A new approach is developed for evaluating the mixing properties of binary solutions at high pressure. This involves solving Poisson's equation throughout three-dimensional cubic lattices, consistent with Thomas-Fermi-Dirac (TFD) theory. Zero temperature calculations are carried out for a variety of compositions and crystal structures in 3 pressure groups relevant to Jovian planetary interiors. Pseudopotentials based on the two-component-plasma model (with a uniform electron background) are fitted to the solid-state results, and are then used in liquid-state calculations using hard-sphere perturbation theory. TFD results for H-He solutions find critical temperatures (above which all compositions are soluble) to be ∿ 0, 500, and 1500°K at pressures of 10, 100, and 1000 Mbar, respectively. These temperatures are much lower than those obtained using free electron perturbation theory, where T(crit) ∿ 10,000°K at 10 Mbar. Thus, unlike the perturbation theory results, the TFD results predict that helium should be soluble in metallic hydrogen in the deep interiors of both Jupiter and Saturn, and our calculations give an indication of the degree of model-dependence in computing high pressure mixing properties. In addition, TFD calculations for H-C and H-O solutions find phase separation temperatures to be≲ 10⁴ °K for pressures ≲ 10³ Mbar. These temperatures are considerably lower than those found assuming a uniform electron distribution (where T(crit) ≳ 10⁵ °K), and suggest that H-C and H-O solutions should also be miscible in the metallic zones of Jupiter and Saturn.