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Electrochemical removal of hexavalent chromium using electrically conducting carbon nanotube/polymer composite ultrafiltration membranes

Duan, Wenyan, Chen, Gongde, Chen, Chuxiao, Sanghvi, Riya, Iddya, Arpita, Walker, Sharon, Liu, Haizhou, Ronen, Avner, Jassby, David
Journal of membrane science 2017 v.531 pp. 160-171
artificial membranes, carbon nanotubes, chromium, composite polymers, electrochemistry, electrodes, electrostatic interactions, ionic strength, ions, membrane potential, pH, pollution, polyvinyl alcohol, salinity, tap water, ultrafiltration, uranium
Hexavalent chromium (Cr(VI)) contamination in drinking water resources remains a challenge in many parts of the United States, as well as in regions affected by industrial pollution. In this study, we demonstrated how electrically conducting carbon nanotube (CNT) – polyvinyl alcohol (PVA) composite ultrafiltration (UF) membranes can be used to remove Cr(VI) from water through a combined process of electrostatic repulsion, electrochemical reduction, and precipitation. The impact of different operational (flux, contact time, applied electrical potential) and environmental (pH and salinity) conditions on Cr(VI) removal were evaluated. Due to the native electrical potential of the CNT/PVA UF membrane material, approximately 45% removal of 1ppm Cr(VI) solution was detected under neutral pH conditions in deionized water. Increased Cr(VI) removal was observed with increasing membrane surface charge density, which was accomplished through the application of an external potential (3V, 5V and 7V, membrane as cathode) to the electrically conductive membrane surface. The solution ionic strength showed a significant impact on Cr(VI) removal. By increasing the ionic strength without applying external potential on the membrane, the electrostatic repulsive force between the charged membrane surface and the CrO4²⁻ ion was eliminated, and Cr(VI) removal dropped to zero. The highest removal (95%) was achieved when 7V was applied to the membrane/counter electrode with a 6µm-thick membrane. Here, Cr(VI) was electrochemically reduced to Cr(III) on the membrane surface, followed by Cr(III) precipitation as chromium hydroxide Cr(OH)3(s), which occurred by Cr(III) reacting with hydroxide ions generated via water splitting on the CNT network. Precipitated Cr(OH)3 was then removed by the UF membrane. In addition, CNT-PVA UF membranes were used to treat tap water spiked with Cr(VI); under these conditions, 99% Cr(VI) removal was observed when 7V were applied to the membrane/counter electrode. Furthermore, we demonstrate that other trace inorganic contaminants, such as uranium, were effectively removed as well.