Nitrogen‐doped C60 as a robust catalyst for CO oxidation

The O2 activation and CO oxidation on nitrogen‐doped C59N fullerene are investigated using first‐principles calculations. The calculations indicate that the C59N fullerene is able to activate O2 molecules resulting in the formation of superoxide species ( ) both kinetically and thermodynamically. The active superoxide can further react with CO to form CO2 via the Eley–Rideal mechanism by passing a stepwise reaction barrier of only 0.20 eV. Ab initio molecular dynamics (AIMD) simulation is carried out to evidence the feasibility of the Eley–Rideal mechanism. In addition, the second CO oxidation takes place with the remaining atomic O without any activation energy barrier. The full catalytic reaction cycles can occur energetically favorable and suggest a two‐step Eley–Rideal mechanism for CO oxidation with O2 catalyzed by the C59N fullerene. The catalytic properties of high percentage nitrogen‐doped fullerene (C48N12) is also examined. This work contributes to designing higher effective carbon‐based materials catalysts by a dependable theoretical insight into the catalytic properties of the nitrogen‐doped fullerene.