Hostname: page-component-74656f9884-j7cmm Total loading time: 0 Render date: 2026-11-10T12:54:31.686Z Has data issue: false hasContentIssue false

Solidification of binary aqueous solutions under periodic cooling. Part 1. Dynamics of mushy-layer growth

Published online by Cambridge University Press:  07 May 2019

Guang-Yu Ding
Affiliation:
School of Physics Science and Engineering, Tongji University, Shanghai 200092, China Department of Physics, Chinese University of Hong Kong, Hong Kong, China
Andrew J. Wells
Affiliation:
Department of Physics, University of Oxford, Oxford OX1 3PU, UK
Jin-Qiang Zhong*
Affiliation:
School of Physics Science and Engineering, Tongji University, Shanghai 200092, China
*
†Email address for correspondence: jinqiang@tongji.edu.cn

Abstract

We present studies of the solidification of binary aqueous solutions that undergo time-periodic cooling from below. We develop an experiment for solidification of aqueous $\text{NH}_{4}\text{Cl}$ solutions, where the temperature of the cooling boundary is modulated as a simple periodic function of time with independent variations of the modulation amplitude and frequency. The thickness of the mushy layer exhibits oscillations about the background growth obtained for constant cooling. We consider the deviation given by the difference between states with modulated and fixed cooling, which increases when the modulation amplitude increases but decreases with increasing modulation frequency. At early times, the deviation amplitude is consistent with a scaling argument for growth with quasi-steady modulation. In situ measurements of the mush temperature reveal thermal waves propagating through the mushy layer, with amplitude decaying with height within the mushy layer, whilst the phase lag behind the cooling boundary increases with height. This also leads to phase lags in the variation of the mushy-layer thickness compared to the boundary cooling. There is an asymmetry of the deviation of mushy-layer thickness: during a positive modulation (where the boundary temperature increases at the start of a cycle) the peak thickness deviation has a greater magnitude than the troughs in a negative modulation mode (where the boundary temperature decreases at the start of the cycle). A numerical model is formulated to describe mushy-layer growth with constant bulk concentration and turbulent heat transport at the mush–liquid interface driven by compositional convection associated with a finite interfacial solid fraction. The model recovers key features of the experimental results at early times, including the propagation of thermal waves and oscillations in mushy-layer thickness, although tends to overpredict the mean thickness.

Information

Type
JFM Papers
Copyright
© 2019 Cambridge University Press 
Figure 0

Figure 1. (a) Schematic of the experimental apparatus. A rectangular cell ($80~\text{mm}\times 80~\text{mm}\times 150$  mm) filled with aqueous ammonium chloride solution is cooled from below by an array of Peltier modules and a circulating water bath. A thermal shield regulates the ambient air temperature $T_{air}$ surrounding the cell such that it remains the same as the initial temperature of the solution ($T_{air}\approx T_{0}$). Two optical windows are fabricated on the end walls of the shield for light transmission and hence shadowgraph imaging. (b) Sketch of the Plexiglas probe for the thermistors. The positions of the thermistor leads are shown by black dots.

Figure 1

Figure 2. Illustration of the coordinate transformation method we apply in the numerical calculations. Temperature profiles are sketched as black curves in the real mushy-layer domain (a) and in the non-dimensional domain (b).

Figure 2

Table 1. The parameter values used in the model.

Figure 3

Figure 3. (a) The bottom-plate temperatures $T_{b}(t)$ as a function of time. Results for $A=10~\text{K}$, $\unicode[STIX]{x1D70F}=4000~\text{s}$, $\unicode[STIX]{x1D719}_{0}=0$ (red curve) and $\unicode[STIX]{x1D719}_{0}=\unicode[STIX]{x03C0}$ (blue curve) and for $A=0$ (black curve). (b) The height of the mushy layer as a function of time. The dashed curve shows a fitting to the initial growth in the constant-cooling mode: $h(t)=2\unicode[STIX]{x1D6EC}(Dt)^{1/2}$ with $D$ the solute diffusivity and the coefficient $\unicode[STIX]{x1D6EC}=4.85$. The vertical dashed lines indicate the time at which each modulation period begins. Inset: a shadowgraph image focusing on the mush–liquid interface. The green solid line shows the position of the mush–liquid interface identified by our image processing system. The red dashed line represents the mean height of the mushy layer.

