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Single-Crystalline 3D Covalent Organic Frameworks for One-Step Propylene Purification from a
Shangwei Yuan1, Baoqiu Yu1, Zhongwei Liu1
1Key Laboratory of Macrocyclic and Supramolecular Chemistry of Guizhou Province, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China.
None:
Developing energy-efficient technologies for purifying propylene (C3H6) from a ternary C3 hydrocarbon mixture is critically important but remains unexploited in porous covalent organic frameworks (COFs). Herein, two single-crystalline 3D COFs with uniform octahedral morphologies, TAM-TFTB-COF and TATB-TFS-COF, were synthesized via Schiff-base condensation of Td-symmetric building blocks. Both COFs display isostructural 3-fold interpenetrated dia-b networks based on 3D electron diffraction analysis, complemented by powder X-ray diffraction data and theoretical simulations. The N2 sorption isotherms of desolvated TAM-TFTB-COF and TATB-TFS-COF at 77 K exhibit type I sorption behavior with Brunauer-Emmett-Teller surface areas up to 2899 m2 g-1, among the top 3D imine-linked COFs. The activated TAM-TFTB-COF and TATB-TFS-COF show remarkably higher adsorption capacities for C3H4 (294.8 cm3 g-1) and C3H8 (205.2 cm3 g-1) than for C3H6 (173.4 cm3 g-1) for the former species and 246.6, 175.2, and 155.4 cm3 g-1 for the latter at 298 K and 1 bar. This endows the activated COFs with a one-step C3H6 purification capability from a C3H4/C3H6/C3H8 ternary mixture at 298 K according to single-component adsorption and dynamic breakthrough experimental results. On the basis of theoretical calculations, such a one-step C3H6 purification originates from the more intense multipoint supramolecular interactions of the framework with C3H4 and C3H8 than with C3H6 together with the favorable shape matching between the pores of the framework and C3H8. This work offers valuable insights for guiding the design of next-generation adsorbents for high-value gas purification.
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