Universität zu Köln

Liu, Maoyuan, Jacob, Aurelie ORCID: 0000-0001-8447-4438, Schmetterer, Clemens, Masset, Patrick J., Hennet, Louis, Fischer, Henry E., Kozaily, Jad, Jahn, Sandro ORCID: 0000-0002-2137-8833 and Gray-Weale, Angus (2016). From atomic structure to excess entropy: a neutron diffraction and density functional theory study of CaO-Al2O3-SiO2 melts. J. Phys.-Condes. Matter, 28 (13). BRISTOL: IOP PUBLISHING LTD. ISSN 1361-648X

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Abstract

Calcium aluminosilicate CaO-Al2O3-SiO2 (CAS) melts with compositions (CaO - SiO2)(x)(Al2O3)(1-x) for x < 0.5 and (Al2O3)(x)(SiO2)(1-x) for x >= 0.5 are studied using neutron diffraction with aerodynamic levitation and density functional theory molecular dynamics modelling. Simulated structure factors are found to be in good agreement with experimental structure factors. Local atomic structures from simulations reveal the role of calcium cations as a network modifier, and aluminium cations as a non-tetrahedral network former. Distributions of tetrahedral order show that an increasing concentration of the network former Al increases entropy, while an increasing concentration of the network modifier Ca decreases entropy. This trend is opposite to the conventional understanding that increasing amounts of network former should increase order in the network liquid, and so decrease entropy. The two-body correlation entropy S-2 is found to not correlate with the excess entropy values obtained from thermochemical databases, while entropies including higher-order correlations such as tetrahedral order, O-M-O or M-O-M bond angles and Q(N) environments show a clear linear correlation between computed entropy and database excess entropy. The possible relationship between atomic structures and excess entropy is discussed.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Liu, Maoyuan UNSPECIFIED UNSPECIFIED UNSPECIFIED Jacob, Aurelie UNSPECIFIED orcid.org/0000-0001-8447-4438 UNSPECIFIED Schmetterer, Clemens UNSPECIFIED UNSPECIFIED UNSPECIFIED Masset, Patrick J. UNSPECIFIED UNSPECIFIED UNSPECIFIED Hennet, Louis UNSPECIFIED UNSPECIFIED UNSPECIFIED Fischer, Henry E. UNSPECIFIED UNSPECIFIED UNSPECIFIED Kozaily, Jad UNSPECIFIED UNSPECIFIED UNSPECIFIED Jahn, Sandro UNSPECIFIED orcid.org/0000-0002-2137-8833 UNSPECIFIED Gray-Weale, Angus UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-278838
DOI:	10.1088/0953-8984/28/13/135102
Journal or Publication Title:	J. Phys.-Condes. Matter
Volume:	28
Number:	13
Date:	2016
Publisher:	IOP PUBLISHING LTD
Place of Publication:	BRISTOL
ISSN:	1361-648X
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language INITIO MOLECULAR-DYNAMICS; RADIAL-DISTRIBUTION FUNCTIONS; INTERMEDIATE-RANGE ORDER; INTERIONIC POTENTIALS; SILICATE MELTS; SIMULATIONS; LIQUIDS; SCATTERING; GLASSES; SPECTRA Multiple languages Physics, Condensed Matter Multiple languages
Refereed:	Yes
URI:	http://kups.ub.uni-koeln.de/id/eprint/27883