Catalytic
ozonation relies on the direct oxidation by ozone (O3)
and indirect oxidation by reactive oxygen species (ROS)
produced from activated ozone molecules, and the technique has been
recognized as one of the most promising remediation technologies in
water decontamination. Functional nanocarbon materials have been extensively
exploited as heterogeneous catalysts to drive catalytic ozonation
because of the environmental-benign process, easy applicability, and
high efficiency. Nevertheless, the bottlenecks in the processes are
the economical production of high-performance and robust carbocatalysts
and the debatable oxidation regimes. Different active sites have been
suggested in engineered nanocarbons, and the corresponding mechanisms
of the carbocatalytic ozonation are ambiguous including the evolution
of various ROS, occurrence of radical and nonradical reaction pathways,
selectivity toward organics, and tunable oxidation capacity. In this
Review, we will showcase the roadmap of the development of reaction-oriented
carbocatalysts and clarify the arguments in the mechanisms of the
intrinsic active sites, identification of ROS, reaction intermediates,
and oxidation pathways in carbocatalytic ozonation. We will provide
critical comments and innovative strategies on the mechanistic investigations
in carbon-based ozonation from the molecular level (electronic structures)
to macroscale (kinetics), by deliberate radical screening/capture
techniques, advanced characterizations and in situ analysis, and theoretical
computations. More importantly, the critical issues and future directions
will be proposed in the rational material/system design, mechanistic
exploration, and the implementation of this powerful technology in
catalytic oxidation and real wastewater treatment.