Wang Hongjian, Zhai Yeming, Li Yang, Cao Yu, Shi Benbing, Li Runlai, Zhu Zingting, Jiang Haifei, Guo Zheyuan, Wang Meidi, Chen Long, Liu Yawei, Zhou Kai-Ge, Pan Fusheng, Jiang Zhongyi
Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, 300072, Tianjin, China.
Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), 300072, Tianjin, China.
Nat Commun. 2022 Nov 19;13(1):7123. doi: 10.1038/s41467-022-34849-7.
Covalent organic frameworks (COF), with rigid, highly ordered and tunable structures, can actively manipulate the synergy of entropic selectivity and enthalpic selectivity, holding great potential as next-generation membrane materials for ion separations. Here, we demonstrated the efficient separation of monovalent cations by COF membrane. The channels of COF membrane are decorated with three different kinds of acid groups. A concept of confined cascade separation was proposed to elucidate the separation process. The channels of COF membrane comprised two kinds of domains, acid-domains and acid-free-domains. The acid-domains serve as confined stages, rendering high selectivity, while the acid-free-domains preserve the pristine channel size, rendering high permeation flux. A set of descriptors of stage properties were designed to elucidate their effect on selective ion transport behavior. The resulting COF membrane acquired high ion separation performances, with an actual selectivity of 4.2-4.7 for K/Li binary mixtures and an ideal selectivity of ~13.7 for K/Li.
共价有机框架(COF)具有刚性、高度有序且可调节的结构,能够积极调控熵选择性和焓选择性之间的协同作用,作为下一代离子分离膜材料具有巨大潜力。在此,我们展示了COF膜对单价阳离子的高效分离。COF膜的通道装饰有三种不同的酸性基团。提出了受限级联分离的概念来阐释分离过程。COF膜的通道由两种区域组成,酸性区域和无酸区域。酸性区域作为受限阶段,具有高选择性,而无酸区域保留了原始通道尺寸,具有高渗透通量。设计了一组阶段性质描述符来阐明它们对选择性离子传输行为的影响。所得的COF膜具有高离子分离性能,对于K/Li二元混合物的实际选择性为4.2 - 4.7,对于K/Li的理想选择性约为13.7。