材料科学
氢气储存
氢
分子
氢键
化学工程
纳米技术
化学
有机化学
工程类
作者
Youlie Cai,Junkuo Gao,Jing‐Hong Li,Puxu Liu,Yanchun Zheng,Wei Zhou,Hui Wu,Libo Li,Rui‐Biao Lin,Banglin Chen
标识
DOI:10.1002/anie.202308579
摘要
Developing hydrogen-bonded organic frameworks (HOFs) that combine functional sites, size control, and storage capability for targeting gas molecule capture is a novel and challenging venture. However, there is a lack of effective strategies to tune the hydrogen-bonded network to achieve high-performance HOFs. Here, a series of HOFs termed as HOF-ZSTU-M (M=1, 2, and 3) with different pore structures are obtained by introducing structure-directing agents (SDAs) into the hydrogen-bonding network of tetrakis (4-carboxyphenyl) porphyrin (TCPP). These HOFs have distinct space configurations with pore channels ranging from discrete to continuous multi-dimensional. Single-crystal X-ray diffraction (SCXRD) analysis reveals a rare diversity of hydrogen-bonding models dominated by SDAs. HOF-ZSTU-2, which forms a strong layered hydrogen-bonding network with ammonium (NH4+ ) through multiple carboxyl groups, has a suitable 1D "pearl-chain" channel for the selective capture of propylene (C3 H6 ). At 298 K and 1 bar, the C3 H6 storage density of HOF-ZSTU-2 reaches 0.6 kg L-1 , representing one of the best C3 H6 storage materials, while offering a propylene/propane (C3 H6 /C3 H8 ) selectivity of 12.2. Theoretical calculations and in situ SCXRD provide a detailed analysis of the binding strength of C3 H6 at different locations in the pearl-chain channel. Dynamic breakthrough tests confirm that HOF-ZSTU-2 can effectively separate C3 H6 from multi-mixtures.
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