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Title: Low-Dimensional Network Formation in Molten Sodium Carbonate

Abstract

Molten carbonates are highly inviscid liquids characterized by low melting points and high solubility of rare earth elements and volatile molecules. An understanding of the structure and related properties of these intriguing liquids has been limited to date. We report the results of a study of molten sodium carbonate (Na2CO3) which combines high energy X-ray diffraction, containerless techniques and computer simulation to provide insight into the liquid structure. Total structure factors (F-x(Q)) are collected on the laser-heated carbonate spheres suspended in flowing gases of varying composition in an aerodynamic levitation furnace. The respective partial structure factor contributions to Fx(Q) are obtained by performing molecular dynamics simulations treating the carbonate anions as flexible entities. The carbonate liquid structure is found to be heavily temperature-dependent. At low temperatures a low-dimensional carbonate chain network forms, at T = 1100 K for example similar to 55% of the C atoms form part of a chain. The mean chain lengths decrease as temperature is increased and as the chains become shorter the rotation of the carbonate anions becomes more rapid enhancing the diffusion of Na+ ions.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Argonne National Laboratory - Advanced Photon Source; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1391802
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

Citation Formats

Wilding, Martin C., Wilson, Mark, Alderman, Oliver L. G., Benmore, Chris, Weber, J. K. R., Parise, John B., Tamalonis, Anthony, and Skinner, Lawrie. Low-Dimensional Network Formation in Molten Sodium Carbonate. United States: N. p., 2016. Web. doi:10.1038/srep24415.
Wilding, Martin C., Wilson, Mark, Alderman, Oliver L. G., Benmore, Chris, Weber, J. K. R., Parise, John B., Tamalonis, Anthony, & Skinner, Lawrie. Low-Dimensional Network Formation in Molten Sodium Carbonate. United States. doi:10.1038/srep24415.
Wilding, Martin C., Wilson, Mark, Alderman, Oliver L. G., Benmore, Chris, Weber, J. K. R., Parise, John B., Tamalonis, Anthony, and Skinner, Lawrie. Fri . "Low-Dimensional Network Formation in Molten Sodium Carbonate". United States. doi:10.1038/srep24415.
@article{osti_1391802,
title = {Low-Dimensional Network Formation in Molten Sodium Carbonate},
author = {Wilding, Martin C. and Wilson, Mark and Alderman, Oliver L. G. and Benmore, Chris and Weber, J. K. R. and Parise, John B. and Tamalonis, Anthony and Skinner, Lawrie},
abstractNote = {Molten carbonates are highly inviscid liquids characterized by low melting points and high solubility of rare earth elements and volatile molecules. An understanding of the structure and related properties of these intriguing liquids has been limited to date. We report the results of a study of molten sodium carbonate (Na2CO3) which combines high energy X-ray diffraction, containerless techniques and computer simulation to provide insight into the liquid structure. Total structure factors (F-x(Q)) are collected on the laser-heated carbonate spheres suspended in flowing gases of varying composition in an aerodynamic levitation furnace. The respective partial structure factor contributions to Fx(Q) are obtained by performing molecular dynamics simulations treating the carbonate anions as flexible entities. The carbonate liquid structure is found to be heavily temperature-dependent. At low temperatures a low-dimensional carbonate chain network forms, at T = 1100 K for example similar to 55% of the C atoms form part of a chain. The mean chain lengths decrease as temperature is increased and as the chains become shorter the rotation of the carbonate anions becomes more rapid enhancing the diffusion of Na+ ions.},
doi = {10.1038/srep24415},
journal = {Scientific Reports},
issn = {2045-2322},
number = 1,
volume = 6,
place = {United States},
year = {2016},
month = {4}
}

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