Nitrogen-doped C₆₀ as a robust catalyst for CO oxidation

The O₂ activation and CO oxidation on nitrogen-doped C₅₉ N fullerene are investigated using first-principles calculations. The calculations indicate that the C₅₉ N fullerene is able to activate O₂ molecules resulting in the formation of superoxide species ( O2-) 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 C₅₉ N fullerene. The catalytic properties of high percentage nitrogen-doped fullerene (C₄₈ N₁₂ ) 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. © 2017 Wiley Periodicals, Inc.