Rational Design of a Low-Dimensional and Metal-free Heterostructure for Efficient Water Oxidation: DFT and Experimental Studies

A nitrogen-doped fullerene dimer is synthesized and compounded with multi-walled carbon nanotubes (MWCNTs) to construct a low-dimensional and metal-free 0D–1D heterostructure for electrocatalytic water oxidation. The (C59N)2/MWCNTs heterostructure exhibits a highly efficient performance, as verified by both first-principles density functional theory and experimental studies. The *O → *OOH process is confirmed as the rate-determining step of water oxidation. The negatively charged N-doping leads to electronic redistribution and intermolecular charge transfer and thus reduces the uphill free energies of intermediates on the (C59N)2/MWCNTs interface. Therefore, the (C59N)2/MWCNTs heterostructure has great potential to emit light and heat in metal-free-based electrocatalytic water oxidation.