Industrially‐Driven Ultramicroporous Physisorbent with a Trifecta of Customized Functions for Upgrading C2H2/CO2 Separation Performance

Abstract Targeting an adsorption‐based strategy to achieve effective C 2 H 2 purification while synchronously upgrading CO 2 effluent from C 2 H 2 /CO 2 mixtures is a daunting task given their similar physical natures. Herein, an ultramicroporous network with a trifecta of customized functions that can realize efficient C 2 H 2 /CO 2 separation is reported. Static and kinetic adsorption tests have cooperatively illustrated the potential separation performance. Column breakthrough tests confirm effective C 2 H 2 purification at 298 K, yielding the desired C 2 H 2 purity of 99.9–99.98% and a separation factor of 19.1 for equimolar C 2 H 2 /CO 2 . Notably, food‐grade CO 2 effluent with a higher purity of ≥99.95% can also be collected. Further, shaped 1a /PAN (PAN = polyacrylonitrile) nanofiber is formed by using an appealing net‐fishing‐inspired electrospinning (NFIE) strategy to accelerate the diffusion process of guests, as revealed by breakthrough tests. In situ high‐resolution synchrotron X‐ray diffraction (HRSXRD), simulations, etc. have explicitly unraveled the potential adsorption mechanism. Notably, the structurally stable 1a can be readily synthesized on a kilogram scale using cost‐effective raw material (merely $320.3 kg −1 ), which is of significant importance for industrial applications.