Evolution of a Generic Clay/Cement Interface: First Reactive Transport Calculations Utilizing a Gibbs Energy Minimization Based Approach for Geochemical Calculations

Kosakowski, Georg; Blum, Philipp; Kulik, Dmitrii A.; Pfingsten, Wilfried; Shao, Haibing; Singh, Ashutosh

doi:10.3107/jesss.3.41

Cited by 8 publications

(3 citation statements)

References 25 publications

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“…However, the application of this relationship depends upon specific calibration to the system under study and thus cannot be applied a priori (e.g. Kosakowski et al, 2009). Moreover, it is important for predictive modelling (especially in fractured rocks) to have a better understanding of how porosity/fractures may be occluded due to the precipitation of neoformed minerals.…”

Section: Porosity-permeability Modif|cationmentioning

confidence: 99%

A review of analogues of alkaline alteration with regard to long-term barrier performance

Savage¹

2011

Mineral. mag.

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Cement and concrete will be used as fracture grouts, shotcrete, tunnel and borehole seals, and as matrices for waste encapsulation inter alia in geological repositories for radioactive wastes. Alteration of the host rock and/or swelling clay in waste package buffers and tunnel backfills by hyperalkaline solutions from cement/concrete may be deleterious to system performance through changes in the physicochemical properties of these barrier materials.Analogue systems (and timescales) relevant to the understanding of the alkaline disturbed zone include: industrial analogues, such as alkaline flooding of hydrocarbon reservoirs (up to 30 y), cementaggregate reactions (up to 100 y) and the Tournemire tunnel (up to 125 y); and natural analogues, including the hyperalkaline springs at Maqarin, Jordan (more than 100,000 y), saline, alkaline lakes (more than 1,000,000 y) and certain fracture fillings in granites (more than 1,000,000 y).These systems show that alkaline alteration can be observed for thousands of years over distance scales of hundreds of metres under extreme conditions of hydraulic gradients in fractured rocks (Maqarin), but may be limited to a few centimetres over tens to a hundred years in mudstone (Tournemire). Important reaction mechanisms for retardation of alkaline fluids include: fluid mixing (alkaline oil floods, Maqarin), ion exchange (alkaline oil floods, Tournemire) and kinetic mineral dissolution-precipitation reactions (all systems studied). Qualitative and quantitative kinetic data for mineral reactions are available from cement aggregate reactions and the Searles Lake analogue, respectively. Short-term alteration observed in cement-aggregates is characterized by calcium silicate hydrate (C-S-H) minerals and incipient zeolite formation, whereas evidence from the Tournemire tunnel shows the growth of K-feldspar after relatively short time intervals (tens to a hundred years). There is a tendency for alkaline alteration to result in porosity decreases, but locally, porosity may be enhanced (e.g. near-injection well interactions in alkaline oil floods, or at fracture margins at Maqarin, Jordan). Data from industrial and natural analogues may thus supply some key data for bridging time and space scales between laboratory and in situ experiments on one hand and the requirements for safety assessment on the other.

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Section: Porosity-permeability Modif|cationmentioning

confidence: 99%

A review of analogues of alkaline alteration with regard to long-term barrier performance

Savage¹

2011

Mineral. mag.

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“…To simplify the model, boric acid interaction with the aggregate was assumed to be negligible and the aggregate in the model was represented by the relatively insoluble mineral rutile (TiO 2 ). Kosakowski, et al (2009) [5] employed a similar approach and used SnO 2 to represent inert components in their cement model. Values of concrete porosity and pore diffusion coefficient were set equal to 0.07 and 1  10 6 cm 2 /s, respectively [4].…”

Section: Reactive Transport Modelingmentioning

confidence: 99%

Experimental Study and Reactive Transport Modeling of Boric Acid Leaching of Concrete

Pabalan

Chiang

2013

EPJ Web of Conferences

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Abstract. Borated water leakage through spent fuel pools (SFPs) at pressurized water reactors is a concern because it could cause corrosion of reinforcement steel in the concrete structure, compromise the integrity of the structure, or cause unmonitored releases of contaminated water to the environment. Experimental data indicate that pH is a critical parameter that determines the corrosion susceptibility of rebar in borated water and the degree of concrete degradation by boric acid leaching. In this study, reactive transport modeling of concrete leaching by borated water was performed to provide information on the solution pH in the concrete crack or matrix and the degree of concrete degradation at different locations of an SFP concrete structure exposed to borated water. Simulations up to 100 years were performed using different boric acid concentrations, crack apertures, and solution flow rates. Concrete cylinders were immersed in boric acid solutions for several months and the mineralogical changes and boric acid penetration in the concrete cylinder were evaluated as a function of time. The depths of concrete leaching by boric acid solution derived from the reactive transport simulations were compared with the measured boric acid penetration depth.

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“…Particularly challenging from the computational point of view are the simulations of systems in which precipitation and/or dissolution reactions led to significant changes of porosity in the media. Strong porosity changes typically observed at interfaces of engineered technical barriers and natural rock formations with different geochemical characteristics, e.g., clay and cement interfaces [ Marty et al , 2009; Kosakowski et al , 2009; De Windt et al , 2004]. Mineral precipitation in aquifers and reservoirs change their transport properties significantly and may lead eventually to complete clogging of the pore space [ Saripalli et al , 2001].…”

Section: Introductionmentioning

confidence: 99%

A class of analytical solutions for multidimensional multispecies diffusive transport coupled with precipitation‐dissolution reactions and porosity changes

Hayek¹,

Kosakowski²,

Jakob³

et al. 2012

Water Resources Research

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[1] One of the challenging problems in mathematical geosciences is the determination of analytical solutions of nonlinear partial differential equations describing transport processes in porous media. We are interested in diffusive transport coupled with precipitation-dissolution reactions. Several numerical computer codes that simulate such systems have been developed. Analytical solutions, if they exist, represent an important tool for verification of numerical solutions. We present a methodology for deriving such analytical solutions that are exact and explicit in space and time variables. They describe transport of several aqueous species coupled to precipitation and dissolution of a single mineral in one, two, and three dimensions. As an application, we consider explicit analytical solutions for systems containing one or two solute species that describe the evolution of solutes and solid concentrations as well as porosity. We use one of the proposed analytical solutions to test numerical solutions obtained from two conceptually different reactive transport codes. Both numerical implementations could be verified with the help of the analytical solutions and show good agreement in terms of spatial and temporal evolution of concentrations and porosities.Citation: Hayek, M., G. Kosakowski, A. Jakob, and S. V. Churakov (2012), A class of analytical solutions for multidimensional multispecies diffusive transport coupled with precipitation-dissolution reactions and porosity changes, Water Resour. Res., 48, W03525,

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Evolution of a Generic Clay/Cement Interface: First Reactive Transport Calculations Utilizing a Gibbs Energy Minimization Based Approach for Geochemical Calculations

Cited by 8 publications

References 25 publications

A review of analogues of alkaline alteration with regard to long-term barrier performance

A review of analogues of alkaline alteration with regard to long-term barrier performance

Experimental Study and Reactive Transport Modeling of Boric Acid Leaching of Concrete

A class of analytical solutions for multidimensional multispecies diffusive transport coupled with precipitation‐dissolution reactions and porosity changes

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