Xie Feng, Chen Lihang, Cedeño Morales Eder Moisés, Ullah Saif, Fu Yiwen, Thonhauser Timo, Tan Kui, Bao Zongbi, Li Jing
Department of Chemistry and Chemical Biology, Rutgers University, 123 Bevier Road, Piscataway, NJ, 08854, USA.
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, P. R. China.
Nat Commun. 2024 Mar 12;15(1):2240. doi: 10.1038/s41467-024-46556-6.
The separation and purification of C6 cyclic hydrocarbons (benzene, cyclohexene, cyclohexane) represent a critically important but energy intensive process. Developing adsorptive separation technique to replace thermally driven distillation processes holds great promise to significantly reduce energy consumption. Here we report a flexible one-dimensional coordination polymer as an efficient adsorbent to discriminate ternary C6 cyclic hydrocarbons via an ideal molecular sieving mechanism. The compound undergoes fully reversible structural transformation associated with removal/re-coordination of water molecules and between activated and hydrocarbon-loaded forms. It exhibits distinct temperature- and adsorbate-dependent adsorption behavior which facilitates the complete separation of benzene, cyclohexene and cyclohexane from their binary and ternary mixtures, with the record-high uptake ratios for CH/CH and CH/CH in vapor phase and highest binary and ternary selectivities in liquid phase. In situ infrared spectroscopic analysis and ab initio calculations provide insight into the host-guest interactions and their effect on the preferential adsorption and structural transformation.
C6 环状烃（苯、环己烯、环己烷）的分离与提纯是一个至关重要但能耗巨大的过程。开发吸附分离技术以取代热驱动蒸馏过程，有望显著降低能源消耗。在此，我们报道一种柔性一维配位聚合物作为高效吸附剂，通过理想的分子筛机制区分三元 C6 环状烃。该化合物经历与水分子的去除/再配位以及活化态和负载烃态之间相关的完全可逆结构转变。它表现出明显的温度和吸附质依赖性吸附行为，这有助于从二元和三元混合物中完全分离苯、环己烯和环己烷，在气相中对 CH/CH 和 CH/CH 具有创纪录的高吸附率，在液相中具有最高的二元和三元选择性。原位红外光谱分析和从头算计算深入了解了主客体相互作用及其对优先吸附和结构转变的影响。
