Nanoarchitectonics of Metal–Organic Framework on Fullerene Assemblies: Fabrication of Hierarchical Nanostructured Carbon Electrocatalysts

High Resolution Image Download MS PowerPoint Slide Designing efficient and durable carbon-based electrocatalysts remains a major challenge for next-generation energy technologies. Here, we introduce a comprehensive nanoarchitectonics approach for constructing metal–organic framework on fullerene (MOFOF) hybrids with diverse dimensionalities spanning 0D nanospheres, 1D nanorods and nanotubes, 2D sheets, and 3D cubic assemblies, and demonstrate their potential for electrocatalyst development through the pyrolysis of a selected hybrid. Through a sequential layer-by-layer (or, step-by-step) growth of a typical MOF (ZIF-67) on self-assembled fullerene supports, we generated a family of MOFOF nanostructures with diverse morphologies. Subsequent high-temperature carbonization and ammonia-assisted nitrogen doping are expected to transform these MOFOF precursors into hierarchical nitrogen-doped Co/C electrocatalysts featuring well-defined Co–N x active sites embedded within graphitized carbon frameworks. Using quasi-1D fullerene nanotubes (FNTs) as a structural template produced the most efficient catalyst, Co–N@CT-900, which delivered an onset potential of 0.78 V vs RHE and a Tafel slope of 56.6 mV dec −1, along with excellent electrochemical durability, retaining 95.2% of its initial current over 42,000 s in acidic electrolyte. More importantly, RRDE analysis revealed high H 2 O 2 selectivity exceeding 70%, indicating that the catalyst preferentially promotes the two-electron oxygen reduction pathway. Despite efficient peroxide generation, Co–N@CT–900 maintained superior stability compared to reference catalysts, highlighting its resistance to oxidative degradation. The superior performance arises from the synergistic integration of Co-supported active sites and protective graphitic carbon shells, which enable efficient H 2 O 2 production while preserving structural integrity under acidic conditions. These findings position Co–N@CT–900 as a promising high-durability catalyst for advanced water treatment technologies based on in situ H 2 O 2 generation.