Impacts of Organic Ligands on Forsterite Reactivity in Supercritical CO2 Fluids

Miller, Quin R. S.; Kaszuba, John P.; Schaef, Herbert T.; Bowden, Mark E.; McGrail, Bernard P.

doi:10.1021/es506065d

Title: Impacts of Organic Ligands on Forsterite Reactivity in Supercritical CO₂ Fluids

Journal Article · Wed Mar 25 00:00:00 EDT 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/es506065d· OSTI ID:1208753

Miller, Quin R. S. ^[1]; Kaszuba, John P. ^[1]; Schaef, Herbert T. ^[2]; Bowden, Mark E. ^[2]; McGrail, Bernard P. ^[2]

Univ. of Wyoming, Laramie, WY (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

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 Mg²⁺ cations by the organic ligands. These results also indicate that the scCO₂ solvated and transported the organic ligands to the forsterite surface. Lastly, this phenomenon has profound implications for mineral transformations and mass transfer in the upper crust.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1208753

Report Number(s):: PNNL-SA-109524; 47427; AA7020000

Journal Information:: Environmental Science and Technology, Vol. 49, Issue 7; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Environmental Molecular Sciences Laboratory
Ligands
Dissolution
Inorganic carbon compounds
Minerals
Precipitation

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Title: Impacts of Organic Ligands on Forsterite Reactivity in Supercritical CO₂ Fluids