A polyvinyl alcohol (PVA)/SiO2 organic-inorganic hybrid membrane was fabricated, using PVA as the basic material, SiO2 nanoparticles as the inorganic material, γ-(2,3)-glycidoxy propyl trimethoxysilane (GPTMS) and 3-aminopropyl triethoxysilane (APTEOS) as the second modified agents. The dehydration performance of PVA-SiO2/polyacrylonitrile (PAN) composite membrane to ethyl acetate (EA)/H2O, EA/ethanol (EtOH)/H2O and EA/EtOH/acetic acid (HAc)/H2O solutions was investigated. After modification of the second coupling agent of APTEOS or GPTMS, PVA-SiO2/PAN composite membrane had the better dehydration performance to these aqueous solutions. When dehydrating PVA-SiO2/PAN composite membrane modified by GPTMS (M5 membrane) in EA/H2O binary solution (98/2, wt%) at 40°C, the separation factor and the total permeation flux were 5245 and 293.9 g m−2 h−1, respectively. The preparation method of PVA/SiO2 membrane through adding the second coupling agent was simple, it had good dehydration performance and has excellent application prospects. The sorption behavior of PVA/SiO2 hybrid membrane was systematically studied, providing sufficient data for studying the separation mechanism of pervaporative membrane. The degree of swelling (DS) and the sorption selectivity of the membrane in different feed compositions and temperatures were measured to determine the static sorption of membrane. Dynamic sorption more clearly reflects the sorption and swelling processes of the membrane, and the dynamic sorption curves of the membrane in EA aqueous solutions were obtained. The sorption behavior of membrane to permeate components was studied by ATR-FTIR. Changes in the characteristic peaks for the permeate components and membrane indicated the sorption behavior of the membrane.
In this study, stable and non-defective multilayer polydimethylsiloxane (PDMS) composite pervaporation mixed matrix membranes incorporated with in-situ transformed metal organic frameworks was successfully synthesized via ligand vapor phase infiltration and spin-coating. Metal zinc sources were uniformly distributed in PDMS which were in-situ transformed into homogeneous zeolitic imidazolate framework-8 (ZIF-8) nanoparticles, effectively alleviating the aggregation of ZIF-8. Thermal cross-linking of PDMS and the formation of MOFs occurred simultaneously, omitting the complicated preparation and re-dispersion steps of MOF nanoparticles. MOF nanoparticles and PDMS formed a more stabilized composite structure by in-situ transformation, in which PDMS and metal of MOFs can interact with the - Si - O - of silane coupling groups on membrane surface to construct solid multilayer composite membrane, ensuring long-term stability. Moreover, with the aid of hydrophobic interlayer, polymer infiltration into channels of substrate was restricted and casting solution spread out smoothly, facilitating the formation of defect-free PDMS selective layer. Various techniques including Attenuated Total Reflection-Fourier Transform Infrared Spectrometer, Field Emission Scanning Electron Microscopy, Atomic Force Microscope and X-ray Diffraction were applied to explore the morphology, composition and structure of nanoparticles and membranes, and pervaporation tests were taken to investigate the behavior of hydrophobic polymer-based multilayer membranes. For the recovery of low concentration n-butanol, the prepared non-defective multilayer TAO/ZIF-8/K-PDMS composite membrane displayed excellently total permeate flux of 2890 g m −2 h −1 with competitive separation factor of 40.3.
Jiayun Shi,Taishan Wang,Jie Han,Yao Liang,Yujia Tong,Weixing Li
A novel SA-f-MWCNTs/PAN composite membrane, sodium alginate- functionalized multi-walled carbon nanotubes/polyacrylonitrile, was prepared to enhance the esterification conversion rate with a pervaporation membrane reactor. The SA-f-MWCNTs/PAN membrane was investigated by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscope. The hydrophilicity, mechanical properties, and separation performance of the composite membrane have been significantly improved. The flux of the composite membrane was 4374 g·m −2 ·h −1 , and the separation factor was 1249 (the water content in the feed was 10 wt%, at 75°C). The composite membrane the trade-off effect between flux and separation factor. The acid conversion rate of SA-f-MWCNTs/PAN membrane was up to 98.3% in 5 h at 75°C, which was a great increase of 18.3% compared with the equilibrium conversion rate of the batch reactor. In addition, SA-f-MWCNTs/PAN membrane exhibited good swelling resistance and reusability. The conversion rate of acetic acid was stable above 95.0% after 8 repetitive tests.
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