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@ARTICLE{Liu:808668,
author = {Liu, Maoyuan and Jacob, Aurélie and Schmetterer, Clemens
and Masset, Patrick J and Hennet, Louis and Fischer, Henry E
and Kozaily, Jad and Jahn, Sandro and Gray-Weale, Angus},
title = {{F}rom {A}tomic {S}tructure to {E}xcess {E}ntropy: {A}
{N}eutron {D}iffraction and {D}ensity {F}unctional {T}heory
{S}tudy of {C}a{O}−{A}l$_{2}$ {O}$_{3}$ −{S}i{O}$_{2}$
{M}elts},
journal = {Journal of physics / Condensed matter},
volume = {28},
number = {13},
issn = {1361-648X},
address = {Bristol},
publisher = {IOP Publ.},
reportid = {FZJ-2016-02301},
pages = {135102},
year = {2016},
abstract = {Calcium aluminosilicate
$\text{CaO}-\text{A}{{\text{l}}_{2}}{{\text{O}}_{3}}-\text{Si}{{\text{O}}_{2}}$
(CAS) melts with compositions
${{\left(\text{CaO}-\text{Si}{{\text{O}}_{2}}\right)}_{x}}{{\left(\text{A}{{\text{l}}_{2}}{{\text{O}}_{3}}\right)}_{1-x}}$
for x < 0.5 and
${{\left(\text{A}{{\text{l}}_{2}}{{\text{O}}_{3}}\right)}_{x}}{{\left(\text{Si}{{\text{O}}_{2}}\right)}_{1-x}}$
for $x\geqslant 0.5$ 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.},
cin = {IEK-2},
ddc = {530},
cid = {I:(DE-Juel1)IEK-2-20101013},
pnm = {111 - Efficient and Flexible Power Plants (POF3-111)},
pid = {G:(DE-HGF)POF3-111},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000371905200016},
doi = {10.1088/0953-8984/28/13/135102},
url = {https://juser.fz-juelich.de/record/808668},
}