Regulating the reactive site density of two-dimensional N self-doped carbon for boosted Fenton-like catalytic ability

Abstract

The mediocre catalytic ability of metal-free carbon-based catalysts limits its practical application in wastewater treatment. Herein, a facile “steam-etching” method is utilized to boost the catalytic ability of N self-doped carbon (NSDC) catalysts. Compared to the original NSDC catalyst (NSDC-N2), the NSDC-H2O-50 catalyst modified with the water vapor content of 50 % exhibits much better catalytic performance. The pseudo-first-order kinetic rate constant k of NSDC-H2O-50 is 4.88 times that of NSDC-N2. The presence of water vapor can cause a massive vacancy-like defects in the carbon structure, which is conducive to form more edge reactive groups. Pyrrolic N and CN groups are proved to be the reactive sites for the catalytic reaction. Reactive site density can be easily adjusted by changing the water vapor content. The prepared NSDC-H2O catalysts can effectively activate peroxydisulfate (PDS) to degrade various organic pollutants with high efficiency in the pH range of 2.02–10.28. In addition, the NSDC-H2O/PDS system exhibits strong anti-interference ability to common anions and humic acid. The catalytic ability has not been affected in actual water sources. By a simple calcination treatment, most of the catalytic ability can be restored. Therefore, the prepared NSDC-H2O catalysts show strong application potential in organic wastewater treatment. Furthermore, singlet oxygen is proved to be the main active species in the NSDC-H2O/PDS system, and sulfate radical and superoxide radical play an auxiliary role.