Mixed matrix membranes (MMMs) combine the advantages of polymers and inorganic materials and demonstrate higher gas permeability than polymeric membranes, which, however, face the challenge of incompatible interface ascribed to the intrinsically different nature of the polymer and inorganic phase. To overcome this hurdle, herein, co-polyimide (6FBDA) was designed with carboxylic side groups to enhance the interfacial compatibility with amino-functionalized MOF(ZIF-8-NH₂) via intensive π-π stacking and hydrogen bonds. The imidazole units in 6FBDA resemble ZIF-8-NH₂ ligands and promote π-π stacking of polymer and MOF while the carboxylic moieties establish hydrogen bonds with the amino ligands of ZIF-8-NH₂, significantly improving the interfacial compatibility of polymer and MOF. The defect-free MMMs with 50 wt% MOF loading demonstrate a CO₂ and H₂ permeability of 80.8 Barrer and 127.5 Barrer, respectively, with a CO₂/CH₄ and H₂/CH₄ selectivity of 89.4 and 141.7, respectively, exceeding 2008 Robeson upper bounds. The experimental concept of this work opens a door for fabricating molecularly selective gas separation membranes with prospects for energy-efficient CO₂ capture and hydrogen separations.

混合基质膜（MMM）结合了聚合物和无机材料的优点，表现出比聚合物膜更高的透气性，然而，由于聚合物和无机相本质上不同的性质，聚合物膜面临着界面不相容的挑战。为了克服这一障碍，本文设计了带有羧基侧基的共聚酰亚胺（6FBDA），通过密集的π-π堆积来增强与氨基功能化MOF（ZIF-8-NH ₂ ）的界面相容性氢键。 6FBDA 中的咪唑单元类似于 ZIF-8-NH ₂ 配体，促进聚合物和 MOF 的 π-π 堆积，而羧基部分与 ZIF-8-NH ₂ 和 H ₂ 渗透率分别为 80.8 Barrer 和 127.5 Barrer，而 CO ₂ /CH ₄ 和 H ₂ /CH ₄ 选择性分别为 89.4 和 141.7，超过 2008 年 Robeson 上限。这项工作的实验概念为制造分子选择性气体分离膜打开了一扇大门，具有节能 CO ₂ 捕获和氢气分离的前景。