Structure and Liquid Fragility in Sodium Carbonate

Wilson, Mark; Ribeiro, Mauro C.  C.; Wilding, Martin C.; Benmore, Chris; Weber, J. K.  R.; Alderman, Oliver; Tamalonis, Anthony; Parise, J. B.

doi:10.1021/acs.jpca.7b10712

Title: Structure and Liquid Fragility in Sodium Carbonate

Journal Article · 15 December 2017 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI: https://doi.org/10.1021/acs.jpca.7b10712 · OSTI ID:1461315

^[1];

^[2]; Wilding, Martin C. ^[3]; Benmore, Chris ^[4]; Weber, J. K. R. ^[5]; Alderman, Oliver ^[5]; Tamalonis, Anthony ^[6]; Parise, J. B. ^[7]

Univ. of Oxford (United Kingdom). Dept. of Chemistry. Physical and Theoretical Chemistry Lab.
Univ. of São Paulo (Brazil). Lab. of Molecular Spectroscopy. Inst. of Chemistry
Univ. College London (United Kingdom). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division; Materials Development Inc., Arlington Heights, IL (United States)
Materials Development Inc., Arlington Heights, IL (United States)
Stony Brook Univ., NY (United States)

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Materials Development Inc., Arlington Heights, IL (United States); Univ. of Oxford (United Kingdom)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC02-06CH11357; SC0015241; EP/L015722/1

OSTI ID:: 1461315

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 122, Issue 4; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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