Graphitic N-Rich Graphene for Nonradical Peroxymonosulfate Activation

Nitrogen-doped graphene has been regarded as one of the most promising materials for nonradical peroxymonosulfate (PMS) activation. However, facile construction of nitrogen-doped graphene and systematic investigation of its nonradical PMS activation in a practical environment still far lag behind. Herein, graphitic N-rich graphene was prepared by one-step pyrolysis of urea. The obtained urea-derived graphitic N-rich graphene (UGNG) possessed a high N content of 12.12 at. % and a graphitic N proportion of 41.12%, giving a high graphitic N content of 4.98 at. %. We confirmed that PMS donated electrons to the graphitic N in UGNG, resulting in the cleavage of PMS to singlet oxygen for nonradical oxidation. The turnover frequency for the oxidation reached the highest value of 10.5 min–1. Also, the reaction could be conducted in a wide temperature (5–45 °C) range, even with the existence of common matrix species and different natural water matrixes. This work presented the direct conversion of N-rich organic urea to UGNG and systematically investigated its nonradical PMS activation, which is believed to be helpful to its further practical use.