Supramolecular pyrolysis enabled sulfur-nitrogen rich graphene for advanced nonradical oxidation

Sulfur-nitrogen co-doped graphene was one of the most promising materials in advanced nonradical oxidation. However, the preparation complexity and low sulfur-nitrogen content greatly hindered its practical application. Herein, sulfur-nitrogen rich graphene (SNRG) was prepared via a one-step supramolecular pyrolysis. The obtained SNRG possessed a N content up to 19.71 at%, in accompanying with S content of 0.77 at%. It, thus, could effectively activate peroxymonosulfate to degrade diverse organic pollutants. The catalytic reaction could conduct in wide temperature (5-45°C) and pH (2.17-9.71) ranges. Also, it could effectively degrade organic pollutants at the existence common matrix species and different natural water matrix. Electron paramagnetic resonance and quenching experiments confirmed that singlet oxygen was the main reactive specie for organics degradation. Peroxymonosulfate donated electron to the sulfur-nitrogen active site in SNRG and followingly decomposed into singlet oxygen for organics degradation. Our work developed a facile methodology for the construction of sulfur-nitrogen rich carbonaceous materials for a wide range of applications.