期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 11, 期 40, 页码 21857-21863出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d3ta04738e
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This study proposes an optimized pore engineering strategy by enlarging the core size of rigid monomers to increase the pore size of benzene cyanide-based HOFs. Through experimental validation, it is demonstrated that the resulting HOF material exhibits the highest Xe/Kr separation performance reported to date.
The efficient separation of xenon (Xe) and krypton (Kr) mixtures is a valuable but challenging process in the gas industry. Hydrogen-bonded organic frameworks (HOFs) have emerged as a promising class of porous materials for gas separation; however, due to the lack of available design methods, accurately adjusting the pore size of HOFs to improve the separation performance remains a major challenge. Herein, we present a pore engineering optimized strategy by enlarging the core size of the rigid monomers to increase the pore size of benzene cyanide-based HOFs. The replacement of the benzene ring in the molecular core of HOF-40 with a larger-sized dipyrrole ring resulted in the assembly of HOF-FJU-8a with a slightly larger pore size of 4.2 x 4.6 angstrom 2, which is demonstrated as the highest performing HOF material for Xe/Kr separation reported to date. The superior Xe/Kr separation was determined by the gas adsorption and dynamic breakthrough experiments, showing a separation factor of 8.5 and a Kr productivity over 72 L kg-1 from the binary Xe/Kr mixture. The tailored pore size of HOF-FJU-8a played a crucial role in enabling the significant differential host-guest interactions and binding affinity, as confirmed by the single crystal structures of Xe-or Kr-loaded HOF-FJU-8a and GCMC calculations. A pore engineering optimized strategy by enlarging the core size of rigid monomers is proposed to increase the pore size of benzene cyanide-based HOFs, resulting in the highest performing HOF material for Xe/Kr separation.
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