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Title: In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO 3 and Quartz Substrates: Thermodynamics of CO 2 Mineral Trapping

Abstract

The precipitation of carbonate minerals—mineral trapping—is considered one of the safest sequestration mechanisms ensuring long-term geologic storage of CO{sub 2}. However, little is known about the thermodynamic factors controlling the extent of heterogeneous nucleation at mineral surfaces exposed to the fluids in porous reservoirs. The goal of this study is to determine the thermodynamic factors controlling heterogeneous nucleation of carbonate minerals on pristine quartz (100) surfaces, which are assumed representative of sandstone reservoirs. To probe CaCO{sub 3} nucleation on quartz (100) in solution and with nanoscale resolution, an in situ grazing incidence small-angle X-ray scattering technique has been utilized. With this method, a value of α = 36 ± 5 mJ/m{sup 2} for the effective interfacial free energy governing heterogeneous nucleation of CaCO{sub 3} has been obtained by measuring nucleation rates at different solution supersaturations. This value is lower than the interfacial energy governing calcite homogeneous nucleation (α ≈ 120 mJ/m{sup 2}), suggesting that heterogeneous nucleation of calcium carbonate is favored on quartz (100) at ambient pressure and temperature conditions, with nucleation barriers between 2.5% and 15% lower than those expected for homogeneous nucleation. These observations yield important quantitative parameters readily usable in reactive transport models of nucleation at themore » reservoir scale.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC); Center for Nanoscale Control of Geologic CO2 (NCGC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1080659
DOE Contract Number:  
AC02–05CH11231
Resource Type:
Journal Article
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 47; Journal Issue: 1; Related Information: NCGC partners with Lawrence Berkeley National Laboratory (lead); University of California, Davis; Lawrence Livermore National Laboratory; Massachusetts Institute of Technology; Ohio State University; Oak Ridge National Laboratory; Washington University, St. Louis; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; bio-inspired, mechanical behavior, carbon sequestration

Citation Formats

Fernandez-Martinez, Alejandro, Hu, Yandi, Lee, Byeongdu, Jun, Young-Shin, and Waychunas, Glenn A. In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO 3 and Quartz Substrates: Thermodynamics of CO 2 Mineral Trapping. United States: N. p., 2013. Web. doi:10.1021/es3014826.
Fernandez-Martinez, Alejandro, Hu, Yandi, Lee, Byeongdu, Jun, Young-Shin, & Waychunas, Glenn A. In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO 3 and Quartz Substrates: Thermodynamics of CO 2 Mineral Trapping. United States. https://doi.org/10.1021/es3014826
Fernandez-Martinez, Alejandro, Hu, Yandi, Lee, Byeongdu, Jun, Young-Shin, and Waychunas, Glenn A. Wed . "In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO 3 and Quartz Substrates: Thermodynamics of CO 2 Mineral Trapping". United States. https://doi.org/10.1021/es3014826.
@article{osti_1080659,
title = {In Situ Determination of Interfacial Energies between Heterogeneously Nucleated CaCO 3 and Quartz Substrates: Thermodynamics of CO 2 Mineral Trapping},
author = {Fernandez-Martinez, Alejandro and Hu, Yandi and Lee, Byeongdu and Jun, Young-Shin and Waychunas, Glenn A.},
abstractNote = {The precipitation of carbonate minerals—mineral trapping—is considered one of the safest sequestration mechanisms ensuring long-term geologic storage of CO{sub 2}. However, little is known about the thermodynamic factors controlling the extent of heterogeneous nucleation at mineral surfaces exposed to the fluids in porous reservoirs. The goal of this study is to determine the thermodynamic factors controlling heterogeneous nucleation of carbonate minerals on pristine quartz (100) surfaces, which are assumed representative of sandstone reservoirs. To probe CaCO{sub 3} nucleation on quartz (100) in solution and with nanoscale resolution, an in situ grazing incidence small-angle X-ray scattering technique has been utilized. With this method, a value of α = 36 ± 5 mJ/m{sup 2} for the effective interfacial free energy governing heterogeneous nucleation of CaCO{sub 3} has been obtained by measuring nucleation rates at different solution supersaturations. This value is lower than the interfacial energy governing calcite homogeneous nucleation (α ≈ 120 mJ/m{sup 2}), suggesting that heterogeneous nucleation of calcium carbonate is favored on quartz (100) at ambient pressure and temperature conditions, with nucleation barriers between 2.5% and 15% lower than those expected for homogeneous nucleation. These observations yield important quantitative parameters readily usable in reactive transport models of nucleation at the reservoir scale.},
doi = {10.1021/es3014826},
url = {https://www.osti.gov/biblio/1080659}, journal = {Environmental Science and Technology},
issn = {0013-936X},
number = 1,
volume = 47,
place = {United States},
year = {2013},
month = {1}
}