AbstractAn extensive screening program has been performed to find a suitable membrane configuration and operating conditions for the effective recovery of ammonia from the syngas loop. All the experiments have been performed at steady state. MFI zeolite membranes in tubular and multi‐channel fiber configurations have been tested along with tubular silica membranes. At 80°C, a high ammonia permeance (2.1 × 10−7 mol.m−2.s−1.Pa−1), and a selectivity of about 10 were found with the tubular zeolite membrane, whereas for the silica membrane an even higher ammonia permeance was measured (7.6 x 10−7 mol.m−2.s−1.Pa−1) with a selectivity of about 7. For both silica and zeolite membranes, the selectivity was found to increase with increasing temperature up to 80°C. This is a combined effect of weaker adsorption of ammonia and increased diffusion at higher temperature. The results have been modeled using both the well‐mixed reactor and the log mean pressure difference approaches. To overcome their limitations in addressing changes in feed concentration along the membrane surface, a segmental model has been used to obtain suitable operating conditions and membrane areas required for an industrial application. © 2006 American Institute of Chemical Engineers AIChE J, 2006