Dutta Subhajit, Mukherjee Soumya, Qazvini Omid T, Gupta Arvind K, Sharma Shivani, Mahato Debanjan, Babarao Ravichandar, Ghosh Sujit K
Department of Chemistry, Indian Institute of Science Education and Research (IISER), Pune, Dr. Homi Bhabha Road, Pashan, Pune, 411008, India.
Catalysis Research Center, Technical University of Munich, Ernst-Otto-Fischer Straße 1, 85748, Garching b. München, Germany.
Angew Chem Int Ed Engl. 2022 Jan 21;61(4):e202114132. doi: 10.1002/anie.202114132. Epub 2021 Dec 16.
Energy-efficient selective physisorption driven C H separation from industrial C2-C1 impurities such as C H , CO and CH is of great importance in the purification of downstream commodity chemicals. We address this challenge employing a series of isoreticular cationic metal-organic frameworks, namely iMOF-nC (n=5, 6, 7). All three square lattice topology MOFs registered higher C H uptakes versus the competing C2-C1 gases (C H , CO and CH ). Dynamic column breakthrough experiments on the best-performing iMOF-6C revealed the first three-in-one C H adsorption selectivity guided separation of C H from 1:1 C H /CO , C H /C H and C H /CH mixtures. Density functional theory calculations critically examined the C H selective interactions in iMOF-6C. Thanks to the abundance of square lattice topology MOFs, this study introduces a crystal engineering blueprint for designing C H -selective layered metal-organic physisorbents, previously unreported in cationic frameworks.
通过节能的选择性物理吸附从工业C2 - C1杂质（如C2H2、CO和CH4）中分离C2H4，对于下游商品化学品的纯化具有重要意义。我们采用一系列等规阳离子金属有机框架，即iMOF - nC（n = 5、6、7）来应对这一挑战。所有这三种方形晶格拓扑结构的金属有机框架对C2H4的吸附量均高于竞争性的C2 - C1气体（C2H2、CO和CH4）。对性能最佳的iMOF - 6C进行的动态柱穿透实验揭示了首次实现的三合一C2H4吸附选择性导向的从1:1的C2H2/CO、C2H2/C2H4和C2H2/CH4混合物中分离C2H4。密度泛函理论计算严格检验了iMOF - 6C中C2H4的选择性相互作用。由于方形晶格拓扑结构的金属有机框架数量众多，本研究引入了一种晶体工程蓝图，用于设计C2H4选择性层状金属有机物理吸附剂，这在阳离子框架中此前未见报道。
