In a previous work (Courthial et al.) a transient state characterization method for zeolite supported membranes has been proposed and tested for single components in the Henry domain. An extension of the method to single components beyond the Henry domain and to binary mixtures is described. Since the method is based on experiments performed within the linear domain, the dynamic model previously developed for single components in the Henry domain is extended. The parameter estimation procedure that is described is based on a deep analysis of the model structure with respect to its structural identifiability properties. Some experimental results concerning pure n-butane as well as isobutane/ n-butane mixtures transport through mordenite framework inverted (MFI)-supported membranes are finally shown to illustrate the technique. (C) 2012 American Institute of Chemical Engineers AIChE J, 59: 959-970, 2013