N-Doped Graphitized Carbon Nanohorns as a Forefront Electrocatalyst in Highly Selective O2 Reduction to H2O2

Electrochemical oxygen reduction (ORR) is a challenging approach for the sustainable production of hydrogen peroxide (H2O2) and is also a reaction of relevance in fuel-cell applications. Here, we propose an outstanding metal-free electrocatalyst for the unexpectedly selective ORR to H2O2, consisting of graphitized N-doped single-wall carbon nanohorns (CNHs). The catalyst can operate at acidic pH to a faradic efficiency as high as 98%, but it also shows excellent performance at either physiological or alkaline pH. Moreover, the very positive onset potentials observed at all pH values investigated (+0.40 V, +0.53 V, and +0.71 V at pH 1.0, 7.4, and 13.0, respectively), good stability, and excellent reproducibility make this material a benchmark catalyst for ORR to H2O2. The outstanding activity arises from a combination of several factors, such as CNH-dependent facilitation of electron delivery, suitable porosity, and a favorable distribution of the types of N atoms.