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To improve the pervaporation performance of polyamide membrane, thin-film composite (TFC) polyamide membranes were prepared through the interfacial polymerization between m-phenylenediamine (MPDA) or 1,3-phenylenediamine-4-sulfonic acid (MPDASA) and trimesoyl chloride (TMC) on the surface of the modified asymmetric polyacrylonitrile (mPAN) membrane and applied in the pervaporation separation of 70 weight % aqueous isopropanol solutions at 25 1C. The variations in the free volume and the thickness of the active polyamide layer of composite membrane were obtained by positron annihilation spectroscopy (PAS) experiments, in which a variable monoenergy slow-positron beam was used. FTIR-ATR spectroscopy, XPS, scanning electron microscopy, AFM and water contact angle measurements were applied to analyze chemical structures, surface elemental compositions, morphologies, surface roughness and hydrophilicity of the active polyamide layer of composite membrane. From the result of PAS experiments, the S parameter (corresponding to the free volume size and amount) and the thickness of the active polyamide MPDASA-TMC/mPAN layer were found to be lower than those of the active MPDA-TMC/mPAN layer. In the aqueous isopropanol solution dehydration, the MPDASA-TMC/mPAN membrane exhibited a higher permeation rate than but maintained the same water concentration in the permeate as did the MPDA-TMC/mPAN membrane. This is in good agreement with the analysis by PAS. Polymer Journal (2010) 42, 242-248; doi:10.1038/pj.2009.334; published online 13 January 2010Keywords: interfacial polymerization; PAS; pervaporation; polyamide; TFC membrane INTRODUCTION Polyamides have been studied as suitable membrane materials because of their high thermal stability, excellent mechanical strength and high resistance to organic solvents. Alcohol dehydration is one of the important areas in pervaporation separation processes. In pervaporation separation processes, polyamides show high selectivity in alcohol dehydration for a wide range of water concentrations. 1-5 Their high selectivity stems from the concept of high diffusion selectivity. This is because they have low free volume/low mobility and the size of water molecules is smaller than that of alcohol. However, they show low permeation rate because of their very low free volume and low water solubility. To increase the permeation rate of polyamide membranes without sacrificing selectivity, the membrane morphology must be converted from a dense thick film into an asymmetric or composite

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To improve the pervaporation performance in separating an aqueous ethanol solution, polyamide thin-film composite (TFC) membranes (m-tolidine-H-TMC/mPAN) were prepared through the interfacial polymerization reaction between trimesoyl chloride (TMC) and 2,2'-dimethylbenzidine hydrochloride (m-tolidine-H) on the surface of a modified polyacrylonitrile (mPAN) membrane. The effects of the feed ethanol concentration on the pervaporation performance and the durability of m-tolidine-H-TMC/mPAN TFC membranes were investigated. To choose the optimal mPAN membrane as the TFC substrate, the effect of hydrolysis time on the chemical properties and separation performance of an mPAN substrate was also studied. An appropriate hydrolysis time of 15 min was chosen to obtain the mPAN substrate due to the corresponding high permeation flux. The m-tolidine-H-TMC/mPAN TFC membrane exhibited a high pervaporation performance for ethanol dehydration. A positron annihilation lifetime spectroscopy experiment was used to estimate the mean free-volume radius of the m-tolidine-H-TMC polyamide selective layer, which lay between the radii of the water and ethanol molecules.

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