a b s t r a c tHydrogen separation with palladium-based membranes is considered as a promising technology for precombustion CO 2 capture as well as for industrial hydrogen production. With improvements in membrane permeance, resistances to mass transfer are becoming increasingly important. In this work, a systematic approach is followed in order to discern and account for different contributions to the overall mass transfer resistance, based on a combined experimental and modelling approach. Experiments have been performed that started with pure H 2 feed, without sweep, subsequently followed by introducing N 2 on the feed side, and N 2 sweep gas. Using a phenomenological description for the palladium layer and the dusty gas model for the membrane support, coupled to a 2D Navier-Stokes solver with a convection-diffusion equation to account for possible concentration polarisation, all relevant mass transfer resistances are adequately modelled. For the conditions investigated, the main resistances to mass transfer are concentration polarisation in the retentate, hydrogen permeation through the metallic palladium layer, and a diffusional resistance in the support layer.