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Title: Chemical controls on the propagation rate of fracture in calcite

Calcite (CaCO 3) is one of the most abundant minerals in the Earth’s crust, and it is susceptible to subcritical chemically-driven fracturing. Understanding chemical processes at individual fracture tips, and how they control the development of fractures and fracture networks in the subsurface, is critical for carbon and nuclear waste storage, resource extraction, and predicting earthquakes. Chemical processes controlling subcritical fracture in calcite are poorly understood. We demonstrate a novel approach to quantify the coupled chemical-mechanical effects on subcritical fracture. The calcite surface was indented using a Vickers-geometry indenter tip, which resulted in repeatable micron-scale fractures propagating from the indent. Individual indented samples were submerged in an array of aqueous fluids and an optical microscope was used to track the fracture growth in situ. The fracture propagation rate varied from 1.6 × 10 -8 m s -1 to 2.4 × 10 -10 m s -1. The rate depended on the type of aqueous ligand present, and did not correlate with the measured dissolution rate of calcite or trends in zeta-potential. We postulate that chemical complexation at the fracture tip in calcite controls the growth of subcritical fracture. Previous studies indirectly pointed to the zeta-potential being the most critical factor, whilemore » our work indicates that variation in the zeta-potential has a secondary effect.« less
Authors:
 [1] ;  [2] ;  [1] ; ORCiD logo [3] ; ORCiD logo [4] ;  [2]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Geochemistry Dept.
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Nanosystems Synthesis/Analysis Dept., Center for Integrated Nanotechnologies
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Geomechanics Dept.
  4. Univ. of New Mexico, Albuquerque, NM (United States). Advanced Materials Lab.
Publication Date:
Report Number(s):
SAND-2018-14261J
Journal ID: ISSN 2045-2322; 671042
Grant/Contract Number:
AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1492352

Ilgen, A. G., Mook, W. M., Tigges, A. B., Choens, R. C., Artyushkova, K., and Jungjohann, K. L.. Chemical controls on the propagation rate of fracture in calcite. United States: N. p., Web. doi:10.1038/s41598-018-34355-1.
Ilgen, A. G., Mook, W. M., Tigges, A. B., Choens, R. C., Artyushkova, K., & Jungjohann, K. L.. Chemical controls on the propagation rate of fracture in calcite. United States. doi:10.1038/s41598-018-34355-1.
Ilgen, A. G., Mook, W. M., Tigges, A. B., Choens, R. C., Artyushkova, K., and Jungjohann, K. L.. 2018. "Chemical controls on the propagation rate of fracture in calcite". United States. doi:10.1038/s41598-018-34355-1. https://www.osti.gov/servlets/purl/1492352.
@article{osti_1492352,
title = {Chemical controls on the propagation rate of fracture in calcite},
author = {Ilgen, A. G. and Mook, W. M. and Tigges, A. B. and Choens, R. C. and Artyushkova, K. and Jungjohann, K. L.},
abstractNote = {Calcite (CaCO3) is one of the most abundant minerals in the Earth’s crust, and it is susceptible to subcritical chemically-driven fracturing. Understanding chemical processes at individual fracture tips, and how they control the development of fractures and fracture networks in the subsurface, is critical for carbon and nuclear waste storage, resource extraction, and predicting earthquakes. Chemical processes controlling subcritical fracture in calcite are poorly understood. We demonstrate a novel approach to quantify the coupled chemical-mechanical effects on subcritical fracture. The calcite surface was indented using a Vickers-geometry indenter tip, which resulted in repeatable micron-scale fractures propagating from the indent. Individual indented samples were submerged in an array of aqueous fluids and an optical microscope was used to track the fracture growth in situ. The fracture propagation rate varied from 1.6 × 10-8 m s-1 to 2.4 × 10-10 m s-1. The rate depended on the type of aqueous ligand present, and did not correlate with the measured dissolution rate of calcite or trends in zeta-potential. We postulate that chemical complexation at the fracture tip in calcite controls the growth of subcritical fracture. Previous studies indirectly pointed to the zeta-potential being the most critical factor, while our work indicates that variation in the zeta-potential has a secondary effect.},
doi = {10.1038/s41598-018-34355-1},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {2018},
month = {11}
}

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