Many medical and industrial applications require high-purity oxygen. Because of the similar physical properties of oxygen and argon, this separation is very challenging, and very few commercial adsorbents offer the ability to separate the two gases. Silver-exchanged titanosilicates (Ag-ETS-10) have the potential to separate these gases based on their adsorption affinities. In this work, adsorption isotherms of O-2, Ar, and N-2 on Ag-ETS-10 extrudates have been measured using a volumetric technique and described using a Langmuir isotherm. Single, binary, and ternary breakthrough profiles were measured using a laboratory-scale dynamic column breakthrough apparatus. These profiles have been modeled by writing mass and energy balances that are solved using the finite volume technique. The model was able to predict the experimental profiles to a high degree of accuracy. A simple vacuum swing adsorption process was simulated using mathematical models to demonstrate the potential of the material to produce high-purity oxygen. Multiobjective optimization to maximize O-2 purity and recovery from a feed containing 95% O-2 and 5% Ar revealed that purities in excess of 99.0% can be achieved at a recovery of 11.35%.