Dou Haozhen, Xu Mi, Wang Baoyu, Zhang Zhen, Luo Dan, Shi Benbing, Wen Guobin, Mousavi Mahboubeh, Yu Aiping, Bai Zhengyu, Jiang Zhongyi, Chen Zhongwei
Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, Ontario, N2L 3G1, Canada.
School of Chemical Engineering and Technology, Collaborative Innovation Centre of Chemical Science and Engineering, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin, 300350, China.
Angew Chem Int Ed Engl. 2021 Mar 8;60(11):5864-5870. doi: 10.1002/anie.202014893. Epub 2021 Jan 27.
The implementation of mixed matrix membranes (MMMs) for sub-angstrom scale gas separations remains a grand challenge. Herein, a series of analogous mixed matrix membrane (AMMMs) were constructed via molecular-level hybridization by utilizing a reactive ionic liquid (RIL) as the continuous phase and graphene quantum dots (GQD) as nanofiller for sub-angstrom scale ethylene/ethane (0.416 nm/0.443 nm) separation. With a small number of GQDs (3.5 wt%) embedded in GQD/RIL AMMMs, ethylene permeability soared by 3.1-fold, and ethylene/ethane selectivity simultaneously boosted by nearly 60 % and reached up to 99.5, which outperformed most previously reported state-of-the-art membranes. Importantly, the interfacial pathway structure was visualized and their self-assembly mechanism was revealed, where the non-covalent interactions between RIL and GQDs induced the local arrangement of IL chains to self-assemble into plenty of compact and superfast interfacial pathways, contributing to the combination of superhigh permeability and selectivity.
用于亚埃尺度气体分离的混合基质膜(MMM)的实现仍然是一个巨大的挑战。在此,通过分子水平杂交构建了一系列类似的混合基质膜(AMMM),利用反应性离子液体(RIL)作为连续相,石墨烯量子点(GQD)作为纳米填料用于亚埃尺度乙烯/乙烷(0.416 nm/0.443 nm)分离。在GQD/RIL AMMM中嵌入少量GQD(3.5 wt%)后,乙烯渗透率飙升3.1倍,乙烯/乙烷选择性同时提高近60%,达到99.5,优于大多数先前报道的先进膜。重要的是,可视化了界面通道结构并揭示了其自组装机制,其中RIL与GQD之间的非共价相互作用诱导IL链局部排列自组装成大量致密且超快的界面通道,有助于实现超高渗透率和选择性的结合。