A novel electrocatalytic membrane : preparation, characterization, and applications

  • Bin Yang

Student thesis: Doctoral thesis

Abstract

A novel electrocatalytic membrane reactor was designed in this study to minimize or eliminate the fouling effect, a significant challenge to membrane filtration process, and improve permeate water quality with the contribution of the electrochemical reactions and electrophoresis. The electrocatalytic membrane was fabricated by using a facile thermal decomposition from the mixtures of chloride precursor solution. The coated membrane surface was employed as an anode in the hybrid electrochemical and membrane filtration system. A kind of general DSA material of ternary oxide (Ir-Sb-Sn) was coated on the α-Al2O3 membrane surface and tested first. The catalytic coating showed high hydrophilicity and good adherence with the membrane substrate. The ternary oxide in the catalytic coating was characterized to be IrO2-SnO2-Sb2O3.25 (or IrO2-SnO2-(Sb2O3)3(SbO2)2). Furthermore, a novel IrO2-Sb2O3.25 membrane with 1D nanostructure has been successfully fabricated. The distinct 1D morphology of catalytic coating shows much rougher surface and higher porosity. The surface area is 149.22 m2/g, which is almost 2.37 times that of IrO2-SnO2-Sb2O3.25 membrane. Moreover, electrically conducting Ru was introduced into 1D IrO2-Sb2O3.25 coating in order to improve the electrical property and electrochemical performance. In particularly, the flat resistivity at the Ir/Sb/Ru molar ratio of 1:1:0.25 with the catalyst loading of 40.2 g/m2 is equal to 22.5 Ω/sq, which is only 18.2% of 122 Ω/sq in IrO2-SnO2-Sb2O3.25 membrane. Similarly, the experimental EIS data show that the charge-transfer resistance (Rct) is equal to 17.1 Ω cm2 in 1D IrO2-RuO2-Sb2O3.25 membrane, which is only 25.8 % of 66.05 Ω cm2 in IrO2-SnO2-Sb2O3.25 membrane. Higher pure water permeability was achieved in the 1D IrO2-RuO2-Sb2O3.25 membrane due to higher porosity, in comparison with IrO2-SnO2-Sb2O3.25 membrane. The water flow resistance of 1D IrO2-RuO2-Sb2O3.25 membrane is only 80% of that of IrO2-SnO2-Sb2O3.25 membrane with the same catalyst loading of 35 g/m2. The extents of fouling of both catalytic membranes for oily wastewater treatment were reduced due to their higher hydrophilicity in comparison with the original uncoated Al2O3 membrane. Electrocatalytic reactions were successfully achieved on the catalytic membrane surface when it was employed as the anode in the electrocatalytic membrane reactor. The extent of fouling was reduced by at least 20% after 30 min of operation, when 0.15A current was applied. The generated gas bubbles may prevent the oily pollutants from adsorption and the reactive intermediates may electrochemically oxidize the oily foulants on the membrane surface. The time-average permeate flux increased by almost 44% owing to the contribution of electrochemical reactions. The water quality of permeate solution for electrocatalytic membrane was further enhanced with the increasing in the applied current. The COD rejections are 95.8% and the permeate COD are 22.3 mg/L at the applied currents of 0.15A. The membrane fouling also can be significantly minimized by electrophoresis, when no appreciable current was passed through the electrocatalytic membrane reactor with the catalytic membrane surface as the anode. Only 25.2% drop in permeate flux was observed after 2.8 h of operation when the 13 V/cm electric field was applied, and the highest permeate volume of 1240 mL was achieved. In contrast, the permeate flux declined rapidly and decreased by 90% after 40 min of operation without the assistance of the electrophoresis. The time-average permeate flux is around 414 L/m2·h·bar, which is over 6 times of that without electric field. The permeate COD and COD rejections are 15.9 mg/L and 97.0%, respectively.
Date of Award2012
Original languageEnglish
Awarding Institution
  • The Hong Kong University of Science and Technology

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