Cited by 44CO2 Sequestration and Geologic InteractionsSubcritical and Supercritical Water ProcessesCalcium Carbonate Crystallization and Inhibition

Impacts of Organic Ligands on Forsterite Reactivity in Supercritical CO2 Fluids

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Miller, Quin R. S., Kaszuba, John P., Schaef, Herbert T., Bowden, Mark E., McGrail, Bernard P.·2015·Environmental Science & Technology

Abstract

Subsurface injection of CO2 for enhanced hydrocarbon recovery, hydraulic fracturing of unconventional reservoirs, and geologic carbon sequestration produces a complex geochemical setting in which CO2-dominated fluids containing dissolved water and organic compounds interact with rocks and minerals. The details of these reactions are relatively unknown and benefit from additional experimentally derived data. In this study, we utilized an in situ X-ray diffraction technique to examine the carbonation reactions of forsterite (Mg2SiO4) during exposure to supercritical CO2 (scCO2) that had been equilibrated with aqueous solutions of acetate, oxalate, malonate, or citrate at 50 °C and 90 bar. The organics affected the relative abundances of the crystalline reaction products, nesquehonite (MgCO3 · 3H2O) and magnesite (MgCO3), likely due to enhanced dehydration of the Mg(2+) cations by the organic ligands. These results also indicate that the scCO2 solvated and transported the organic ligands to the forsterite surface. This phenomenon has profound implications for mineral transformations and mass transfer in the upper crust.

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Authors
Miller, Q. R. S., Kaszuba, J. P., Schaef, H. T., Bowden, M. E., & McGrail, B. P.
Affiliations
  • University of Wyoming (US)
  • Pacific Northwest National Laboratory (US)
Corresponding author
Miller, Quin R. S.
Venue
Environmental Science & Technology
Published
2015-03-25
Volume
49
Issue
7
Pages
4724-4734
ISSN
  • 0013-936X (ISSN-L)
  • 1520-5851
OpenAlex
W2034630914
Cited by
44
References
111
Citations by year
2026: 3 · 2025: 11 · 2024: 4 · 2023: 3 · 2022: 4 · 2021: 1 · 2020: 3 · 2019: 5 · 2018: 6 · 2017: 2 · 2016: 1 · 2014: 1
FWCI
2.16
Type
journal article
Language
en
Open access
Locations
  • Environmental Science & Technology (publishedVersion)
  • PubMed (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders
  • School of Energy Resources, University of Wyoming
  • American Chemical Society Petroleum Research Fund
  • University of Wyoming
  • Office of Fossil Energy
Topics
  • Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
  • Physical Sciences › Engineering › Biomedical Engineering › Subcritical and Supercritical Water Processes
  • Physical Sciences › Materials Science › Biomaterials › Calcium Carbonate Crystallization and Inhibition
Keywords
forsterite, supercritical carbon dioxide, organic ligands, CO2 mineralization, nesquehonite, magnesite, acetate, oxalate, malonate, citrate, CO2 sequestration, enhanced hydrocarbon recovery, hydraulic fracturing, mineral dehydration, ligand solvation, mineral transformation, mass transfer
MeSH terms
Carbon Dioxide, Carbonates, Ligands, Magnesium, Minerals, Water, X-Ray Diffraction, Silicon Compounds, Carbon Sequestration

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