Nitrogen-doped graphene nanosheets as reactive water purification membranes

Oxidation of organic pollutants by sulfate radicals produced via activation of persulfate has emerged as a promising advanced oxidation technology to address various challenging environmental issues. The development of an effective, environmentally-friendly, metal-free catalyst is the key to this technology. Additionally, a supported catalyst design is more advantageous than conventional suspended powder catalysts from the point of view of mass transfer and practical engineering applications (e.g. post-use separation). In this study, a metal-free N-doped reduced graphene oxide (N-rGO) catalyst was prepared via a facile hydrothermal method. N-rGO filters were then synthesized by facile vacuum filtration, such that water can flow through nanochannels within the filters. Various advanced characterization techniques were employed to obtain structural and compositional information of the as-synthesized N-rGO filters. An optimized phenol oxidative flux of 0.036 ± 0.002 mmol·h^–1 was obtained by metal-free catalytic activation of persulfate at an influent persulfate concentration of 1.0 mmol·L^–1 and filter weight of 15 mg, while a N-free rGO filter demonstrated negligible phenol oxidation capability under similar conditions. Compared to a conventional batch system, the flow-through design demonstrates obviously enhanced oxidation kinetics (0.036 vs. 0.010 mmol·h^–1), mainly due to the liquid flow through the filter leading to convection-enhanced transfer of the target molecule to the filter active sites. Overall, the results exemplified the advantages of organic compound removal by catalytic activation of persulfate using a metal-free catalyst in flowthrough mode, and demonstrated the potential of N-rGO filters for practical environmental applications.