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Isoreticular Contraction of Cage-like Metal–Organic Frameworks with Optimized Pore Space for Enhanced C2H2/CO2 and C2H2/C2H4 Separations
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-03-05 , DOI: 10.1021/jacs.3c12032
Lei Zhang 1 , Taotao Xiao 1 , Xiayun Zeng 1 , Jianjun You 1 , Ziyu He 1 , Cheng-Xia Chen 2 , Qianting Wang 1 , Ayman Nafady 3 , Abdullah M Al-Enizi 3 , Shengqian Ma 4
Affiliation  

The C2H2 separation from CO2 and C2H4 is of great importance yet highly challenging in the petrochemical industry, owing to their similar physical and chemical properties. Herein, the pore nanospace engineering of cage-like mixed-ligand MFOF-1 has been accomplished via contracting the size of the pyridine- and carboxylic acid-functionalized linkers and introducing a fluoride- and sulfate-bridging cobalt cluster, based on a reticular chemistry strategy. Compared with the prototypical MFOF-1, the constructed FJUT-1 with the same topology presents significantly improved C2H2 adsorption capacity, and selective C2H2 separation performance due to the reduced cage cavity size, functionalized pore surface, and appropriate pore volume. The introduction of fluoride- and sulfate-bridging cubane-type tetranuclear cobalt clusters bestows FJUT-1 with exceptional chemical stability under harsh conditions while providing multiple potential C2H2 binding sites, thus rendering the adequate ability for practical C2H2 separation application as confirmed by the dynamic breakthrough experiments under dry and humid conditions. Additionally, the distinct binding mechanism is suggested by theoretical calculations in which the multiple supramolecular interactions involving C–H···O, C–H···F, and other van der Waals forces play a critical role in the selective C2H2 separation.

中文翻译:


具有优化孔隙空间的笼状金属有机骨架的等网收缩增强 C2H2/CO2 和 C2H2/C2H4 分离



由于CO 2 和C 2 H 4 具有相似的物理和化学性质,将C 2 H 2与CO 2和C 2 H 4分离在石化工业中具有重要意义但也极具挑战性。在此,基于网状化学,通过缩小吡啶和羧酸官能化连接体的尺寸并引入氟化物和硫酸盐桥接钴簇,完成了笼状混合配体MFOF-1的孔纳米空间工程战略。与原型MFOF-1相比,具有相同拓扑结构的FJUT-1由于减小的笼腔尺寸、功能化的孔表面和适当的孔径而显着提高了C 2 H 2吸附能力和选择性C 2 H 2分离性能体积。氟化物和硫酸盐桥接立方烷型四核钴簇的引入,使FJUT-1在恶劣条件下具有优异的化学稳定性,同时提供多个潜在的C 2 H 2结合位点,从而为实际的C 2 H 2分离应用提供了足够的能力干燥和潮湿条件下的动态突破实验证实了这一点。此外,理论计算表明了独特的结合机制,其中涉及C–H…O、C–H…F和其他范德华力的多重超分子相互作用在选择性C 2 H中发挥着关键作用。 2分离。
更新日期:2024-03-05
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