Solidification of Binary Aqueous Solution Cooled from Above

Freezing and melting phenomena are important in many different fields, including crystal growth, casting, metallurgy, geophysics, and oceanography. Solidification of a multi-component solution is the one often observed in nature. In order to investigate basic features of the freezing processes of binary systems, we conducted a series of laboratory experiments in a rectangular box cooled from above using aqueous NaNO3 solution. During the freezing, the solid phase always grows into many needle-like crystals called the mushy layer. We measured the growth of the mushy layer thickness, the solid fraction, the temperature, and the concentration distributions. The average solid fraction is found to increase with time in the mushy layer. This causes a slow descent of the released solute in the mushy layer and its eventual fall into the liquid region below because of gravity. We propose a one-dimensional model to explain the horizontally-averaged mushy layer growth. In the model, the estimate of a heat flux at the mushy-liquid interface due to natural convection is found essential for a correct prediction. The proposed theory predicts well the growth of the mushy-layer and the average solid fraction, once the convective heat flux is properly given. (C) 2009 Wiley Periodicals, Inc.