An MOF-Based Single-Molecule Propylene Nanotrap for Benchmark Propylene Capture from Ethylene

作者：Jia‐Xin Wang, Tengfei Zhang, Jiyan Pei, Di Liu, Yubo Wang, Xiao‐Wen Gu, Guodong Qian, Bin Li · 发表于：Chem & Bio Engineering · 年份：2024 · DOI：10.1021/cbe.4c00102 · 被引用次数：31 · 研究领域：Metal-Organic Frameworks: Synthesis and Applications、Zeolite Catalysis and Synthesis、Covalent Organic Framework Applications

High Resolution Image Download MS PowerPoint Slide Highly selective capture and separation of propylene (C 3 H 6 ) from ethylene (C 2 H 4 ) presents one of the most crucial processes to obtain pure C 2 H 4 in the petrochemical industry. The separation performance of current physisorbents is commonly limited by insufficient C 3 H 6 binding affinity, resulting in poor low-pressure C 3 H 6 uptakes or inadequate C 3 H 6 /C 2 H 4 selectivities. Herein, we realize a unique single-molecule C 3 H 6 nanotrap in an ultramicroporous MOF material (Co(pyz)[Pd(CN) 4 ], ZJU-74a-Pd), exhibiting the benchmark C 3 H 6 capture capacity at low-pressure regions. This MOF-based nanotrap features the sandwichlike strong multipoint binding sites and the perfect size match with C 3 H 6 molecules, providing an ultrastrong C 3 H 6 binding affinity with the maximal Q st value (55.8 kJ mol –1 ). This affords the nanotrap to exhibit one of the highest C 3 H 6 uptakes at low pressures (60.5 and 103.8 cm 3 cm –3 at 0.01 and 0.1 bar) and record-high C 3 H 6 /C 2 H 4 selectivity (23.4). Theoretical calculations reveal that the perfectly size-matched pore cavities combined with sandwichlike multibinding sites enable this single-molecule C 3 H 6 nanotrap to maximize the C 3 H 6 binding affinity, mainly accounting for its record low-pressure C 3 H 6 capture capacity and selectivity. Breakthrough experiments further confirm its excellent separation capacity for actual 1/99 and 50/50 C 3 H 6 /C 2 H 4 mixtures, aff...