Metal-free nanocarbons with versatile structural dimensions and unique properties emerge as promising catalysts for environmental remediation and other sustainable applications without secondary contamination. In the present work, a three-dimensional (3D) interconnected porous carbonaceous material (CN-3) derived from dicyandiamide (DCD) and hydrothermal cellulose-based carbon (HTC) has been developed for carbocatalysis toward organic oxidation. A solid-state-growth rolling-up mechanism is proposed to explain the conversion from the stacking layered structures (melem and g-C<sub>3</sub>N<sub>4</sub>) into 3D interconnected network nanoarchitectures of CN-3 at annealing temperature at 900 °C. The CN-3 exhibits excellent catalytic activity and stability in peroxymonosulfate (PMS) activation and the PMS activation from radical-dominated reaction to nonradical oxidation via controlling the surface defects and functional groups. This work could provide not only a synthetic strategy for metal-free catalysts in advanced oxidation, but also valuable insights in the relationship between the structural transformation and catalytic activity toward PMS activation to induce different oxidative pathways, which facilitate the generation of a highly active and stable carbon-based catalytic system for treatment of organic contaminants.

Three-dimensional interconnected carbonaceous materials constructed by stepwise carbonization for metal-free catalysis

ACS Fall 2020 Virtual Meeting

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