The supported BILP-101x membranes with an effective area of 1.33 cm2 were mounted in a flange between Viton O-rings. This flange fits in a permeation module, which was placed inside an oven in a homemade permeation setup. The diagram is shown in scheme S1. The H2/CO2 separation measurements were performed using a 50:50 H2/CO2 gas mixture (100 ml min−1 of CO2 and 100 ml min−1 of H2) as feed. Helium (4.6 ml min−1) was used as sweep gas on the permeate side. The absolute pressure of the feed stream was adjusted in a range of 1 to 10 bar using a back-pressure controller at the retentate side, keeping the permeate side at atmospheric pressure. The temperature in the permeation module was adjusted from 298 to 498 K through a convection oven. An online gas chromatograph (Interscience Compact GC) equipped with a packed Carboxen 1010 PLOT (30 m × 0.32 mm) column and a thermal conductivity detector was used to periodically analyze the permeate stream. For single gas permeation tests, there was a 1-bar pressure drop between the feed and permeate side. The typical A3 membrane (table S1) was repeated once to ensure reproducibility of the reported data. In all cases, gas separation performance was evaluated after ensuring steady operation.

Gas separation performance was defined by the selectivity (α) and the gas permeance (P) of the individual components. The permeance of component i (Pi) was calculated as follows (Eq. 1)Embedded Image(1)where flux Fi denotes the molar flux of compound i (mol m−2 s−1), Ni is the permeate rate of component i (mol s−1), A is the membrane area, and Δpi is the partial pressure difference of component i across the membrane, and it can be calculated according to Eq. 2Embedded Image(2)where pfeed and pperm represent the pressures at the feed and permeate sides and Yi,feed and Xi,perm are the molar fractions of component i in the feed and permeate gas streams, respectively.

The SI unit for permeance is mol s−1 m−2 Pa−1. However, gas permeances are reported in the widely used unit GPUs, where 1 GPU = 3.3928 × 10−10 mol s−1 m−2 Pa−1.

The separation factor or mixed gas selectivity (α) was calculated as the ratio of the permeance of the faster permeating component (H2) to the permeance of the less permeating component (CO2) (Eq. 3)Embedded Image(3)

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