Mixed matrix membranes (MMMs) comprising size-sieving fillers dispersed in polymers exhibit diffusivity selectivity and may surpass the upper bound for gas separation, but their performance is limited by defects at the polymer/ filler interface. Herein, a fundamentally different approach employing a highly sorptive filler that is inherently less sensitive to interfacial defects is reported. Palladium nanoparticles with extremely high H 2 sorption are dispersed in polybenzimidazole at loadings near the percolation threshold, which increases both H 2 permeability and H 2 /CO 2 selectivity. Performance of these MMMs surpasses the state-of-the-art upper bound for H 2 /CO 2 separation with polymer-based membranes. The success of these sorption-enhanced MMMs for H 2 /CO 2 separation may launch a new research paradigm that taps the enormous knowledge of affinities between gases and nanomaterials to design MMMs for a wide variety of gas separations.

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