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We apply the principle of maximum entropy to consider the excluded volume effect on the phase separation of binary mixtures consisting of hard spheres with two different diameters. We show that a critical volume fraction of hard spheres exists locating the packing of large spheres. In particular, through numerical calculation, we have found that the critical volume fraction becomes lower when the ratio α = σ1/σ2 of large-to-small sphere diameters increases, but becomes higher when the ratio of the large sphere volume fraction to the total volume fraction of large and small spheres increases.