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Title: Structure and Liquid Fragility in Sodium Carbonate

In this paper, the relationship between local structure and dynamics is explored for molten sodium carbonate. A flexible fluctuating-charge model, which allows for changes in the shape and charge distribution of the carbonate molecular anion, is developed. The system shows the evolution of highly temperature-dependent complex low-dimensional structures which control the dynamics (and hence the liquid fragility). By varying the molecular anion charge distribution, the key interactions responsible for the formation of these structures can be identified and rationalized. Finally, an increase in the mean charge separation within the carbonate ions increases the connectivity of the emerging structures and leads to an increase in the system fragility.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ;  [4] ;  [5] ;  [5] ;  [6] ;  [7]
  1. Univ. of Oxford (United Kingdom). Dept. of Chemistry. Physical and Theoretical Chemistry Lab.
  2. Univ. of São Paulo (Brazil). Lab. of Molecular Spectroscopy. Inst. of Chemistry
  3. Univ. College London (United Kingdom). Dept. of Chemistry
  4. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  5. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division; Materials Development Inc., Arlington Heights, IL (United States)
  6. Materials Development Inc., Arlington Heights, IL (United States)
  7. Stony Brook Univ., NY (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357; SC0015241; EP/L015722/1
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 122; Journal Issue: 4; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States); Materials Development Inc., Arlington Heights, IL (United States); Univ. of Oxford (United Kingdom)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Engineering and Physical Sciences Research Council (EPSRC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1461315

Wilson, Mark, Ribeiro, Mauro C. C., Wilding, Martin C., Benmore, Chris, Weber, J. K. R., Alderman, Oliver, Tamalonis, Anthony, and Parise, J. B.. Structure and Liquid Fragility in Sodium Carbonate. United States: N. p., Web. doi:10.1021/acs.jpca.7b10712.
Wilson, Mark, Ribeiro, Mauro C. C., Wilding, Martin C., Benmore, Chris, Weber, J. K. R., Alderman, Oliver, Tamalonis, Anthony, & Parise, J. B.. Structure and Liquid Fragility in Sodium Carbonate. United States. doi:10.1021/acs.jpca.7b10712.
Wilson, Mark, Ribeiro, Mauro C. C., Wilding, Martin C., Benmore, Chris, Weber, J. K. R., Alderman, Oliver, Tamalonis, Anthony, and Parise, J. B.. 2017. "Structure and Liquid Fragility in Sodium Carbonate". United States. doi:10.1021/acs.jpca.7b10712. https://www.osti.gov/servlets/purl/1461315.
@article{osti_1461315,
title = {Structure and Liquid Fragility in Sodium Carbonate},
author = {Wilson, Mark and Ribeiro, Mauro C. C. and Wilding, Martin C. and Benmore, Chris and Weber, J. K. R. and Alderman, Oliver and Tamalonis, Anthony and Parise, J. B.},
abstractNote = {In this paper, the relationship between local structure and dynamics is explored for molten sodium carbonate. A flexible fluctuating-charge model, which allows for changes in the shape and charge distribution of the carbonate molecular anion, is developed. The system shows the evolution of highly temperature-dependent complex low-dimensional structures which control the dynamics (and hence the liquid fragility). By varying the molecular anion charge distribution, the key interactions responsible for the formation of these structures can be identified and rationalized. Finally, an increase in the mean charge separation within the carbonate ions increases the connectivity of the emerging structures and leads to an increase in the system fragility.},
doi = {10.1021/acs.jpca.7b10712},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 4,
volume = 122,
place = {United States},
year = {2017},
month = {12}
}