Abstract

<h2>Summary</h2> Membranes play an important role in gas separation on account of their low cost, energy efficiency, and durability. Gas-separation membranes, however, are subject to permeability-selectivity trade-off, i.e., atomically thin 2D materials such as porous graphene can provide ultrahigh permeances in the range of ∼10<sup>5</sup>–10<sup>7</sup> GPU but suffer from low gas selectivity. Here, we show a new concept to enhance the selectivity of graphene-based membranes by employing adsorptive separation for binary gas mixtures. The deposition of "microislands" of Pd and Ni on the porous double-layer graphene support allowed us to selectively target H<sub>2</sub> in He/H<sub>2</sub> and CO<sub>2</sub> in H<sub>2</sub>/CO<sub>2</sub> mixtures, respectively, thus enabling efficient separation of He and also leading to the highest H<sub>2</sub>/CO<sub>2</sub> separation factor of 26 within the ∼10<sup>5</sup> GPU permeance range. Moreover, the selective targeting of individual gases in a membrane setting through adsorptive separation at room temperature can be a promising alternative for economical gas separation.

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