Catalytic oxidation of CO using a silicon-coordinated carbon nitride fullerene

We report, for the first time, the possibility of using a silicon atom coordinated carbon nitride fullerene (Si@C24N24) as an efficient catalyst for oxidation of CO by O(2)molecule. According to our results, the CO oxidation reaction over Si-C(24)N(24)proceeds via a two-step Langmuir-Hinshelwood mechanism: i.e. (a) CO + O-2 -> OCOO -> CO2 + O and (b) CO + O -> CO2. The activation energy for the rate-determining step of this process is only 0.42 eV, which seems to be easily overcome at room temperature. Moreover, spin-crossing between singlet and triplet spin states is found to play an important role in CO oxidation via the Eley-Rideal mechanism. Besides, it is found that the moisture effect can promote the catalytic activity of Si@C(24)N(24)and makes a large decrease in the activation energy of O(2)dissociation reaction.