Dense film polyimide membranes for aggressive sour gas feed separations

Dense film membranes of the copolyimide 6FDA-DAM:DABA (3:2) are studied for simultaneous removal of CO2 and H2S from sour natural gas streams. Pure and mixed gas permeation as well as pure gas sorption data are reported at 35 degrees C and pressures up to 62 bar. The H2S partial pressures used are representative of highly aggressive field operations. Penetrant-induced plasticization effects are evident at feed pressures below 1 bar in pure H2S feeds; sub-Tg thermal annealing is used to effectively mitigate this effect, and these annealed films are used throughout the study. Surprisingly, H2S/CH4 selectivity nearly doubles for mixed gas testing in comparison to the pure component ideal selectivity values and approaches the level of a state-of-the-art glassy polymer, cellulose acetate (CA), at H2S partial pressures above 2 bar. Furthermore, permeation experiments using a 9.95% H2S, 19.9% CO2, 70.15% CH4 mixture at low feed pressures give CO2/CH4 selectivity of up to 49-over 30% greater than the pure component selectivity for 6FDA-DAM:DABA (3:2). The overall sour gas separation performance of this polyimide is comparable to high-performance rubbery polymer membranes, which have been reported for only moderate H2S partial pressure feeds, and is superior to that for CA based on a practical combined acid gas separation efficiency metric that we introduce. Finally, methods for continued development of the current polyimide membrane material for aggressive sour gas separations are presented. (C) 2012 Elsevier B.V. All rights reserved.