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Title: Enhancing Magnesite Formation at Low Temperature and High CO2 Pressure: The Impact of Seed Crystals and Minor Components

Abstract

The formation of magnesite was followed in aqueous solution containing initially added Mg(OH)2 equilibrated with supercritical carbon dioxide (90 atm pressure, 50°C) in the presence of introduced magnesite particles and minor components, Co(II). As expected, the introduction of magnesite particles accelerated the formation of magnesite from solution. However, the formation rate of magnesite was even greater when small concentrations of Co(II) were introduced, indicating that the increased rate of magnesite formation in the presence of Co(II) was not solely due to the addition of a growth promoting surface. Detailed analysis of the magnesite particles by scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), and atom probe tomography (APT) revealed that the originally added Co(II) was concentrated in the center but also present throughout the growing magnesite particles. Addition of the Co(II) in different chemical forms (i.e. as solid phase CoCO3 or Co(OH)2) could alter the growth rate of magnesite depending upon the addition of bicarbonate to the starting solution. Geochemical modeling calculations indicate that this difference is related to the thermodynamic stability of these different phases in the initial solutions. More broadly, these results indicate that the presence of even small concentrations of foreign ions thatmore » form carbonate compounds with a similar structure as magnesite can be incorporated into the magnesite lattice, accelerating the formation of anhydrous carbonates in natural environments.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1184912
Report Number(s):
PNNL-SA-107559
47824; KC0302060
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Chemical Geology, 395:119-125
Additional Journal Information:
Journal Name: Chemical Geology, 395:119-125
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Felmy, Andrew R., Qafoku, Odeta, Arey, Bruce W., Kovarik, Libor, Liu, Jia, Perea, Daniel E., and Ilton, Eugene S. Enhancing Magnesite Formation at Low Temperature and High CO2 Pressure: The Impact of Seed Crystals and Minor Components. United States: N. p., 2015. Web. doi:10.1016/j.chemgeo.2014.12.003.
Felmy, Andrew R., Qafoku, Odeta, Arey, Bruce W., Kovarik, Libor, Liu, Jia, Perea, Daniel E., & Ilton, Eugene S. Enhancing Magnesite Formation at Low Temperature and High CO2 Pressure: The Impact of Seed Crystals and Minor Components. United States. https://doi.org/10.1016/j.chemgeo.2014.12.003
Felmy, Andrew R., Qafoku, Odeta, Arey, Bruce W., Kovarik, Libor, Liu, Jia, Perea, Daniel E., and Ilton, Eugene S. 2015. "Enhancing Magnesite Formation at Low Temperature and High CO2 Pressure: The Impact of Seed Crystals and Minor Components". United States. https://doi.org/10.1016/j.chemgeo.2014.12.003.
@article{osti_1184912,
title = {Enhancing Magnesite Formation at Low Temperature and High CO2 Pressure: The Impact of Seed Crystals and Minor Components},
author = {Felmy, Andrew R. and Qafoku, Odeta and Arey, Bruce W. and Kovarik, Libor and Liu, Jia and Perea, Daniel E. and Ilton, Eugene S.},
abstractNote = {The formation of magnesite was followed in aqueous solution containing initially added Mg(OH)2 equilibrated with supercritical carbon dioxide (90 atm pressure, 50°C) in the presence of introduced magnesite particles and minor components, Co(II). As expected, the introduction of magnesite particles accelerated the formation of magnesite from solution. However, the formation rate of magnesite was even greater when small concentrations of Co(II) were introduced, indicating that the increased rate of magnesite formation in the presence of Co(II) was not solely due to the addition of a growth promoting surface. Detailed analysis of the magnesite particles by scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), and atom probe tomography (APT) revealed that the originally added Co(II) was concentrated in the center but also present throughout the growing magnesite particles. Addition of the Co(II) in different chemical forms (i.e. as solid phase CoCO3 or Co(OH)2) could alter the growth rate of magnesite depending upon the addition of bicarbonate to the starting solution. Geochemical modeling calculations indicate that this difference is related to the thermodynamic stability of these different phases in the initial solutions. More broadly, these results indicate that the presence of even small concentrations of foreign ions that form carbonate compounds with a similar structure as magnesite can be incorporated into the magnesite lattice, accelerating the formation of anhydrous carbonates in natural environments.},
doi = {10.1016/j.chemgeo.2014.12.003},
url = {https://www.osti.gov/biblio/1184912}, journal = {Chemical Geology, 395:119-125},
number = ,
volume = ,
place = {United States},
year = {Tue Feb 24 00:00:00 EST 2015},
month = {Tue Feb 24 00:00:00 EST 2015}
}