Nitrogen-Doped C-60 as a Robust Catalyst for CO Oxidation

作者：Lin I Hsiang; Lu Yu Huan; Chen Hsin Tsung

来源：Journal of Computational Chemistry, 2017, 38(23): 2041-2046.

DOI：10.1002/jcc.24851

• nitrogen-doped C60 fullerene
• first-principles calculations
• CO oxidation
• Eley-Rideal mechanism

The O-2 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 O-2 molecules resulting in the formation of superoxide species (O-2 2) both kinetically and thermodynamically. The active superoxide can further react with CO to form CO2 via the EleyRideal 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 O-2 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.

• 出版日期2017-9-5