produce the numerical data shown in this paper can be found at https://github.com/vitst/dissolFoam/releases/tag/v1712. Additional output data is available on request. AJCL was funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under Award Number DE-SC0018676. Research by VS was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U. S. Department of Energy. FD, FO, SM and PS acknowledge the support by the National Science Center (Poland) under research grant no. 2012/07/E/ST3/01734.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Chemical Sciences, Geosciences, and Biosciences Division	DE-SC0018676
Narodowe Centrum Nauki	2012/07/E/ST3/01734
Polska Akademia Nauk	v1712

Keywords

Dissolution rate
Gypsum dissolution
Pore scale modeling
Reactive surface area
Simulation and experiment

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10.1016/j.chemgeo.2019.119459

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title = "Time-dependent shapes of a dissolving mineral grain: Comparisons of simulations with microfluidic experiments",

abstract = "Experimental observations of the dissolution of calcium sulfate by flowing water have been used to investigate the assumptions underlying pore-scale models of reactive transport. Microfluidic experiments were designed to observe changes in size and shape as cylindrical disks (radius 10 mm) of gypsum dissolved for periods of up to 40 days. The dissolution flux over the whole surface of the sample can be determined by observing the motion of the interface. However, in order to extract surface reaction rates, numerical simulations are required to account for diffusional hindrance across the concentration boundary layer; the geometry is too complex for analytic solutions. We have found that a first-principles simulation of pore-scale flow and transport, with a single value of the surface reaction rate, was able to reproduce the time sequence of sample shapes without any fitting parameters. The value of the rate constant is close to recent experimental measurements but much smaller than some earlier values. The shape evolution is a more stringent test of the validity of the method than average measurements such as effluent concentration, because it requires the correct flux at each point on the sample surface.",

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AU - Ladd, Anthony J.C.

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N2 - Experimental observations of the dissolution of calcium sulfate by flowing water have been used to investigate the assumptions underlying pore-scale models of reactive transport. Microfluidic experiments were designed to observe changes in size and shape as cylindrical disks (radius 10 mm) of gypsum dissolved for periods of up to 40 days. The dissolution flux over the whole surface of the sample can be determined by observing the motion of the interface. However, in order to extract surface reaction rates, numerical simulations are required to account for diffusional hindrance across the concentration boundary layer; the geometry is too complex for analytic solutions. We have found that a first-principles simulation of pore-scale flow and transport, with a single value of the surface reaction rate, was able to reproduce the time sequence of sample shapes without any fitting parameters. The value of the rate constant is close to recent experimental measurements but much smaller than some earlier values. The shape evolution is a more stringent test of the validity of the method than average measurements such as effluent concentration, because it requires the correct flux at each point on the sample surface.

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Time-dependent shapes of a dissolving mineral grain: Comparisons of simulations with microfluidic experiments

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Keywords

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