The single-gas and mixture-gas permeation tests were performed in a homemade permeation cell (fig. S5). The W substrate acted both as a membrane support and a gasket in the membrane module (VCR, Swagelok) to achieve a leak-tight connection. Ar was used as the sweep gas. The flow rates of the feed and the sweep gas were controlled via mass flow controllers. The pressure on the feed side was maintained at 2 bar. Before each test, the membrane was heated to 150°C to desorb the adsorbed contaminants on the graphene surface (fig. S6, table S12, and note S6). The permeate gas concentration was analyzed in real time by a mass spectrometer (HPR-20, Hiden Analytical). The data were recorded and averaged after reaching the steady-state condition (typically 30 min after changing the operation conditions). The gas permeance J, IS α (for single-gas test), and SF β (for mixture-gas test) were calculated by the following equationsEmbedded Image(3)Embedded Image(4)Embedded Image(5)where Xi is the flow rate of the component i, A is the membrane area, ΔPi is the transmembrane pressure difference of component i, and Ci and Cj are the concentrations of component i and j in feed or permeate with i being the faster permeating component.

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