Figure 4

Figure 4. The relative mushy-layer height $\unicode[STIX]{x1D6FF}h=h(t)-h_{0}$ as a function of time for different modulation amplitudes and phases. Results for $\unicode[STIX]{x1D70F}=4000~\text{s}$ and $5.0~\text{K}\leqslant A\leqslant 15.0~\text{K}$. Solid lines: $\unicode[STIX]{x1D719}_{0}=\unicode[STIX]{x03C0}$; dashed lines: $\unicode[STIX]{x1D719}_{0}=0$. Results from (a) the numerical model and (b) the experiment. (c) An expanded view of the experimental data in the region with $1.0\leqslant t/\unicode[STIX]{x1D70F}\leqslant 1.5$.

Figure 5

Figure 5. The relative mushy-layer height $\unicode[STIX]{x1D6FF}h=h(t)-h_{0}$ as a function of time for different modulation periods. Results for $A=7~\text{K}$ and $2000~\text{s}\leqslant \unicode[STIX]{x1D70F}\leqslant 5000~\text{s}$. Solid lines: $\unicode[STIX]{x1D719}_{0}=\unicode[STIX]{x03C0}$; dashed lines: $\unicode[STIX]{x1D719}_{0}=0$. (a) Numerical model and (b) experimental results. (c) An expanded view of the experimental data in the region with $1.0\leqslant t/\unicode[STIX]{x1D70F}\leqslant 1.5$.

Figure 6

Figure 6. (a) The distances $|h^{2}-h_{0}^{2}|$ measured at the first peak (trough) as a function of the modulation amplitude. Results for $\unicode[STIX]{x1D70F}=4000~\text{s}$. The dashed line shows a proportional relation: $|h^{2}-h_{0}^{2}|=8.35A~(\text{mm}^{2}~\text{K}^{-1})$. (b) Distances $|h^{2}-h_{0}^{2}|$ as a function of the modulation frequency for $A=7~\text{K}$. The dashed line indicates a scaling relation: $|h^{2}-h_{0}^{2}|=0.0873\unicode[STIX]{x1D714}^{-1}~(\text{mm}^{2}~\text{s}~\text{rad}^{-1})$. Red squares: $\unicode[STIX]{x1D719}_{0}=0$; blue circles: $\unicode[STIX]{x1D719}_{0}=\unicode[STIX]{x03C0}$.

Figure 7

Figure 7. The fluid temperature as a function of time at various heights measured in the first modulation period. The coloration represents the heights as indicated by the upper colour bar. The dashed curve shows the position of the mush–liquid interface and above that the liquid region is indicated in shadow colour. The orange curve shows the variation of the bottom temperature $T_{b}(t)$. The minima of $T(z,t)$ in the first modulation period and the maxima in the second modulation period are marked by the blue and red circles, respectively. Experimental results for $A=10~\text{K}$, $\unicode[STIX]{x1D70F}=4000~\text{s}$ and $\unicode[STIX]{x1D719}_{0}=0$.

Figure 8

Figure 8. Numerical results for the fluid temperature distribution as a function of time within the mushy layer. The height is indicated by the colour scale. Results for $A=10~\text{K}$, $\unicode[STIX]{x1D70F}=4000~\text{s}$ and $\unicode[STIX]{x1D719}_{0}=0$. The minima of $T(z,t)$ in the first modulation period and the maxima in the second modulation period are marked by the blue and red circles, respectively. The orange curve shows the variation of the bottom temperature $T_{b}(t)$.

Figure 9

Figure 9. Properties of oscillations of the temperature $T(z,t)$ as a function of height. (a) The phase lags of the minima of $T(z,t)$ in the first modulation period. (b) The peak-to-trough temperature amplitude $\unicode[STIX]{x1D6FF}T=T_{p}-T_{v}$. Open diamonds: experimental data; solid squares: numerical data. Results extracted from the temperature traces shown in figures 7 and 8.

Figure 10

Figure 10. Four instantaneous profiles of normalized temperature $T^{\ast }(z^{\ast })=[T(t)-T_{b,0}]/[T_{i}(t)-T_{b,0}]$ of the mushy layer measured during the first modulation period, where $z^{\ast }=z/h(t)$. Symbols: experimental data; dashed lines: numerical results. The inset sketches the variation of the bottom temperature in these four phases. Results for $A=10~\text{K}$, $\unicode[STIX]{x1D70F}=4000~\text{s}$ and $\unicode[STIX]{x1D719}_{0}=0$.

Ding et al. supplementary movie

Shadowgraphy movies that show the growth of mushy layers and the flows in the liquid region in three modulation modes with Φ0=0 (left), constant cooling (middle) and Φ0=π (right). Results for A=15K, τ=4000s. The movies display 400 times faster than the real time.

Download Ding et al. supplementary movie(Video)
Video 63 MB