Liu Jiaqi, Wang Hao, Li Jing
Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic 7098 Liuxian Blvd., Nanshan Shenzhen 518055 Guangdong P. R. China
Department of Chemistry and Chemical Biology, Rutgers University 123 Bevier Road Piscataway New Jersey 08854 USA
Chem Sci. 2023 May 15;14(22):5912-5917. doi: 10.1039/d3sc01134h. eCollection 2023 Jun 7.
The selective adsorption of CH and CH over CH from CH/CH/CH ternary mixtures for one-step CH purification represents a crucial yet challenging task in industry. The pore structure of the adsorbents must be finely tailored to meet the demanding requirements for the separation considering the very similar physicochemical properties of the three gases. Herein, we report a Zn-triazolate-dicarboxylate framework, HIAM-210, featuring a novel topology which possesses one-dimensional channels decorated with adjacent uncoordinated carboxylate-O atoms. The suitable pore size and customized pore environment enable the compound to selectively capture CH and CH with high CH/CH and CH/CH selectivities of both 2.0. Breakthrough experiments show that polymer-grade CH can be directly harvested from CH/CH/CH (34/33/33 and 1/90/9) ternary mixtures. The underlying mechanism of the preferential adsorption was uncovered by grand canonical Monte Carlo simulations and DFT calculations.
从CH₄/C₂H₄/C₂H₆三元混合物中选择性吸附CH₄和C₂H₄以实现一步法CH₄提纯,这在工业上是一项关键但具有挑战性的任务。考虑到这三种气体非常相似的物理化学性质,吸附剂的孔结构必须经过精细调整,以满足分离的严格要求。在此,我们报道了一种锌三唑啉二羧酸盐框架结构HIAM-210,其具有一种新颖的拓扑结构,拥有一维通道,通道由相邻的未配位羧酸盐 - O原子修饰。合适的孔径和定制的孔环境使该化合物能够以2.0的CH₄/C₂H₄和CH₄/C₂H₆选择性选择性捕获CH₄和C₂H₄。突破实验表明,可以从CH₄/C₂H₄/C₂H₆(34/33/33和1/90/9)三元混合物中直接获得聚合物级CH₄。通过巨正则蒙特卡罗模拟和密度泛函理论计算揭示了优先吸附的潜在机制。