Chemical and Mechanical Properties of Wellbore Cement Altered by CO2-Rich Brine Using a Multianalytical Approach
Abstract
Defining chemical and mechanical alteration of wellbore cement by CO(2)-rich brines is important for predicting the long-term integrity of wellbores in geologic CO(2) environments. We reacted CO(2)-rich brines along a cement-caprock boundary at 60 °C and pCO(2) = 3 MPa using flow-through experiments. The results show that distinct reaction zones form in response to reactions with the brine over the 8-day experiment. Detailed characterization of the crystalline and amorphous phases, and the solution chemistry show that the zones can be modeled as preferential portlandite dissolution in the depleted layer, concurrent calcium silicate hydrate (CSH) alteration to an amorphous zeolite and Ca-carbonate precipitation in the carbonate layer, and carbonate dissolution in the amorphous layer. Chemical reaction altered the mechanical properties of the core lowering the average Young's moduli in the depleted, carbonate, and amorphous layers to approximately 75, 64, and 34% of the unaltered cement, respectively. The decreased elastic modulus of the altered cement reflects an increase in pore space through mineral dissolution and different moduli of the reaction products.
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The extent of carbonation may be compromised via precipitation of silica or other phases such as amorphous aluminosilicates on the surface of the silicate mineral, forming a passivating layer.
“In addition, the extent of carbonation may be compromised via precipitation of silica (SiO2) or other phases such as amorphous aluminosilicates [5, 6] on the surface of the silicate mineral, forming a passivating layer in between the starting material and the solution [7-9].”
From Mechanochemical formation of highly stable amorphous calcium carbonate in calcium silicates: Potential long-term storage of CO2 in cement (2024) · cites this paper as [5]
The breadth and chemical shifts of additional peaks in 29Si CP NMR are consistent with formation of an amorphous silicate phase.
“The breadth of additional peaks and their chemical shifts are consistent with the formation of an amorphous silicate phase [5, 29, 30].”
From Mechanochemical formation of highly stable amorphous calcium carbonate in calcium silicates: Potential long-term storage of CO2 in cement (2024) · cites this paper as [5]
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The Fumed Silica Surface: A Study by NMR
Liu, C. C., & Maciel, G. E. (1996) · Journal of the American Chemical Society · doi:10.1021/ja954120w · Cited by 303 · see citing works
Characterization of hydrous species in minerals by high-speed proton MAS-NMR
Yesinowski, J. P., Eckert, H., & Rossman, G. R. (1988) · Journal of the American Chemical Society · doi:10.1021/ja00213a007 · Cited by 200 · see citing works
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Vaughn, J. S., Marple, M. A. T., & Mason, H. E. (2024) · Cement and Concrete Research · doi:10.1016/j.cemconres.2023.107413 · Cited by 18 · see citing works
Self-citation
- Authors
- Mason, H. E., Du Frane, W. L., Walsh, S. D. C., Dai, Z., Charnvanichborikarn, S., & Carroll, S. A.
- Affiliations
- Lawrence Livermore National Laboratory (US)
- Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, 7000 East Ave., Livermore, California 94551, United States
- Corresponding author
- Mason, Harris E.
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2013-01-11
- Volume
- 47
- Issue
- 3
- Pages
- 1745-1752
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2333732274
- Cited by
- 128
- References
- 2
- Citations by year
- 2026: 12 · 2025: 13 · 2024: 16 · 2023: 5 · 2022: 4 · 2021: 10 · 2020: 8 · 2019: 7 · 2018: 9 · 2017: 8 · 2016: 10 · 2015: 14 · 2014: 9 · 2013: 3
- FWCI
- 9.95
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- PubMed (publishedVersion)
- Funders
- U.S. Department of Energy
- Lawrence Livermore National Laboratory
- Topics
- Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
- Physical Sciences › Engineering › Ocean Engineering › Drilling and Well Engineering
- Physical Sciences › Engineering › Civil and Structural Engineering › Concrete and Cement Materials Research
- Keywords
- wellbore cement, CO2-rich brine, CO2 geological storage, portlandite dissolution, zeolite synthesis, calcium carbonate precipitation, carbonate dissolution, Young's modulus, elastic properties, pore space, flow-through experiments
- MeSH terms
- Carbon, Carbon Dioxide, Construction Materials, Hydrogen-Ion Concentration, Microscopy, Electron, Scanning, Magnetic Resonance Spectroscopy, Powders, Salts, Solutions, X-Ray Diffraction, Nanotechnology, Mechanical Phenomena
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