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The configurational heat capacity, shear modulus and shear viscosity of a series of Na2O–Fe2O3–Al2O3–SiO2 melts have been determined as a function of composition. A change in composition dependence of each of the physical properties
is observed as Na2O/(Na2O + Al2O3) is decreased, and the peralkaline melts become peraluminous and a new charge-balanced Al-structure appears in the melts.
Of special interest are the frequency dependent (1 mHz–1 Hz) measurements of the shear modulus. These forced oscillation measurements
determine the lifetimes of Si–O bonds and Na–O bonds in the melt. The lifetime of the Al–O bonds could not, however, be resolved
from the mechanical spectrum. Therefore, it appears that the lifetime of Al–O bonds in these melts is similar to that of Si–O
bonds with the Al–O relaxation peak being subsumed by the Si–O relaxation peak. The appearance of a new Al-structure in the
peraluminous melts also cannot be resolved from the mechanical spectra, although a change in elastic shear modulus is determined
as a function of composition. The structural shear-relaxation time of some of these melts is not that which is predicted by
the Maxwell equation, but up to 1.5 orders of magnitude faster. Although the configurational heat capacity, density and shear
modulus of the melts show a change in trend as a function of composition at the boundary between peralkaline and peraluminous,
the deviation in relaxation time from the Maxwell equation occurs in the peralkaline regime. The measured relaxation times
for both the very peralkaline melts and the peraluminous melts are identical with the calculated Maxwell relaxation time.
As the Maxwell equation was created to describe the timescale of flow of a mono-structure material, a deviation from the prediction
would indicate that the structure of the melt is too complex to be described by this simple flow equation. One possibility
is that Al-rich channels form and then disappear with decreasing Si/Al, and that the flow is dominated by the lifetime of
Si–O bonds in the Al-poor peralkaline melts, and by the lifetime of Al–O bonds in the relatively Si-poor peralkaline and peraluminous
melts with a complex flow mechanism occurring in the mid-compositions. This anomalous deviation from the calculated relaxation
time appears to be independent of the change in structure expected to occur at the peralkaline/peraluminous boundary due to
the lack of charge-balancing cations for the Al-tetrahedra. 相似文献