Does the reactive surface area of sandstone depend on water saturation?—The role of reactive-transport in water film

Nishiyama, Naoki; Yokoyama, Tadashi

doi:10.1016/j.gca.2013.08.024

Cited by 27 publications

(22 citation statements)

References 65 publications

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“…The surface areas are in the high end of literature values for grounded magnesite ( 0.0662 to 0.224 m 2 /g) (Pokrovsky et al, 2005;Saldi et al, 2012) and are similar to those of chalk cores from carbonate reservoirs around 2.0 m 2 /g (Austad et al, 2012). The quartz BET surface area of 0.10 m 2 /g, similar to literature values between 0.06 to 0.10 m 2 /g (Colon et al, 2004;Nishiyama and Yokoyama, 2013). The magnesite volume percentages in all columns are 11.02 %±0.20% and 10.55%±0.06% of the total solid volume for the MgHigh and MgLow columns, respectively.…”

Section: Column Experimentssupporting

confidence: 82%

The role of magnesite spatial distribution patterns in determining dissolution rates: When do they matter?

Salehikhoo

2015

Geochimica et Cosmochimica Acta

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We systematically explore the role of magnesite distribution patterns in dictating its dissolution rates under an array of flow velocity and permeability contrast conditions using flow-through column experiments and reactive transport modeling. Columns were packed with magnesite distributed within quartz matrix in different spatial patterns: the Mixed column has uniformly distributed magnesite while the zonation columns contain magnesite in different number of zones parallel to the main flow. Dissolution rates are highest under conditions that maximize the water flowing through the magnesite zone. This occurs under fast flow and high-permeability or uniformly distributed magnesite zones. Under high flow and low permeability magnesite conditions, dissolution only occurs at the magnesite-quartz interface, leading to rates an order of magnitude lower in the One-zone columns than those in the Mixed columns. Spatial patterns do not make a difference under low flow when the system approaches equilibrium (v < 0.36 m/d) or under high permeability magnesite conditions. The bulk column-scale rate depends on A e through , where A e is the surface area that effectively dissolves with IAP/K eq < 0.1. The rate constant of 10-9.60 is very close to 10-10.0 mol/m 2 /s under well-mixed conditions, suggesting the potential resolution of laboratory-field rate discrepancy when A e , instead of the total BET surface area A T , is used. The A e values are 1 to 3 orders of magnitude lower than A T. The effectively-dissolving magnesite-quartz interface area ranges between 60~100% of A e , pointing the importance of "reactive interfaces" in heterogeneous porous media. This work quantifies the significance of magnesite spatial distribution patterns and has important implications in understanding biogeochemical processes and ecosystem functioning in the Critical Zone, as well as energy extraction from the deep subsurface.

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Section: Column Experimentssupporting

confidence: 82%

The role of magnesite spatial distribution patterns in determining dissolution rates: When do they matter?

Salehikhoo

2015

Geochimica et Cosmochimica Acta

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“…The parameter ϕ open was determined based on the difference between the water‐saturated and dry weights of the sample. The procedure to saturate the pores with water was the same as that used in Yokoyama [] and Nishiyama and Yokoyama []: the dried sample and water were separately placed in bottles; the bottles inserted in a vacuum chamber were degassed; water was poured into the bottle containing the sample while degassing; and finally, the chamber was ventilated, and the rock pores were saturated with water. The parameter ϕ tra was determined from the volume of water expelled to the upper end of the sample by exerting a high differential gas pressure Δ P = Δ P high on the water‐saturated sample (Figure ).…”

Section: Methodsmentioning

confidence: 99%

Permeability of porous media: Role of the critical pore size

2017

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The knowledge of the permeability of porous media is crucial to understand fluid flow in various natural and artificial materials. Due to the complex nature of pore structure, the pore characteristic (porosity and pore radius) determining the permeability has long been under discussion. Here we determined the critical pore radius, which is the radius of the largest sphere that can freely pass through a porous medium, using the water expulsion method, an experimental technique measuring the pressure at which gas passes through a water‐saturated porous medium. We demonstrate that the critical pore radius correlates well with the permeability for a variety of porous granular media and volcanic products with an extensive range of porosities (0.71%–50%) and permeabilities (10−20–10−10 m2). We also obtained a porosity‐critical pore radius‐permeability relationship that provides a better prediction of the permeability compared with predictions obtained by previous correlations.

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“…Ferrihydrite likely trapped and concentrated the resultant AspAsp even from a dilute aqueous solution. If a ferrihydrite-coated sandstone with 10% porosity, which corresponds to the pore volume to mass ratio of 0.042 L•kg −1 [75], is considered, 0.1 wt% of ferrihydrite enables the accumulation of 1.4 mmol AspAsp per one-kilogram of sandstone from a 0.01 mM AspAsp-containing solution at pH 4 (background electrolyte: 1 mM NaCl). The accumulated AspAsp will eventually be released through the aging of ferrihydrite, but its transportation with limited diffusion onto a catalytic surface may lead to the next stage of peptide bonding.…”

Section: Thermodynamic Prediction Of Asp Dimerization At the Mineral-water Interfacementioning

confidence: 99%

Thermodynamic Impact of Mineral Surfaces on Amino Acid Polymerization: Aspartate Dimerization on Two-Line Ferrihydrite, Anatase, and γ-Alumina

2021

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The presence of amino acids in diverse extraterrestrial materials has suggested that amino acids are widespread in our solar system, serving as a common class of components for the chemical evolution of life. However, there are a limited number of parameters available for modeling amino acid polymerization at mineral–water interfaces, although the interfacial conditions inevitably exist on astronomical bodies with surface liquid water. Here, we present a set of extended triple-layer model parameters for aspartate (Asp) and aspartyl-aspartate (AspAsp) adsorptions on two-line ferrihydrite, anatase, and γ-alumina determined based on the experimental adsorption data. By combining the parameters with the reported thermodynamic constants for amino acid polymerization in water, we computationally demonstrate how these minerals impact the AspAsp/Asp equilibrium over a wide range of environmental conditions. It was predicted, for example, that two-line ferrihydrite strongly promotes Asp dimerization, leading to the AspAsp/Asp ratio in the adsorbed state up to 41% even from a low Asp concentration (0.1 mM) at pH 4, which is approximately 5 × 107 times higher than that attainable without mineral (8.5 × 10−6%). Our exemplified approach enables us to screen wide environmental settings for abiotic peptide synthesis from a thermodynamic perspective, thereby narrowing down the geochemical situations to be explored for life’s origin on Earth and Earth-like habitable bodies.

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Does the reactive surface area of sandstone depend on water saturation?—The role of reactive-transport in water film

Cited by 27 publications

References 65 publications

The role of magnesite spatial distribution patterns in determining dissolution rates: When do they matter?

The role of magnesite spatial distribution patterns in determining dissolution rates: When do they matter?

Permeability of porous media: Role of the critical pore size

Thermodynamic Impact of Mineral Surfaces on Amino Acid Polymerization: Aspartate Dimerization on Two-Line Ferrihydrite, Anatase, and γ-Alumina

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