The structural orientation of an amphiphilic crystalline polymer to a highly ordered microphase-separated lamellar structure on a hydrophobic surface is presented. It is formed by the surface graft polymerization of poly(ethylene glycol)behenyl ether methacrylate onto poly(trimethylsilyl) propyne in the presence of allylamine. In particular, allylamine plays a pivotal role in controlling the crystalline phase, configuration, and permeation properties. The resulting materials are effectively used to improve the CO 2 capture property of membranes. Upon the optimization of the reaction conditions, a high CO 2 permeability of 501 Barrer and a CO 2 /N 2 ideal selectivity of 77.2 are obtained, which exceed the Robeson upper bound limit. It is inspiring to surpass the upper bound limit via a simple surface modification method.
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