Fabrication of a Novel Covalent Organic Framework Membrane and Its Gas Separation Performance

doi:10.6023/A20040128

Abstract

Herein, we employ 2,5-dimethoxyterephthalaldehyde (DMTA) containing ether oxygen group in the structure as the construction unit to react with tetra-(4-anilyl)-methane (TAM) through Schiff-based condensation reaction in a Teflon-lined autoclave to synthesize a novel three-dimensional covalent organic framework named DMTA-COF. Furthermore, the condensation reaction was confirmed by Fourier transform infrared spectroscopy (FT-IR). The crystal structure of DMTA-COF was analyzed by the powder X-ray diffraction (PXRD) measurement in conjunction with structural simulation. The morphology, thermal stability, porosity and pore distribution of DMTA-COF were measured by scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and N₂ adsorption-desorption at 77 K. The high affinity for CO₂ adsorption was also confirmed by low pressure CO₂ sorption. Considering the relatively small pore size and the strong CO₂ adsorption interaction of DMTA-COF due to an abundant of ether oxygen group and imine linkage, we synthesized one continuous supported DMTA-COF membrane for H₂/CO₂ separation. In our study, the porous Al₂O₃ support surface was first coated with polyaniline (PANI) and was then further functionalized with aldehyde groups by reaction with DMTA at 150 ℃ for 1 h. Finally, in situ growth of the COF membrane utilizing the covalent linkage yielded a novel continuous DMTA-COF membrane. X-ray diffraction (XRD) result indicated that the DMTA-COF membrane was pure phase and had high crystallinity. From SEM characterization, we could see that the DMTA-COF membrane was compact and well intergrowth and adhered to the support tightly. Gas separation performance results shown that DMTA-COF membrane had a high H₂ permeance and selectivity of H₂/CO₂. For DMTA-COF membrane, the 1∶1 binary mixture gas separation factors of H₂/CO₂ calculated as the gas molar ratios in permeate and retentate side was 8.3 at room temperature and atmospheric pressure. And H₂/CO₂ separation factor of DMTA-COF membrane exceeded the corresponding Knudsen coefficient (4.7), with H₂ permeance of up to 6.3×10^－7 mol·m^－2·s^－1·Pa^－1. Because of its outstanding characteristics, the novel DMTA-COF membrane is expected to be widely used in the field of H₂ purification and separation.

Key words: covalent organic framework, crystal structure, membranes, gas separation, H₂ purification

Cite this article

Fu Jingru, Ben Teng. Fabrication of a Novel Covalent Organic Framework Membrane and Its Gas Separation Performance[J]. Acta Chimica Sinica, 2020, 78(8): 805-814.

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一种新型的共价有机骨架膜的制备与气体分离性能