Mechanism and efficiency research of P- and N-codoped graphene for enhanced paracetamol electrocatalytic degradation

Electrocatalytic oxidation is an effective technology for treatment of refractory organic pollutants, and its performance strongly depends on anode materials. Among all anode materials, graphene (GN) owns the advantages of high stability and lack of secondary pollution. The catalytic performance of GN can be further improved through heteroatom doping. Here, P/N-codoped graphene (PN-GN) materials were optimized and used as an anode material for 4-acetamidophenol (APAP) electrocatalytic degradation. Result indicated that PN-GN had lower internal resistance, larger specific surface area, and higher electrochemical activity than single-doped graphene materials. The catalytic activity of GN was greatly improved by P/N codoping. When PN-GN (P8.4%-N7.6%-500 °C) was used as catalyst (current of 20 mA, initial pH of 7, reaction time of 60 min), the degradation efficiency of APAP reached 98.2% ± 1.8%, which was 17.9% ± 3.6% higher than P-codoped graphene (P-GN), 14.7% ± 4.6% higher than N-codoped graphene (N-GN), and 54.0% ± 5.2% higher than GN. After 180 min of reaction, the degradation efficiency of total organic carbon (TOC) was 78.5%. The reaction conditions were optimized and the degradation pathway of APAP was estimated to elucidate the catalytic mechanism. The main active substances generated in the system were identified as active chlorine and O₂^•-.