Seiichi Murayama

Kinetics and energy efficiency for the degradation of 1,4-dioxane by electro-peroxone process

Degradation of 1,4-dioxane by ozonation, electrolysis, and their combined electro-peroxone (E-peroxone) process was investigated. The E-peroxone process used a carbon-polytetrafluorethylene cathode to electrocatalytically convert O2 in the sparged ozone generator effluent (O2 and O3 gas mixture) to H2O2. The electro-generated H2O2 then react with sparged O3 to yield aqueous OH, which can in turn oxidize pollutants rapidly in the bulk solution. Using p-chlorobenzoic acid as OH probe, the pseudo-steady concentration of OH was determined to be ∼0.744×10(-9)mM in the E-peroxone process, which is approximately 10 and 186 times of that in ozonation and electrolysis using a Pt anode. Thanks to its higher OH concentration, the E-peroxone process eliminated 96.6% total organic carbon (TOC) from a 1,4-dioxane solution after 2h treatment with a specific energy consumption (SEC) of 0.376kWhg(-1) TOCremoved. In comparison, ozonation and electrolysis using a boron-doped diamond anode removed only ∼6.1% and 26.9% TOC with SEC of 2.43 and 0.558kWhg(-1) TOCremoved, respectively. The results indicate that the E-peroxone process can significantly improve the kinetics and energy efficiency for 1,4-dioxane mineralization as compared to the two individual processes. The E-peroxone process may thus offer a highly effective and energy-efficient alternative to treat 1,4-dioxane wastewater.

Electro-peroxone degradation of diethyl phthalate: Cathode selection, operational parameters, and degradation mechanisms.

This study compares the degradation of diethyl phthalate (DEP) by the electro-peroxone (E-peroxone) process with three different carbon-based cathodes, namely, carbon-polytetrafluorethylene (carbon-PTFE), carbon felt, and reticulated vitreous carbon (RVC). Results show that the three cathodes had different electrocatalytic activity for converting sparged O2 to H2O2, which increased in order of carbon felt, RVC, and carbon-PTFE. The in-situ generated H2O2 then reacts with sparged O3 to yield OH, which can in turn oxidize ozone-refractory DEP toward complete mineralization. In general, satisfactory total organic carbon removal yields (76.4-91.8%) could be obtained after 60min of the E-peroxone treatment with the three carbon-based cathodes, and the highest yield was obtained with the carbon-PTFE cathode due to its highest activity for H2O2 generation. In addition, the carbon-PTFE and carbon felt cathodes exhibited excellent stability over six cycles of the E-peroxone treatment of DEP solutions. Based on the intermediates (e.g., monoethyl phthalate, phthalic acid, phenolics, and carboxylic acids) identified by HPLC-UV, plausible reaction pathways were proposed for DEP mineralization by the E-peroxone process. The results of this study indicate that carbon-based cathodes generally have good electrocatalytic activity and stability for application in extended E-peroxone operations to effectively remove phthalates from water.