Abstract
The effect of temperature on the adsorption of a simple mixture (Ar/Kr) in disordered porous materials is investigated by means of molecular simulation. In the larger mesopores of porous silica glasses, capillary condensation occurs upon decreasing the temperature. At temperatures above the capillary condensation temperature, Kr is preferentially adsorbed at the pore surface and Ar adsorption occurs in regions of low Kr density. For temperatures below the capillary condensation temperature, Ar density surprisingly increases as temperature increases, the behaviour that is consistent with an over-solubility effect. In contrast, in the disordered sub-nanoporous carbon, filling of the pores occurs in a reversible and continuous way upon decreasing the temperature, owing to the small size and amorphous shape of the pores. These results show that the crossover between capillary condensation and continuous reversible filling observed for pure fluids in pores also exists for mixtures. We also show that the Kr selectivity exhibits a minimum in the disordered porous silica that is located at the capillary condensation temperature. In contrast, in the disordered porous carbon where no capillary condensation occurs, the selectivity decreases monotonically with increasing the temperature. These results shed light on low-temperature adsorption of mixtures confined in porous materials and provide a guide to design efficient phase separation processes.
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