Core–shell-structured MOF-derived 2D hierarchical nanocatalysts with enhanced Fenton-like activities

Abstract

Fenton-like reactions activated by peroxymonosulfate for the efficient and environmentally friendly degradation of refractory pollutants have gained significant attention in recent years. However, the fabrication of Fenton-like catalysts with adequate activity and stability towards toxic benzene derivates is still a long-term goal. Herein, we report a novel Fenton-like 2D porous carbon catalyst with co-anchored Co-N_x sites and nanocrystalline Co by annealing core–shell bimetallic metal–organic framework (MOF)-coated graphene oxide. During carbonization, the N-ligands in the MOF provide self-pyrolyzed reducing gases, while the Co²⁺ salts and gradually formed nanocrystalline Co serve as the in situ catalysts for the growth of Co/Co-N_x co-doped carbon nanotubes, which avoids the use of the chemical vapor deposition process. Benefiting from the unique core–shell MOF nanostructures, the fabricated 2D hierarchical catalysts display delicate micro/mesoporous structures, conductive carbon frameworks, and abundant Co/Co-N_x/pyridinic-N active sites. These unique advantages endow the catalysts with high degradation efficiencies towards different toxic benzene-derived compounds, such as bisphenol A, phenol, biphenyl, naphthalene, and even benzene-derived macromolecules. This research not only provides Fenton-like catalysts with excellent potential for the water remediation of benzene-derived contaminants, but also takes a step toward the production of advanced metal/metal-N co-doped 2D porous carbon for diverse catalytic and energy applications.