The Role of Interfacial Water on Mineral Transformations in Wet Supercritical CO2
EMSL Project ID
47824
Abstract
We propose a comprehensive experimental and theoretical investigation of the molecular mechanisms governing the role of interfacial water in the reactivity of mineral phases in supercritical carbon dioxide. In order to achieve these objectives were propose to examine the molecular mechanisms of interfacial water reactivity at both the mineral-water interface and the water-supercritical CO2 (scCO2) interface, as well as in the associated aqueous solutions. Reactions at the mineral-water interface will be probed both at the surface of reacting mineral phases, e.g. orthosilicates, as well as in the interlayer region of hydrous phyllosilicates. Reactions at the both the surface of orthosilicates and in the interlayer region of phyllosilicates will be probed using new in situ high resolutions IR/FTIR and NMR spectroscopy as well as new in situ X-Ray diffraction methods. In addition, reactions at the orthosilicate surface will be probed by new atom probe tomography (APT) and in situ atomic force microscopy (AFM). Changes in the structure of the water-supercritical CO2 (scCO2) interface will also be probed using new sum frequency generation capabilities being developed in the EMSL. These experimental studies will be coupled with theoretical investigations of the binding of water and CO2 to both the orthosilicate surface and interlayer of phyllosilicates as well as complexation reactions in the associated aqueous solutions. The proposed research will provide new insights into mineral transformations under extreme conditions of high CO2 partial pressures including geologic conditions associated with the sequestration of atmospheric CO2.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2015-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
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Qafoku O, ES Ilton, ME Bowden, L Kovarik, X Zhang, RK Kukkadapu, MH Engelhard, CJ Thompson, HT Schaef, BP McGrail, KM Rosso, and JS Loring. 2018. "Synthesis of Nanometer-Sized Fayalite and Magnesium-Iron(II) Mixture Olivines." Journal of Colloid and Interface Science 515:129-138. doi:10.1016/j.jcis.2018.01.036
Direction-specific interaction forces underlying zinc oxide crystal growth by oriented attachment
Zhang X, Z Shen, J Liu, SN Kerisit, ME Bowden, ML Sushko, JJ De Yoreo, and KM Rosso. 2017. "Direction-Specific Interaction Forces Underlying ZnO Crystal Growth by Oriented Attachment." Nature Communications 8:835. doi:10.1038/s41467-017-00844-6
Electron Mobility and Trapping in Ferrihydrite Nanoparticles
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Hu MY, X Deng, S Thanthiriwatte, VE Jackson, C Wan, O Qafoku, DA Dixon, AR Felmy, KM Rosso, and JZ Hu. 2016. "In Situ Natural Abundance 17O and 25Mg NMR Investigation of Aqueous Mg(OH)2 Dissolution in the Presence of Supercritical CO2." Environmental Science & Technology 50(22):12373-12384. doi:10.1021/acs.est.6b03443
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