Li Hao-Nan, Sun Ze-Yu, Yu Zhen-Jie, Man Kexin, Zhang Chao, Xu Zhi-Kang
MOE Key Laboratory of Macromolecular Synthesis and Functionalization, and Key Laboratory of Adsorption and Separation Materials & Technologies of Zhejiang Province, Department of Polymer Science and Engineering, Zhejiang University, Hangzhou, China.
The "Belt and Road" Sino-Portugal Joint Lab on Advanced Materials, International Research Center for X Polymers, Zhejiang University, Hangzhou, China.
Nat Commun. 2025 Sep 2;16(1):8199. doi: 10.1038/s41467-025-63502-2.
Mixed matrix membranes (MMMs) capable of breaking the permeability-selectivity trade-off suffer from the inefficient and disconnected bulky transport channels as well as inferior interfacial compatibility between nanomaterials and polymers. Herein, we propose an original photothermal-triggered in-situ gelation approach to elaborate an original class of MMMs, termed nanofiber-interwoven gel membranes (NIGMs) that feature tunable 3D-interconnected ultrafast transport channels and highly-selective CO-philic gel for boosting CO separation performance. The key design of NIGMs lies in leveraging dual functions of CNT-interwoven skeleton: (1) serving as a photothermal confined reactor that rapidly triggers in-situ gelation of highly-selective CO-philic gel without phase separation-induced interfacial defects to construct defect-free and thickness-controllable NIGMs; (2) functioning as a 3D-interconnected continuous skeleton for providing ultrafast CO transport channels. By orchestrating the distribution and configuration of interwoven nanofibers, the NIGMs possess a boosted CO permeance of 211.0 GPU increased by 1558% over polymeric gel counterparts and an ultrahigh CO/N and CO/CH selectivity of up to 151 and 47 respectively. Our work offers a paradigm shift in developing advanced MMMs beyond gas separation.
能够打破渗透性-选择性权衡的混合基质膜（MMMs）存在着低效且不连续的庞大传输通道，以及纳米材料与聚合物之间较差的界面相容性问题。在此，我们提出一种原创的光热触发原位凝胶化方法来制备一类原创的MMMs，称为纳米纤维交织凝胶膜（NIGMs），其具有可调谐的三维互连超快传输通道和用于提高CO分离性能的高选择性亲CO凝胶。NIGMs的关键设计在于利用碳纳米管交织骨架的双重功能：（1）作为光热受限反应器，快速触发高选择性亲CO凝胶的原位凝胶化，而不会因相分离导致界面缺陷，从而构建无缺陷且厚度可控的NIGMs；（2）作为三维互连的连续骨架，提供超快的CO传输通道。通过精心设计交织纳米纤维的分布和构型，NIGMs的CO渗透率提高到211.0 GPU，比聚合物凝胶对应物提高了1558%，并且具有高达151和47的超高CO/N和CO/CH选择性分别。我们的工作为开发超越气体分离的先进MMMs提供了范式转变。
