Fabrication of 3D Hierarchical Byttneria Aspera-Like Ni@Graphitic Carbon Yolk-Shell Microspheres as Bifunctional Catalysts for Ultraefficient Oxidation/Reduction of Organic Contaminants.

Abstract

The search for earth-abundant, low-cost, recyclable, multifunctional as well as highly active catalysts remains the most pressing demand for heterogeneous catalytic elimination of pollutants in water environment remediation. Herein, a porous graphitic carbon-encapsulated Ni nanoparticles (NPs) hybrid (Ni@GC) is designed/constructed by direct pyrolysis of a Ni-based metal-organic framework (MOF) in N2 . The resulting Ni@GC exhibits a unique 3D hierarchical byttneria aspera-like yolk-shell structure with a high surface area, abundant active sites as well as good microwave (MW)-absorbing performance. The outstanding MW-driven oxidation of norfloxacin to inorganic molecules and direct catalytic reduction of 4-nitrophenol to less toxic and more useful chemical raw material (4-aminophenol) can originate from the synergistic effects, including the presence of both zero-valent Ni NPs as the active center and graphitic carbon as the protective layer/electron acceptor as well as unique porous yolk-void-shell structure, which facilitates the MW energy-harvesting and/or rapid mass transfer of the reactant/product in the channels and cavities. Accordingly, the localized surface plasmon resonance-excitation and electronic relay mechanism are proposed to account for the catalytic oxidation/reduction, respectively. This work provides a new strategy for the design/assembly of multifunctional metal@GC hybrids with a unique architecture and elucidates new opportunities for remediation of environmental water.