The glasses of the system Na
2O-B
2O
3-SiO
2, with or without the addition of Al
2O
3, were melted in a platinum crusible using refined silica and chemical reagents.
The quenched glasses were subjected to the repeated heating at a constant temperature in the range of 350°-633°C, and the densities were measured by sink float method. The change of density was analysed in conformity to the theory advanced by the author (
J. Ceram. Assoc. Japan,
66, 117, (1958).
The change of density
ΔD may be expressed by an equation
ΔD=Σ
pie-t/φi=
pe-t/φ4+
qe-t/φ3+
re-t/φ2+
se-t/φ1+……, where
t is the time, φ the relaxation time containing a certain activation energy, and increase with decreasing temperature.
pe-t/φ4,
qe-t/φ3 represent the decrease of density.
The author assumed that both termes represent the density change due, respectively, to the growth of the phase separated out by heating at an elevated temperature, and to the separation at lower temperatures.
re-t/φ2 was considered as the density increase due to the compacting of quenched glass brought about by the recombination of atoms in the comparatively open stracture.
The activation energies in φ
4, φ
3, φ
2, are of the order of 80kcal/mol, and
se-t/φ1 is regarded as the primary cause of the density increase at the temperatures considerably lower than the transformation region. It has low activation energy.
In the same way as given in a previous paper (
J. Ceram. Assoc. Japan, 61, 178, (1959)) it was possible to elusidate the above characteristic properties of density change by introducing the reaction model composed of the energy levels,
L1,
L2,
L3,
L4, which is corresponding, respectively, to the quenched state, compacted state, and those of separation at comparatively lower and higher temperatures, and assuming that
Li is composed of two closely adjoined energy levels
li1 and
li2.
Furthermore, the opalisation and the surface devitrification of the same glass were studied with some results on the relation between the separation and the characteristic features of phase diagrams.
As far as the composition range of present paper is concerned the borosilicate glasses did not show any trend of progress from separation to crystallization, except on the surface layer.
Moreover, the measurement of thermal expansion and of density change have revealed that the addition of Al
2O
3 checks the excessive development of the size of separated phase.
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