Role of N-Doping and O-Groups in Unzipped N-Doped CNT Carbocatalyst for Peroxomonosulfate Activation: Quantitative Structure-Activity Relationship

We examined the relationship between the intrinsic structure of a carbocatalyst and catalytic activity of peroxomonosulfate (PMS) activation for acetaminophen degradation. A series of nitrogen-doped carbon nanotubes with different degrees of oxidation was synthesized by the unzipping method. The linear regression analysis proposes that pyridinic N and graphitic N played a key role in the catalytic oxidation, rather than pyrrolic N and oxidized N. Pyridinic N reinforce the electron population in the graphitic framework and initiate the non-radical pathway via the formation of surface-bound radicals. Furthermore, graphitic N forms activated complexes (carbocatalyst-PMS*), facilitating the electron-transfer oxidative pathway. The correlation also affirms that -C=O was dominantly involved as a main active site, rather than -C-OH and -COOH. This study can be viewed as the first attempt to demonstrate the relationship between the fraction of N-groups and activity, and the quantity of O-groups and activity by active species (quenching studies) was established to reveal the role of N-groups and O-groups in the radical and non-radical pathways.

Automated summary

This study examines the relationship between the intrinsic structure of a carbocatalyst and its catalytic activity in peroxomonosulfate (PMS) activation for acetaminophen degradation. It is found that pyridinic N and graphitic N play a crucial role in the catalytic oxidation process.