Many researchers have paid more attention to the progress of carbon materials owing to their advantages, such as high activity, low cost, large surface area, high conductivity and high stability. Carbon materials have been widely used in persulfate-based advanced oxidation processes (PS-AOPs), especially for graphene (G), carbon nanotubes (CNTs) and biochar (BC). Various strategies are applied to promote their activity, however, up to now, the relationship between the structures of carbon materials and their activities in PS-AOPs has not been specifically reviewed. The methods to switch reaction pathway (radical and nonradical pathways) in carbon-persulfate-based AOPs have not been systematically explored. Hereon, this review illustrated the active sites of G, CNTs, BC and other carbon materials, and generalized the modification methods to promote the activity of carbon materials and to switch reaction pathway in PS-AOPs. The roles of carbon materials in PS-AOPs were discussed around reactive oxygen species (ROS) and the structures. ROS are frequently complex in AOPs, but main ROS generation is related to the active sites on carbon materials. The structures of carbon materials (e.g., metal-carbon bonds, the electron-deficient C atoms, unbalanced electron distribution and graphitized structures) play a decisive role in the nonradical pathway. Finally, future breakthroughs of carbon materials were proposed for practical engineering and multi-field application.
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