Geochemical and mineralogical impacts of sulfuric acid on clays between pH 5.0 and -3.0
type: CreativeWork
description: Natural and constructed clay liners are routinely used to contain waste and wastewater. The impact of acidic solutions on the geochemistry and mineralogy of clays has been widely investigated in relation to acid mine drainage systems at pH > 1.0. The impact of sulfuric acid leachate characterized by pH < 1.0, including potentially negative pH values on the geochemistry and mineralogy of clays is, however, not clear. To address this deficiency a series of batch and diffusion cell studies, investigating the geochemical and mineralogical impacts of H2SO4 solutions (pH 5.0 to -3.0), were conducted on three mineralogically distinct clays (Kc, Km, and BK). Batch testing was conducted at seven pH treatments (5.0, 3.0, 1.0, 0.0, -1.0, -2.0 and -3.0) using standardized sulfuric acid solutions for four exposure periods (14, 90, 180, and 365 d). Aqueous geochemical, XRD, and Si and Al XANES analyses showed: increased dissolution of aluminosilicates with decreasing pH and increasing exposure period; preferential dissolution of aluminosilicate Al-octahedral layers relative to Si-tetrahedral layers; formation of an amorphous silica-like phase that was confined to the surface layer of the altered clay samples at pH ≤ 0.0 and t ≥ 90 d; and precipitation of anhydrite and a Al-SO4-rich phase (pH ≤ -1.0, t ≥ 90 d). The diffusive transport of H2SO4 (pH =1.0, -1.0, and -3.0) through the Kc and Km clays for 216 d was examined using single reservoir, constant concentration, diffusion cells. The diffusive transport of H+ within the cells was modeled using 1-D transport models that assumed no absorption, linear absorption, and non-linear absorption of H+. The absorption isotherms were calculated from the pH 5.0, 3.0, and 1.0 batch experiment results, which were assumed representative of H+ absorption at pH < 1.0. However, model results indicated that the batch test results can not account for the observed H+ consumption in all cells and greatly underestimate the amount of H+ consumption in …
abstract: Natural and constructed clay liners are routinely used to contain waste and wastewater. The impact of acidic solutions on the geochemistry and mineralogy of clays has been widely investigated in relation to acid mine drainage systems at pH > 1.0. The impact of sulfuric acid leachate characterized by pH < 1.0, including potentially negative pH values on the geochemistry and mineralogy of clays is, however, not clear. To address this deficiency a series of batch and diffusion cell studies, investigating the geochemical and mineralogical impacts of H2SO4 solutions (pH 5.0 to -3.0), were conducted on three mineralogically distinct clays (Kc, Km, and BK). Batch testing was conducted at seven pH treatments (5.0, 3.0, 1.0, 0.0, -1.0, -2.0 and -3.0) using standardized sulfuric acid solutions for four exposure periods (14, 90, 180, and 365 d). Aqueous geochemical, XRD, and Si and Al XANES analyses showed: increased dissolution of aluminosilicates with decreasing pH and increasing exposure period; preferential dissolution of aluminosilicate Al-octahedral layers relative to Si-tetrahedral layers; formation of an amorphous silica-like phase that was confined to the surface layer of the altered clay samples at pH ≤ 0.0 and t ≥ 90 d; and precipitation of anhydrite and a Al-SO4-rich phase (pH ≤ -1.0, t ≥ 90 d). The diffusive transport of H2SO4 (pH =1.0, -1.0, and -3.0) through the Kc and Km clays for 216 d was examined using single reservoir, constant concentration, diffusion cells. The diffusive transport of H+ within the cells was modeled using 1-D transport models that assumed no absorption, linear absorption, and non-linear absorption of H+. The absorption isotherms were calculated from the pH 5.0, 3.0, and 1.0 batch experiment results, which were assumed representative of H+ absorption at pH < 1.0. However, model results indicated that the batch test results can not account for the observed H+ consumption in all cells and greatly underestimate the amount of H+ consumption in …
author: Shaw, Sean Adam
language: en_US
keywords: negative pH, geochemistry, clay, diffusion, acid mine drainage, mineralogy, Sulfur
date published: 2008-01-01
date modified: 2026-07-24T04:27:08Z
provider: University of Saskatchewan
publisher: Networked Digital Library of Theses and Dissertations
type: WebPage
source organization: University of Saskatchewan

PropertyValue
property ID: Handle
value: https://hdl.handle.net/10388/etd-11252008-122801