Scale dependence of mineral dissolution rates within single pores and fractures

Li, Li; Steefel, Carl I.; Yang, Li

doi:10.1016/j.gca.2007.10.027

Cited by 196 publications

(179 citation statements)

References 64 publications

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“…10, we used the geometric surface area for a 420 µm diameter calcite grain (in the middle of the range of the sieved grain size), with an additional surface roughness factor of 2.303 based on BET measurements of the initial calcite spar crystals. In the CrunchFlow calculations, all of the reacting surface area is considered to be present within a single spherical geometry grid cell of 0.1 µm thickness, as in the calculations presented in Li et al [2008]. The rest of the domain is solution only and mineral precipitation is not allowed.…”

Section: Reactive Transport Modelingmentioning

confidence: 99%

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Upscaling calcium carbonate precipitation rates from pore to continuum scale

et al. 2012

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The upscaling of calcite precipitation rates in porous media from the pore (micron) to continuum (centimeter) scale is evaluated with an integrated experimental and modeling approach. Experiments using cylindrical cores packed with glass beads and calcite (Iceland spar) crystals were injected over a period of 28 days with a supersaturated mixture of CaCl 2 and NaHCO 3 to induce calcite growth. Bulk rates of precipitation based on the change in aqueous chemistry over the length of the column are compared with spatially resolved determinations of carbonate precipitation using X-ray synchrotron microtomographic imaging at the micron scale. These data are supplemented by continuously-stirred reactor experiments using the same calcite seed material so as to minimize differences in the effects of reactive site density of the seed material, and to evaluate the rate of precipitation in the absence of transport or "porous medium" effects. Calcite precipitation rates determined in the stirred flowthrough reactor in this study are considerably slower than rates determined at similar supersaturation in unseeded batch experiments by Tang et al. [2008a], although these rates are compatible with those reported in Nehrke et al. [2007] for precipitation on Iceland spar when the same normalization to reactive surface area is used. The nearly linear dependence of the rates on supersaturation cannot be attributed to a diffusion control in the case of the stirred reactors and is likely the result of multi-sourced spiral growth.Integrated precipitation rates based on column effluent chemistry from a higher supersaturation experiment are in good agreement with determinations of total carbonate precipitated based on determination of pre-and post-experiment mass in the column using X-ray microtomography. Using the rates of precipitation determined in the well-stirred flowthrough reactors, it is possible to match the spatially-resolved microtomographic and aqueous data with a coarser resolution continuum model using volume-averaged flow and reactive surface area if the generation of new reactive surface area is accounted for. A nucleation or surface roughening event, which is most pronounced within two millimeters of the column inlet where the supersaturation is highest, is recorded by both BET analysis, which indicates an increase in specific surface area from 0.012 m 2 •g -1 to a value of 0.21 m 2 •g -1 for neoformed calcium carbonate, and by X-ray microtomography. The best fit of the column X-ray microtomography data is provided by simulating calcite precipitation either as a single nearly linear rate for multi-sourced spiral growth, or as two parallel rates that include the spiral growth model and a 2D heterogeneous nucleation model modified by a partial diffusion control, although nucleation needs to be relatively minor on a mass basis in order to match the data. The combined experiments and modeling indicate that it is possible to develop upscaled quantitative models for porous media reactivity, but changes in such propert...

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Section: Reactive Transport Modelingmentioning

confidence: 99%

“…It is highly likely that they do, as demonstrated by such studies as those of Li et al [2006]. Even at the single pore scale, gradients may develop under certain conditions, although Li et al [2008] demonstrated that for typical groundwater flow rates, gradients within single pores were unlikely.…”

Section: Introductionmentioning

confidence: 98%

Upscaling calcium carbonate precipitation rates from pore to continuum scale

et al. 2012

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“…1. This type of quenched disorder in the reaction and diffusion properties may occur in heterogeneous geological media characterized by a spatial distribution of minerals and thus specific reactive surface, and porosity [7], which leads to scale effects in the reaction properties [23,24].…”

Section: A Stochastic Decay Ratesmentioning

confidence: 99%

Reaction–diffusion with stochastic decay rates

Lapeyre

Dentz

2017

Phys. Chem. Chem. Phys.

