Evaluation of the stability of polyacrylonitrile-based carbon fiber electrode for hydrogen peroxide production and phenol mineralization during electro-peroxone process

Abstract

This study evaluated the stability of polyacrylonitrile-based carbon fiber cathode for hydrogen peroxide (H2O2) production and phenol mineralization during multiple cycles of electro-peroxone (E-peroxone) process. Results show that the oxidation of bulk carbon fiber by electro-generated H2O2 and bubbled ozone (O3) is negligible during the E-peroxone process. Nevertheless, the carbon fiber surface was oxidized to some extent as the cathode was repeatedly used in the multi-cycle E-peroxone process. Due to the oxidation by H2O2 and O3, nitrogen-containing groups on the carbon fiber surface were converted from pyridinic-N to pyridonic-N during the E-peroxone process. These changes resulted in an increase in the activity of the cathode for oxygen reduction reaction (ORR), but a decrease in the selectivity of the cathode for two-electron ORR to H2O2. After the carbon fiber cathode was used for 30 cycles of the E-peroxone treatment of phenol solutions, the cathodic potentials for ORR shifted positively by ~450 mV, which is beneficial to reduce the energy consumption of electrochemical H2O2 production. Nevertheless, the apparent current efficiency (ACE) for H2O2 production decreased from ~91.5% for the virgin cathode to ~48.2% for the used cathode. Despite the decrease in the ACE for H2O2 production, sufficient amounts of H2O2 could still be produced during the E-peroxone process with the used cathode. Therefore, complete phenol mineralization was maintained during all 30 cycles of the E-peroxone treatment of phenol solutions. These results suggest that the polyacrylonitrile-based carbon fiber is a promising cathode material for long-term E-peroxone operations.