Ionic Hydrophobic Gates on Metal–Organic Frameworks Enable High-Purity CO 2 Separation from Humid Flue Gas

作者：Deyun Sun, Shangqing Chen, He Miao, Hongxue Xu, Yongxiang Sun, Lijuan Shi, Hongbo Zeng, Qun Yi · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c02093 · 被引用次数：27 · 研究领域：Metal-Organic Frameworks: Synthesis and Applications、Carbon Dioxide Capture Technologies、Covalent Organic Framework Applications

Efficient extraction of high-purity CO 2 from humid flue gas via adsorptive separation offers a promising and sustainable solution for carbon reduction and downstream applications. However, the coadsorption of H 2 O vapor and N 2 from humid flue gas remains a persistent challenge that limits separation efficiency. To overcome this issue, this work introduces a novel concept of ionic hydrophobic gates on porous adsorbents, which enables one-step separation of high-purity CO 2 directly from humid flue gas. By assembling hydrophobic ionic liquids and fluorine-rich terephthalaldehyde onto the surface of a metal–organic framework (MOF), this design establishes H 2 O barriers and CO 2 channels on the outer shell while maintaining pore integrity in the core. The resulting core–shell material demonstrates exceptional CO 2 adsorption capacity and an extraordinary CO 2 /N 2 selectivity of 1780 (15/85, v/v), surpassing conventional adsorbents. Notably, dry CO 2 with 99.999% purity is successfully extracted from humid flue gas (relative humidity, RH = 100%) in a single breakthrough experiment. In situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and density functional theory calculations reveal that fluorine-rich hydrophobic sites act as effective H 2 O barriers, while ionic liquid segments facilitate the transport of CO 2 through hydrogen bonding and electrostatic interactions. Owing to its excellent scalability and broad compatibility with diverse MOF pl...