Silver-modified
LTA zeolites are validated to be one
of the most
efficient nanomaterials applied in adsorptive separation, which is
an energy-efficient alternative to the state-of-the-art cryogenic
distillation for ethylene and ethane separation. Here, three representative
LTA zeolites, Ag modifications via different methods including ion-exchange,
mechanical mixing, and acid leaching, are systematically explored
by X-ray photoelectron spectroscopy, high-resolution transmission
electron microscopy, H2 temperature-programming reduction,
and ultraviolet–visible spectroscopy with the assistance of
Grand Canonical Monte Carlo simulations to identify the location of
various Ag species in the LTA zeolite and thus to understand the mechanism
of promoted separation performance in nature. The performance of these
zeolites for the separation of ethylene/ethane is validated via ideal
adsorbed solution theory and breakthrough experiments under ambient
conditions. It is confirmed that Ag+ can afford selective
binding of ethylene via π-complexation. Ag2O nanoparticles
encapsulated in the zeolitic channels narrow the pore diameters to
the suitable size, excluding ethane via molecular sieving. The synergistic
effect of π-complexation and molecular sieving from Ag+ and Ag2O nanoparticles in the zeolitic channels triggers
highly selective adsorption of ethylene over ethane.