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Understanding anomalous transport and reaction kinetics due to microscopic physical and chemical disorder is a long-standing goal in many fields including geophysics, biology, and engineering. We consider reaction-diffusion characterized by fluctuations in both transport times and decay rates. We introduce and analyze a model framework that explicitly connects microscopic fluctuations with the mescoscopic description. For broad distributions of transport and reaction time scales we compute the particle density and derive the equations governing its evolution, finding power-law decay of the survival probability, and spatially varying decay that leads to subdiffusion and an asymptotically stationary surviving-particle density. These anomalies are clearly attributable to non-Markovian effects that couple transport and chemical properties in both reaction and diffusion terms.

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“…Experimental studies of mineral dissolution kinetics (e.g., Hamilton et al 2001;Hellmann and Tisserand 2006;Yang and Steefel 2008;Pierce et al 2010) and of the related process of glass degradation (e.g., Strachan and Croak 2000;Advocet et al 2001;Wolf-Boenisch et al 2004;Pierce et al 2006;Cailleteau et al 2008) have provided data to show that there is a complex coupled feedback process that changes glass degradation from simple far-from equilibrium dissolution kinetics at the start to slower degradation controlled in part by diffusion processes in gel and secondary phase layer(s) in which the reaction solution has a modified composition near the surface (i.e., the reactive interface) of fresh glass (see Grambow 2006;Van Iseghem et al 2007). In these cases the compositional gradients of the solution need to be taken into account and evaluated on a smaller scale than the bulk solution (Li et al 2008) and the appropriate approach to developing models of this coupled reaction and transport system is in general a reactive transport methodology (e.g., Steefel et al 2005). This allows capture of both far-from equilibrium dissolution processes of the initial attack stage for glass as well as the evolved system with secondary phases, transport process limitations, locally modified solution composition, and changes to reactive interface surface areas.…”

Section: Current Understanding and Gap Identificationmentioning

confidence: 99%

Nuclear Energy Advanced Modeling and Simulation (NEAMS) Waste Integrated Performance and Safety Codes (IPSC) : FY10 development and integration.

Criscenti¹,

Sassani²,

Argüello³

et al. 2011

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This report describes the progress in fiscal year 2010 in developing the Waste Integrated Performance and Safety Codes (IPSC) in support of the U.S. Department of Energy (DOE) Office of Nuclear Energy Advanced Modeling and Simulation (NEAMS) Campaign. The goal of the Waste IPSC is to develop an integrated suite of computational modeling and simulation capabilities to quantitatively assess the long-term performance of waste forms in the engineered and geologic environments of a radioactive waste storage or disposal system. The Waste IPSC will provide this simulation capability (1) for a range of disposal concepts, waste form types, engineered repository designs, and geologic settings, (2) for a range of time scales and distances, (3) with appropriate consideration of the inherent uncertainties, and (4) in accordance with robust verification, validation, and software quality requirements.Waste IPSC activities in fiscal year 2010 focused on specifying a challenge problem to demonstrate proof of concept, developing a verification and validation plan, and performing an initial gap analyses to identify candidate codes and tools to support the development and integration of the Waste IPSC. The current Waste IPSC strategy is to acquire and integrate the necessary Waste IPSC capabilities wherever feasible, and develop only those capabilities that cannot be acquired or suitably integrated, verified, or validated. This year-end progress report documents the FY10 status of acquisition, development, and integration of thermal-hydrologicchemical-mechanical (THCM) code capabilities, frameworks, and enabling tools and infrastructure.iv ACKNOWLEDGEMENTS

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Scale dependence of mineral dissolution rates within single pores and fractures

Cited by 196 publications

References 64 publications

Upscaling calcium carbonate precipitation rates from pore to continuum scale

Upscaling calcium carbonate precipitation rates from pore to continuum scale

Reaction–diffusion with stochastic decay rates

Nuclear Energy Advanced Modeling and Simulation (NEAMS) Waste Integrated Performance and Safety Codes (IPSC) : FY10 development and integration.

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