The metal-organic framework Ni-MOF-74 was synthesized and then characterized by XRD, SEM, and N-2 adsorption techniques. The unary isotherms of CO2, CH4, C3H6, and C3H8 on Ni-MOF-74 were measured by means of a volumetric method. The Langmuir-Freundlich model appropriately describes the adsorption equilibrium data. The selective separations of two mixtures CO2/CH4 and C3H6/C3H8 on Ni-MOF-74 were experimentally investigated by a breakthrough-column technique. Simulations of transient breakthroughs for the two mixtures agree well with the experimental data In addition, with the inclusion of intra-crystalline diffusion into the simulations, the quality of the simulated breakthrough curves are improved and agree better with the experimental data. The results indicate that Ni-MOF-74 might be a candidate for the removal of C3H6 from C3H6/C3H8 mixtures and for the efficient separation of CO2 from CH4. (C) 2014 Elsevier Ltd. All rights reserved.