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Title: Formation of Submicron Magnesite during Reaction of Natural Forsterite in H2O-Saturated Supercritical CO2

Abstract

Natural forsterite was reacted in a) liquid water saturated with supercritical CO2 (scCO2) and in b) H2O-saturated scCO2 at 35-80 °C and 90 atm. The solid reaction products were analyzed with nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), and confocal Raman spectroscopy. Two carbonate phases, nesquehonite (MgCO3.3H2O) and magnesite (MgCO3), were identified with the proportions of the two phases depending on experimental conditions. In water saturated with scCO2, nesquehonite was the dominant carbonate phase at 35-80 °C with only a limited number of large, micron size magnesite particles forming at the highest temperature, 80 °C. In contrast, in H2O-saturated scCO2 magnesite formation was identified at all three temperatures: 35 °, 50 °, and 80 °C. Magnesite was the dominant carbonation reaction product at 50 ° and 80 °C; but nesquehonite was dominant at 35 °C. The magnesite particles formed under H2O-saturated scCO2 conditions exhibited an extremely uniform submicron grain-size and nearly identical rhombohedral morphologies at all temperatures. The distribution and form of the particles were not consistent with epitaxial nucleation and growth on the forsterite surface.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1130653
Report Number(s):
PNNL-SA-93839
37193; KC0302060
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Geochimica et Cosmochimica Acta, 134:197-209
Additional Journal Information:
Journal Name: Geochimica et Cosmochimica Acta, 134:197-209
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Qafoku, Odeta, Hu, Jian Z., Hess, Nancy J., Hu, Mary Y., Ilton, Eugene S., Feng, Ju, Arey, Bruce W., and Felmy, Andrew R. Formation of Submicron Magnesite during Reaction of Natural Forsterite in H2O-Saturated Supercritical CO2. United States: N. p., 2014. Web. doi:10.1016/j.gca.2013.09.024.
Qafoku, Odeta, Hu, Jian Z., Hess, Nancy J., Hu, Mary Y., Ilton, Eugene S., Feng, Ju, Arey, Bruce W., & Felmy, Andrew R. Formation of Submicron Magnesite during Reaction of Natural Forsterite in H2O-Saturated Supercritical CO2. United States. https://doi.org/10.1016/j.gca.2013.09.024
Qafoku, Odeta, Hu, Jian Z., Hess, Nancy J., Hu, Mary Y., Ilton, Eugene S., Feng, Ju, Arey, Bruce W., and Felmy, Andrew R. Sun . "Formation of Submicron Magnesite during Reaction of Natural Forsterite in H2O-Saturated Supercritical CO2". United States. https://doi.org/10.1016/j.gca.2013.09.024.
@article{osti_1130653,
title = {Formation of Submicron Magnesite during Reaction of Natural Forsterite in H2O-Saturated Supercritical CO2},
author = {Qafoku, Odeta and Hu, Jian Z. and Hess, Nancy J. and Hu, Mary Y. and Ilton, Eugene S. and Feng, Ju and Arey, Bruce W. and Felmy, Andrew R.},
abstractNote = {Natural forsterite was reacted in a) liquid water saturated with supercritical CO2 (scCO2) and in b) H2O-saturated scCO2 at 35-80 °C and 90 atm. The solid reaction products were analyzed with nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), and confocal Raman spectroscopy. Two carbonate phases, nesquehonite (MgCO3.3H2O) and magnesite (MgCO3), were identified with the proportions of the two phases depending on experimental conditions. In water saturated with scCO2, nesquehonite was the dominant carbonate phase at 35-80 °C with only a limited number of large, micron size magnesite particles forming at the highest temperature, 80 °C. In contrast, in H2O-saturated scCO2 magnesite formation was identified at all three temperatures: 35 °, 50 °, and 80 °C. Magnesite was the dominant carbonation reaction product at 50 ° and 80 °C; but nesquehonite was dominant at 35 °C. The magnesite particles formed under H2O-saturated scCO2 conditions exhibited an extremely uniform submicron grain-size and nearly identical rhombohedral morphologies at all temperatures. The distribution and form of the particles were not consistent with epitaxial nucleation and growth on the forsterite surface.},
doi = {10.1016/j.gca.2013.09.024},
url = {https://www.osti.gov/biblio/1130653}, journal = {Geochimica et Cosmochimica Acta, 134:197-209},
number = ,
volume = ,
place = {United States},
year = {2014},
month = {6}
}