Description: This report provides a description of the main accomplishments of the EMSP funded research, including products such as conference presentations and publications (including those still in preparation). The purpose of this study was to better understand the chemical interactions between dissolved aqueous contaminants and carbonate minerals occurring as coatings on mineral grains in the vadose zone beneath the Hanford reserve. This information is important for construction of improved reactive transport models intended to predict the subsurface migration of contaminants. We made improvements to the hydrothermal atomic force microscope (HAFM) design to be used in this project. The original HAFM was built with funding from the U.S. DOE, Office of Basic Energy Sciences. Improvements include operating limits of 70 bars and 170 C, from an original limit of 12 bars and 150 C. This product is patented. We completed a series of studies of magnesite, MgCO3, because this mineral is structurally equivalent to calcite but reacts much more slowly, allowing us to study carbonate reactivity under pH conditions (i.e., low pH) that are much more problematic for studies of calcite but which are nevertheless relevant to in-situ conditions. We found that dissolving magnesite exhibits a dramatic change in step orientation, and therefore etch pit shape, as pH is lowered through 4.2 to 3 and 2. This change in step orientation is NOT accompanied by an increase in step velocity with decreasing pH. We also found that, after growing magnesite on a magnesite substrate, the newly grown magnesite dissolved much more readily than the underlying substrate magnesite, and exhibited far larger etch pit densities. This effect may have been related to the rate of growth or to the presence of an Fe impurity in the growth solutions. We studied the dissolution of magnesite and calcite (104) surfaces under a wider variety of ...
Date: December 12, 2003
Creator: Eggleston, Carrick M.
Partner: UNT Libraries Government Documents Department