Jia Youyu, Shi Feng, Li Hongying, Yan Zhikun, Xu Jiwei, Gao Jiale, Wu Xiaoli, Li Yifan, Wang Jingtao, Zhang Bing
School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, People's Republic of China.
ACS Nano. 2022 Sep 27;16(9):14379-14389. doi: 10.1021/acsnano.2c04670. Epub 2022 Sep 12.
Two-dimensional (2D) lamellar membranes, with highly ordered nanochannels between the adjacent layers, have revealed potential application prospects in various fields. To separate gases with similar kinetic diameters, intercalation of a functional liquid, especially an ionic liquid (IL), into 2D lamellar membranes is proved to be an efficient method due to the capacity of imparting solubility-based separation and sealing undesired defects. Stable immobilization of a high content of liquid is challenging but extremely required to achieve and maintain high separation performance. Herein, we describe the intercalation of a typical IL, 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF]), into the ionized nanochannels of sulfonated MXene lamellar membranes, where the sulfonate groups are anchored onto MXene nanosheets through a facile method based on metal-catechol chelating chemistry. Thanks to the intrinsic benefits of MXene as building blocks and the decorated sulfonate groups, the optimal membrane possesses adequate interlayer spacing (∼1.8 nm) and high IL uptake (∼47 wt %) and therefore presents a CO permeance of 519 GPU and a CO/N selectivity of 210, outperforming the previously reported liquid-immobilized lamellar membranes. Moreover, the IL loss rate of the membrane within 7 days at elevated pressure (5 bar) is measured to be significantly decreased (from 43.2 to 9.0 wt %) after growing sulfonate groups on the nanochannel walls, demonstrating the excellent IL storage stability.
二维(2D)层状膜在相邻层之间具有高度有序的纳米通道,在各个领域都展现出了潜在的应用前景。为了分离具有相似动力学直径的气体,将功能液体,尤其是离子液体(IL)插入二维层状膜被证明是一种有效的方法,因为它能够实现基于溶解度的分离并封闭不希望出现的缺陷。稳定固定高含量的液体具有挑战性,但对于实现和维持高分离性能来说是极为必要的。在此,我们描述了将一种典型的离子液体1-丁基-3-甲基咪唑四氟硼酸盐([BMIM][BF₄])插入磺化MXene层状膜的离子化纳米通道中,其中磺酸根基团通过基于金属-儿茶酚螯合化学的简便方法锚定在MXene纳米片上。得益于MXene作为构建单元的固有优势以及修饰的磺酸根基团,优化后的膜具有足够的层间距(约1.8纳米)和高离子液体吸收率(约47重量%),因此呈现出519 GPU的CO渗透通量和210的CO/N₂选择性,优于先前报道的固定液体的层状膜。此外,在纳米通道壁上生长磺酸根基团后,该膜在高压(5巴)下7天内的离子液体损失率显著降低(从43.2降至9.0重量%),证明了其优异的离子液体储存稳定性。