HY2SEPS was an EU-funded project directed at the reduction of CO2 emissions. The principal objective of the project was to develop a hybrid membrane-adsorptive H2/CO2 separation technique that would form an integral element of the pre-combustion process. Specific tasks included the derivation of simplified mathematical models for the membrane separation of H2/CO2 mixtures.In the present study one of the developed models is discussed in detail, namely that with the countercurrent plug flow of the feed and the permeate. A number of simulations were carried out concerning the separation of binary mixtures that may appear following steam conversion of methane. The numerical results were then compared with the experimental data obtained by FORTH/ICEHT. The estimated fluxes of pure CO2, H2, CH4 and N2 are shown alongside those measured experimentally as a function of temperature and CO2 partial pressure in Figs 2 - 7. It is concluded that, in general, CO2 flux increases monotonically with both temperature and CO2 partial pressure. It is also found that the fluxes of hydrogen, methane and nitrogen reach a minimum at a temperature slightly above 323 K. Overall, a good agreement was obtained between the simulations and experiments.