Doped Carbon Nanotube Networks for Electrochemical Filtration of Aqueous Phenol: Electrolyte Precipitation and Phenol Polymerization

Electrochemical filtration with anodic carbon nanotube (CNT) networks is reported to be effective for chemical and microbiological water treatment. Here, we investigate how CNT doping affects the electrochemical filtration performance toward the remediation of aromatic wastewaters. Purified and well-characterized undoped (C-CNT), boron-doped (B-CNT), and nitrogen-doped (N-CNT) anodic carbon nanotube networks are challenged with aqueous phenol in a sodium sulfate electrolyte. Steady-state current and effluent total organic carbon (TOC) measurements are utilized to evaluate the oxidative performance as a function of voltage and electrolysis time. In terms of steady-state TOC removal, at an applied voltage of 3 V all three anodic CNT networks are able to remove approximately 7 to 8 mgC L-1 of the influent TOC within the similar to 1 s liquid residence time of the electrochemical filter. The anodic CNT networks are partially passivated over the 5 h electrolysis time with the B-CNT network displaying the least passivation. The extent of passivation was observed to be inversely correlated to the CNT work function. SEM, XPS, and TGA of the electrolyzed CNT networks are used to identify the two primary passivation mechanisms of electrochemical phenols polymerization and electrochemical electrolyte precipitation. In agreement with chronoamperometry results, the B-CNT network has the lowest extent of passivating polymer and precipitate formation. The precipitant is determined to likely be sodium persulfate or carbonate and is removed with a simple acidic water wash. The polymer is determined to likely be polyphenylene oxide and is partially removed with the wash. All three anodic CNT networks display potential for energy efficient electrochemical filtration of aromatic wastewaters and the B-CNT are determined to be the most resistant to passivation.