A novel supported thin NH2-MIL-125 MOF layer has been prepared and evaluated as a new membrane in the separation of an equimolar hydrogen (H-2)/carbon dioxide (CO2) mixture at different temperatures. Additionally, Mixed-Matrix-Membranes (MMMs), consisting of the NH2-MIL-125 MOF powder and Matrimid as continuous polymer matrix, were prepared and investigated for the same separation process. Permeation measurements were performed at 150 degrees C and varying feed pressures (3, 4, 5 bar), thus simulating the pre-combustion process for CO2 sequestration. Since NH2-MIL-125 has free amine groups in its pore system, the attractive interaction with the polar acidic molecule CO2 is expected to retain it in comparison to H-2, resulting in an enhanced separation performance. For the neat supported NH2-MIL-125 membrane, the H-2 permeability is indeed by the factor of 8 larger than that of CO2 at room temperature. In case of the MMMs, the addition of the MOF powder enhances both the permeability and the selectivity in comparison to the neat polymer Matrimid. (C) 2016 Elsevier B.V. All rights reserved.