Pore Modulation of Hydrogen-Bonded Organic Frameworks for Efficient Separation of Propylene

Published

September 11, 2023

Author(s)

Youlie Cai, Junkuo Gao, Jing-Hong Li, Puxu Liu, Yanchun Zheng, Wei Zhou, Hui Wu, Libo Li, Rui-Biao Lin, Banglin Chen

Abstract

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. Singlecrystal 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 (C3H6). At 298 K and 1 bar, the C3H6 storage density of HOF-ZSTU-2 reaches 0.6 kgL-1, representing one of the best C3H6 storage materials, while offering a propylene/propane (C3H6/C3H8) selectivity of 12.2. Theoretical calculations and in situ SCXRD provide a detailed analysis of the binding strength of C3H6 at different locations in the pearl-chain channel. Dynamic breakthrough tests confirm that HOF-ZSTU-2 can effectively separate C3H6 from multi-mixtures.

Citation

Angewandte Chemie

Pub Type

Journals

Citation

Cai, Y. , Gao, J. , Li, J. , Liu, P. , Zheng, Y. , Zhou, W. , Wu, H. , Li, L. , Lin, R. and Chen, B. (2023), Pore Modulation of Hydrogen-Bonded Organic Frameworks for Efficient Separation of Propylene, Angewandte Chemie (Accessed November 21, 2024)