Directional construction of micron‐scale vertical <scp>MOFs</scp> channels for ultrafast, in‐parallel <scp> CO ₂ </scp> transport

Abstract Constructing vertically aligned, penetrating metal–organic framework (MOFs) gas transfer pathways within mixed matrix membranes (MMMs) is an effective strategy for optimizing gas transport under low filler loading (≤25 wt.%). Herein, we developed a novel “stack‐polymerize‐section” process to construct vertically aligned ZIF‐8 pathways in MMMs by tailoring the density and channel size of PAN@ZIF‐8 NFM for optimizing CO 2 ultrafast and in‐parallel transport. The designed XLPEO/PAN@ZIF‐8 MMM exhibits excellent performance far exceeding the 2019 McKeown upper bound, with CO 2 permeability and CO 2 /N 2 selectivity of 369.2 Barrer and 90.0, respectively. Meanwhile, a novel parallel computational model that synergistically integrates the Maxwell model with resistance‐based (RB) model methodology was proposed to introduce the interfacial resistance coefficient derived from polymer–MOFs interface heterogeneous concentration gradients. This work demonstrates the potential of vertically aligned MOFs channels for high‐performance gas separation, providing a scalable and controllable fabrication pathway for maximizing the efficiency of MOFs in membrane technology.