Effect of quartz overgrowth precipitation on the multiscale porosity of sandstone: A (U)SANS and imaging analysis

Lawrence M. Anovitz, David R. Cole, Andrew J. Jackson, Gernot Rother, Kenneth C. Littrell, Lawrence F. Allard, Anthony D. Pollington, David J. Wesolowski

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Abstract

We have performed a series of experiments to understand the effects of quartz overgrowths on nanometer to centimeter scale pore structures of sandstones. Blocks from two samples of St. Peter Sandstone with different initial porosities (5.8% and 18.3%) were reacted from 3. days to 7.5. months at 100 and 200. °C in aqueous solutions supersaturated with respect to quartz by reaction with amorphous silica. Porosity in the resultant samples was analyzed using small and ultrasmall angle neutron scattering and scanning electron microscope/backscattered electron (SEM/BSE)-based image-scale processing techniques.Significant changes were observed in the multiscale pore structures. By 3. days much of the overgrowth in the low-porosity sample dissolved away. The reason for this is uncertain, but the overgrowths can be clearly distinguished from the original core grains in the BSE images. At longer times the larger pores are observed to fill with plate-like precipitates. As with the unreacted sandstones, porosity is a step function of size. Grain boundaries are typically fractal, but no evidence of mass fractal or fuzzy interface behavior was observed suggesting a structural difference between chemical and clastic sediments. After the initial loss of the overgrowths, image scale porosity (>~1. cm) decreases with time. Submicron porosity (typically ~25% of the total) is relatively constant or slightly decreasing in absolute terms, but the percent change is significant. Fractal dimensions decrease at larger scales, and increase at smaller scales with increased precipitation.

Original languageEnglish
Pages (from-to)199-222
Number of pages24
JournalGeochimica et Cosmochimica Acta
Volume158
DOIs
StatePublished - Jun 1 2015

Funding

Effort by L.M.A., G.R. and L.F.A. was supported by research sponsored by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy . D.R.C. was funded by the Department of Energy Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences through the Energy Frontier Research Center – Nanoscale Control of Geologic CO 2 . We acknowledge the support of the National Institute of Standards and Technology, Center for Neutron Research , U.S. Department of Commerce , and the High-Flux Isotope Reactor at the Oak Ridge National Laboratory in providing the research neutron facilities used in this work. This work utilized facilities supported in part by the National Science Foundation under agreement No. DMR-0944772 . Certain commercial equipment, instruments, materials and software are identified in this paper to foster understanding. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology, the Department of Energy, or the Oak Ridge National Laboratory, nor does it imply that the materials or equipment identified are necessarily the best available for the purpose. John Valley, Mike Spicuzza, Anthony Pollington, and Brian Hess at the University of Wisconsin–Madison provided samples as part of research sponsored by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy under contract 93ER14389 at the University of Wisconsin–Madison. Help and comments from Dr. Hsiu-Wen Wang were greatly appreciated. Atomic Adsorption analyses were performed by Leslie Wilson at ORNL. We would also like to thank Dr. Michael Schmid, Institut für Angewandte Physik, Technische Universität Wien, for his help with the ImageJ plugins for calculating the autocorrelation functions and scattering curves from the BSE images.

FundersFunder number
Department of Energy Office of Basic Energy Sciences
National Institute of Standards and Technology, Center for Neutron Research
National Science FoundationDMR-0944772
U.S. Department of Energy
U.S. Department of Commerce
Basic Energy Sciences
Oak Ridge National Laboratory
University of Wisconsin-Madison93ER14389
Chemical Sciences, Geosciences, and Biosciences Division

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