Adsorbent compositions useful in adsorption and separation processes are made using silicone-derived binding agents. The adsorbent compositions are made from crystallite aluminosilicate particles bound with silicone-derived binding agents, and optionally small amounts of a clay binder, to form agglomerated crystallite particles and are calcined to volatilize the organic components associated with the silicone-derived binding agents. The agglomerated crystallite particles have superior pore structures and superior crush strengths at low binder concentrations and exhibit enhanced N2 adsorption rates and capacities when used in air separation processes.